energies

Review
Dairy Wastewater as a Potential Feedstock for Valuable
Production with Concurrent Wastewater Treatment through
Microbial Electrochemical Technologies
Anusha Ganta 1 , Yasser Bashir 2 and Sovik Das 2, *

1 Environmental and Water Resources Division, Department of Civil Engineering,

Indian Institute of Technology Madras, Chennai 600036, India
2 Department of Civil Engineering, Indian Institute of Technology Delhi, New Delhi 110016, India
* Correspondence: [email protected]

Abstract: A milk-processing plant was drafted as a distinctive staple industry amid the diverse field of
industries. Dairy products such as yogurt, cheese, milk powder, etc., consume a huge amount of water
not only for product processing, but also for sanitary purposes and for washing dairy-based industrial
gear. Henceforth, the wastewater released after the above-mentioned operations comprises a greater
concentration of nutrients, chemical oxygen demand, biochemical oxygen demand, total suspended
solids, and organic and inorganic contents that can pose severe ecological issues if not managed
effectively. The well-known processes such as coagulation–flocculation, membrane technologies,
electrocoagulation, and other biological processes such as use of a sequencing batch reactor, upflow
sludge anaerobic blanket reactor, etc., that are exploited for the treatment of dairy effluent are
extremely energy-exhaustive and acquire huge costs in terms of fabrication and maintenance. In
addition, these processes are not competent in totally removing various contaminants that exist in
Citation: Ganta, A.; Bashir, Y.; Das, S. dairy effluent. Accordingly, to decrease the energy need, microbial electrochemical technologies
Dairy Wastewater as a Potential (METs) can be effectively employed, thereby also compensating the purification charges by converting
Feedstock for Valuable Production the chemical energy present in impurities into bioelectricity and value-added products. Based on
with Concurrent Wastewater this, the current review article illuminates the application of diverse METs as a suitable substitute for
Treatment through Microbial traditional technology for treating dairy wastewater. Additionally, several hindrances on the way to
Electrochemical Technologies. real-world application and techno-economic assessment of revolutionary METs are also deliberated.
Energies 2022, 15, 9084. https://
doi.org/10.3390/en15239084 Keywords: bioelectrochemical system; dairy wastewater; microbial fuel cell; microbial electrochemical
Academic Editors: Booki Min and system; wastewater treatment
Md Tabish Noori

Received: 25 October 2022

Accepted: 24 November 2022
1. Introduction
Published: 30 November 2022
Industrial pollution is a gigantic global concern that is triggering environmental
Publisher’s Note: MDPI stays neutral
deterioration and polluting the air, water, and food around us. With the excessive ingestion
with regard to jurisdictional claims in
of water and the increase in the effluent generation per unit of product manufactured, food-
published maps and institutional affil-
processing industries have created a significant impact from an ecological perspective [1].
iations.
Specifically, among the food-processing industries recently, the dairy sector has witnessed
massive progress due to the escalating demand for milk and dairy products globally [2].
According to the International Dairy Federation’s World Dairy Situation 2016, 800 MT of milk
Copyright: © 2022 by the authors.
was produced worldwide, which was 2% higher than the production rate of 2014 [3]. In
Licensee MDPI, Basel, Switzerland. addition, with the increasing demand, the quantity of effluent released from the dairy sector
This article is an open access article has also increased; i.e., about 2 to 2.5 L of wastewater is discharged for each 1 L of milk
distributed under the terms and processed [4]. This dairy effluent comprises proteins, fats, milk carbohydrates, nutrients,
conditions of the Creative Commons and other cleaning solutions that contribute to the pollution load. Usually, dairy wastewater
Attribution (CC BY) license (https:// is found to have characteristics such as a chemical oxygen demand (COD) that varies from
creativecommons.org/licenses/by/ 80,000 to 90,000 mg/L and a biochemical oxygen demand (BOD) of around 50,000 to
4.0/). 45,000 mg/L, high total suspended solids (TSS) of about 25,000 to 45,000 mg/L, and a

Energies 2022, 15, 9084. https://doi.org/10.3390/en15239084 https://www.mdpi.com/journal/energies

Energies 2022, 15, 9084 2 of 34

varying pH that ranges between 4 and 10 [5–7]. The existing wastewater management
machinery is inefficient for eliminating all these contaminants at one time; as a result,
partially treated water is discharged into the environment. In addition, due to a lack
of proper rules and regulations, a considerable quantity of effluent is discharged into
the environment without providing the required treatment, which can further result in
adverse environmental impacts such as eutrophication, massive depletion of oxygen, etc.
Therefore, dairy wastewater requires appropriate treatment before being disposed into the
environment [8,9]. Further, if strategies such as zero-liquid discharge and reuse of treated
water are implemented in the dairy industry, it would go a long way toward dealing with
the issues associated with water pollution from this industrial sector [10,11].
Dairy effluents are also the basis for numerous emerging pollutants, especially estro-
genic compounds containing hormones that end up in the environment with industrial
discharges [4]. The destiny of these emerging pollutants is renowned as a matter of concern
for civic well-being and ecology. In addition, dairy wastewater is characterized by extensive
variations in volume and flow rates that are associated with incoherence in the diverse
production cycles in a milk-processing unit. The highly mutable attributes of dairy effluent
in terms of the pH and other characteristics such as the TSS make it challenging to select an
efficient wastewater-treatment technology and scheme [12]. On the other hand, to align
with the new discharge standards and implement the sustainable development goals, dairy
plants have implemented an intricate treatment mechanism that has influenced the indus-
try’s total expenses. For this reason, a vital requisite is to perceive a pioneering low-cost
and sustainable technology that would aid in the accomplishment of all these objectives.
Treatment of dairy effluents comprises the utilization of physicochemical and bio-
logical treatment technologies. Among the physicochemical processes, methods such as
membrane technologies, coagulation–flocculation, etc., are adapted [13], whereas the bi-
ological processes comprise both aerobic and anaerobic processes such as the activated
sludge process, lagoons, sequencing batch reactors (SBRs), upflow anaerobic sludge blan-
kets (UASB), etc. [12,14]. Nevertheless, with the limitation of soluble COD removal through
physicochemical methods and higher reagent costs, the preference for biological methods
in the dairy industry has risen immensely recently. However, these traditional processes
are associated with several drawbacks that include colossal capital costs/energy demands
and substantial sludge production. The huge energy demands of these treatment facilities
have also furthered the need for alternate wastewater-management techniques that are
economical and necessitate limited energy for operation.
In this veneration, microbial electrochemical technologies (METs) have gained atten-
tion from scholars due to the opportunity to yield energy and valuables such as bioenergy,
hydrogen, etc., from wastewater along with pollution remediation. In 1911, for the first
time, an English botanist Potter expressed the capability of microbes to develop energy
from their dynamic activities. In his study, he measured the potential of a galvanic cell using
Saccharomyces cerevisiae and Escherichia coli, and ascribed his interpretations to the break-
down of organic matter [15]. Further, in 1931 Cohen established that by using necessary
electron acceptors such as potassium ferricyanide, etc., the cell reactions could be sustained,
thereby increasing the cell potential [16]. In the early 1960s, a proof of principle for energy
production via diverse microbes was established that stated that the enzymatic action of
the bacterial culture results in the generation of an overall cell voltage; the term microbial
fuel cell (MFC) was coined for this process [17,18]. Conversely, only in the 1990s did the
MFC-derived technologies, which are frequently mentioned as microbial electrochemical
technologies (METs), attain communal consideration and show increasing signs of progress
in publications due to their inherent advantage of the usage of microbes for value-added
product recovery from waste [19,20].
METs are an amalgamation of technologies that can transform the chemical energy
present in organic matter into electrical energy and valuables such as H2 , acetate, etc. [21].
A typical MET setup consists of two electrodes; namely, the anode and cathode, separated
using a cation or anion exchange membrane (AEM). From an application point of view,
Energies 2022, 15, 9084 3 of 34

METs are categorized as MFCs for the simultaneous wastewater treatment and bioen-
ergy production, as microbial electrolysis cells (MECs) majorly for the production of H2 ,
as microbial desalination cells (MDCs) for desalination along with bioenergy recovery,
as microbial carbon capture cells (MCCs) for carbon sequestration with bioenergy and
biofuel recovery, and as microbial electrosynthesis (MES) for recycling carbon dioxide to
commodity chemicals [22–24].
Usually, the energy generation of METs is majorly associated with the ability of
microbial catalysts to oxidize the organic substrate and discharge electrons. As a result,
the substrate composition and characteristics highly impact the evolution of the bacterial
community and therefore the performance of METs in terms of efficiency and yield of
valuables [25]. Therefore, this state-of-the-art review concisely narrates the practicality of
employing METs as a prospective choice for generating valuables from dairy wastewater,
thus demonstrating a circular economy. Further, it also discusses the challenges involved,
system configurations, and strategies for improving the efficiency of METs to cultivate a
better understanding of this innovative technology among budding researchers. In addition,
the current review article provides information on all the processes involved in a typical
dairy industry as well as the sources and categories of dairy wastewater along with their
characteristics. Moreover, the environmental impact and techno-economic assessment of
METs and future forecasts are also deliberated in this review. To the best of our knowledge,
there is no prior review article that focused on the application of METs for dairy wastewater
treatment. The current review article is compared with other review articles that elucidated
the treatment of different types of wastewater such as petrochemical wastewater in Table 1.
The crystal-clear comparison proves that this review is a comprehensive article that provides
detailed information on different aspects of METs in treating dairy wastewater. Therefore,
there lies a lacuna in exploiting the use of METs for dairy wastewater management, so
the present state-of-the-art review aimed to bridge this by connecting the dots starting
from the origin of dairy wastewater to different treatment procedures employed for dairy
effluent management, including its treatment through METs with concomitant value-added
product recovery. Therefore, this review will serve as a guidebook for researchers and
scientists who work in the domain of METs and the dairy industry that will abet them in
designing a more efficient MET-based wastewater treatment scheme for the dairy industry.

Table 1. Detailed comparison of information covered in different review articles pertaining to the
treatment of different pollutants.

Prevailing Different
Application Environmental
Review Type of Technolo- Electrode Membrane Configura- Integrated Circular
of METs for Impact
Article Pollutant gies for Modifica- Modifica- tion for System Economy
Pollutant Assessment of
Reference Covered Pollutant tions tions Pollutant Approach in METs
Removal METs
Treatment Treatment

[26] Heavy metals No Yes No No No Yes No No

Volatile organic
[27] compounds No Yes No No Yes No No No
(VOCs)
Perchlorate and
[28] No Yes No No No No No No
nitrate
Nitrogen
[29] No Yes No No No No No No
removal
Petrochemical
[22] Yes Yes No No No Yes No No
wastewater
Current
Dairy wastewater Yes Yes Yes Yes Yes Yes Yes Yes
review

2. Characteristics of Dairy Wastewater and Pollutants Present

Water plays a key role in the unit operations of milk processing, including in cleaning,
washing, sterilization, pasteurizing, cooling, heating, and other processes required for the
preparation of dairy products [12,30]. As a result, the dairy industry consumes a huge
amount of water to manufacture milk-based products, which results in an increase in dairy
wastewater generation. Approximately 50–80% of the total water consumed in a dairy
Energies 2022, 15, 9084 4 of 34

factory is transformed into wastewater, which includes sanitary wastewater, whereas the
remaining 20–50% is provisionally clean and can be used for cleaning equipment, watering
lawns, etc. [12]. The amount of wastewater produced by the dairy industry is around
2.5 times higher than the amount of milk processed, and the organic compounds present in
effluent differ according to the composition of the product and the process used therein [12].
Especially in the process of manufacturing ghee, commonly known as clarified butter, the
generated wastewater contains a high amount of carbohydrates and proteins along with
the presence of a higher level of lipids. Furthermore, dairy wastewater is also composed of
nitrogenous compounds as well as other complex organic matter such as carbohydrates,
lipids, and proteins [30]; it also contains soluble and trace organics in addition to suspended
solids [31], which increases the BOD and chemical oxygen demand (COD) of the industrial
effluent. Dairy effluents are whitish in colour and possess a slightly alkaline pH that ranges
from 6.5 to 8.0; however, dairy wastewater can sometimes also be acidic due to the rapid
fermentation of sugar-producing lactic acid in milk [31].
Dairy effluent can be characterized based on the temperature, color, pH, dissolved
oxygen (DO), BOD, COD, dissolved solids, suspended solids, chlorides, sulfate, oil, and
grease. Both the quality and quantity of dairy effluent is largely dependent on the quantity
of milk processed and the type of products manufactured [32]. Wastewater effluent from the
dairy industry comprises hefty quantities of milk ingredients such as casein and inorganic
salts as well as cleansers and sanitisers that are used for washing purposes [31]. As there
is a wide variety of products manufactured in the dairy industry, the characteristics and
quantity of the wastewater generated by a plant also vary considerably [33]. However,
based on the origin and composition of the wastewater, dairy effluent can be divided into
three main categories, which are presented in the subsequent section.

2.1. Processing Water

The processing water is polluted water formed from the cooling of milk in coolers and
condensers as well as condensates from the milk or whey evaporations [12]. Moreover,
while drying milk and whey, vapors are produced. These are among the cleanest dairy
effluents; however, milk or whey droplets, along with volatile substances originating from
evaporators, might also be present in the effluent [32]. In processing water, pollutants
are absent and thus, after negligible pretreatment, it can be discharged with stormwater
or reused to augment the water supply for milk processing [31]. The reuse of treated
wastewater is conceivable in installations that are not in direct contact with the finished
products; it can be applied in hot water and steam production as well as in the cleaning of
the membrane used in the clarification of milk and in the separation of the specific valuable
components from milk and/or dairy byproducts [34]. Further, the water produced from
the cooling of products during pasteurization can be used for the cleaning of rooms, lawn
irrigation, etc.

2.2. Cleaning Wastewater

Cleaning wastewater is produced while washing equipment that is directly in contact
with milk and/or dairy products [12]. Cleaning wastewater contains spillage products.
milk, brine, whey, clean in place (CIP) wastes, and discharges initiated from equipment
malfunctions and operational errors [35]. More than 90% of the organic solids present
in dairy effluent originate from milk and manufacturing residues such as cheese pieces,
cream, whey, water originating from separation and clarification of suspended solids and
color, starter cultures, yogurt, fruit concentrates, or stabilizers [12]. Therefore, appropriate
treatment is required for this moderately polluted cleaning water prior to its reuse or
disposal.

2.3. Sanitary Wastewater

Sanitary wastewater present in dairy wastewater comes from lavatories, shower rooms,
etc., used by staff and workers. The composition of sanitary wastewater is like that of
Energies 2022, 15, 9084 5 of 34

municipal wastewater and is disposed of into the sewerage system directly [12,31]. For
unbalanced dairy effluents before secondary aerobic treatment, sanitary wastewater can be
used as a source of nitrogen [35]. A more detailed discussion of the various processes in-
volved in the dairy industry with their respective wastewater quantities and characteristics
is elucidated in a later section.

3. Environmental Impacts from the Discharge of Dairy Wastewater

Wastewater that originates from dairy industries contains cleaning chemicals such as
nitric acid and sodium hydroxide, milk, and other wastes produced during the different
operations of the dairy industry [31]. These contaminants increase the organic content of
the wastewater and also make it slightly alkaline when fresh and thus are characterized
as having a high organic load (COD in the range of 1500 to 3000 mg/L and BOD5 of 1000
to 1900 g/L), nitrogen content (70 to 100 mg/L), and phosphorus content (10 to 60 mg/L)
that are much higher than the discharge limits [31]. Therefore, dairy wastewater must be
treated efficiently prior to disposal into the environment because it contains a higher load
of harmful substances that can adversely affect the natural ecosystem [12,31,36–38].
The major problem with milk production is that it affects the air, water, and biodiver-
sity, which often causes the growth of algae and bacteria that can consume oxygen from
water bodies and choke rivers, which leads to the gradual disappearance of fishes [39].
Correspondingly, bacteria and other pathogens present in dairy wastewater can spread
harmful diseases such as tuberculosis. Along with these issues, wastewater originating
from the dairy industry also imparts turbidity to the receiving water bodies due to its high
solid content. Milk waste contains significant quantities of soluble organics, suspended
solids, and trace organics that release gases, spread odors, and impart turbidity and color to
the discharged effluents [30,31]. However, the dairy waste should be discharged in a fresh
condition; otherwise, it may cause the corrosion of sewers because dairy waste becomes
acidic via the decomposition of lactose into lactic acid in an anaerobic condition, which
causes rapid DO depletion [40]. In addition to the water streams, dairy effluent also affects
the land because the application of wastewater on the soil is the most common method
of wastewater management followed in the dairy industry. In the process of the disposal
of nitrogen-rich wastewater on the soil, nitrate contamination of the groundwater can
occur; if the groundwater is subsequently used for water supplies, it might be problematic
for humans and can lead to various threatening diseases such as blue baby syndrome,
congenital disabilities, an increased risk of colon cancer, etc. [41].
Similarly, during manufacturing operations, numerous toxic gases such as CO2 , SOx,
NOX , etc., are emitted by the dairy industry into the atmosphere. Emissions of CO2 , SOx,
and NOX into the atmosphere take place from boiler stacks. Further, the emission of
methane can also take place from anaerobic treatment systems and sites irrigated with
wastewater, whereas nitrous oxide is emitted from the soil. In this regard, CO2 , methane,
and nitrous oxide released by the dairy industry are greenhouse gases, which lead to
adverse global consequences. Furthermore, boiler stacks and powder driers also emit
particulate matter, which results in the formation of a dust coating on the surrounding
infrastructures that might be objectionable and corrosive. Smoke and steam plumes from
dairy industries may also be observed and can lead to visual pollution [31,40]. Therefore,
all these adverse environmental impacts that arise from the dairy industry warrant the
employment of appropriate technologies to counter them.

4. Processes from Which Wastewater Is Generated with Characteristics

The dairy industry is a primary food-processing industry that utilizes a large amount
of water in each step of its operation. In the dairy industry, a wide variety of products such
as pasteurized milk, curd, cheese, butter, etc., are processed [42–44]; as a result, a huge
volume of wastewater is generated that is eventually discharged into the environment [3,4].
Therefore, it is important to develop strategies for the treatment of dairy wastewater that
will reduce the stress on the environment that arises due to the discharge of this polluted
Energies 2022, 15, 9084 6 of 34

industrial wastewater. For this reason, it is essential to identify how milk and its products
are processed in the dairy industry as well as and the sources and characteristics of the
wastewater produced at each stage.
Primarily, the processes in the dairy industry are conducted in two major areas: the
milk yield from farmhouses or from producers, which includes the guardianship of cattle
such as cows, buffaloes, etc.; and the milk-processing unit to extend the marketable life
of milk. The processing of milk is the most prominent activity in the production and
packaging of milk. Milk processing is attained through: (a) the pasteurization of milk
to ensure safety for further applications and to extend the shelf life of milk [45]; and (b)
making a wide range of milk foods to store them either in a semi-dried or dried form.
In some parts of the dairy industry in which there is a more than adequate milk supply,
other products such as butter, ghee, whey, cream, ice cream, milk powder, yogurt, cheese,
etc., are also produced [46,47]. Recently, butter and cheese production has been growing
throughout the world and as a result, wastewater generation from the dairy industry is
also on the rise.

4.1. Operations Involved in Milk Processing

A series of processes containing milk reception and storage, processing of milk into
targeted products, packing and storage of finished products, and a set of additional actions
such as cooling and cleaning are a few processes that are carried out in the processing of
milk [2]. The particulars of processes executed in the dairy industry are discussed below.

4.1.1. Milk Reception and Storage

Regardless of the product targeted, every single unit in the dairy industry has a
division in which the milk is transported to the receiving unit and preserved in silos for
further processing. The milk containers are delivered from farms to the receiving unit, then
the contents are emptied into a reception chamber followed by the immediate testing of the
samples. After the milk is delivered, the silos or storage tanks are employed for the storage
of milk for further processing. Milk storage aids in harmonizing the diverse volumes amid
the milk-receiving and -processing stages and thus functions like the equalization tank
frequently employed in a wastewater treatment plant. Typically, stainless steel or fiberglass
storage units with capacities that vary from 20 to 200 m3 are set up outdoors in the industry
for the storage of milk [48]. At this stage, the wastewater arises from the leakages of tanks
and from the washing and disinfection of milk containers, silos, trucks, and pipelines. Most
of the effluent at this phase contains milk solids, detergents, and disinfectants.

4.1.2. Processing of Milk into Dairy Products

In both developed and developing countries such as Europe, North America, India,
etc., milk is pasteurized and further de-creamed using centrifuge machines to isolate the
suspended solids from the milk. Pasteurization is attained by subjecting the milk to a
higher temperature of around 60 ◦ C for 30 min and then cooling it to 4 ◦ C [49]. Next, the
sterilized milk is either sent to a packaging unit for distribution or for further processing to
make dairy products. Butter is another product that is made from churning cream that is
separated from milk by means of centrifugation. However, the process of making butter
is quite varied in developed and developing countries, which can alter the characteristics
of the wastewater generated [50]. During these processes, the wastewater generated by
cooling systems and the cleaning of milk containers, storage units, etc., requires an effective
treatment if reused or to safely dispose of it into water bodies [51].
Cheese is the other dairy product whose manufacturing processes usually includes
several steps such as milk coagulation; cutting, cooking, and molding of curd after draining
the whey; and then hard mold pressing for perfect shaping and packing. The process
of cheese making produces whey, which is the liquid part left in the process; given the
environmental concerns, the whey produced during the curd formation is quite important
due to its high organic and saline content [52]. The quantity of whey varies for distinct types
Energies 2022, 15, 9084 7 of 34

of cheese produced; hard cheese produces a higher amount of whey, whereas soft cheeses
produce either a lower quantity or no whey. Around the globe, there are 500 varieties of
cheese made for different utilization purposes that require different kinds of production
methods [52,53]. Therefore, the characteristic of the effluent during each targeted process
differs according to the different methods used as well as the kind of milk processed.
Ice cream, one of the most famous milk-based desserts, comprises carbohydrates
and fats. In addition, to make ice cream, a few essences or flavorings, sweeteners, and
thickeners are blended with de-creamed milk to form a homogenous mixture [54]. Next,
the mixture is sterilized and chilled and then sent to the packaging unit. Unsweetened
condensed milk is another dairy food that is very thick; to produce unsweetened condensed
milk, the receiving milk is evaporated at elevated temperatures and normalized to produce
condensed milk without sugars. Furthermore, khoa, a prevalent product used to make a
wide variety of sweets on the Indian subcontinent, is typically made via a process of the
thermal evaporation of milk to reach at least 60% of its initial volume [55]. Another product
of the dairy industry is milk powder; to manufacture it, the milk is subjected to vacuum
evaporation followed by spray drying.
As water plays a significant role in all milk-processing operations, the resultant
wastewater is huge in quantity and is almost 80% of the total water consumed in the
dairy industry. In terms of the volume, the wastewater is approximated to be more than
2.5 times that of the milk processed in a factory [12]. In addition, sudden volumetric
variations in effluent are commonly observed in the dairy industry due to the separate
network lines for each milk product. The system of separate network lines can alter the
wastewater composition with the onset of every new operational cycle. Wastewater from
all of the above-mentioned operations is produced during the washing of the units and
the cleaning of the tools employed. Wastewater comprising detergents, cleansers, and
disinfectants is produced during the cleaning of all the production units, which calls for
efficacious treatment of this wastewater prior to its disposal.

4.2. Dairy Effluent Composition

Among the important parameters used in wastewater engineering, dairy wastewater
typically demonstrates a high organic load in terms of BOD and chemical oxygen demand
(COD) that ranges from 0.1 kg/m3 to 100 kg/m3 with an average BOD5 /COD ratio between
0.4 and 0.8. The major contributors to the high organic load in the effluent are carbohydrates
and proteins such as lactose, casein, etc., due to the oozing of milk and dairy products into
wastewater. Moreover, fats ranging from 0.1 to 10.6 kg/m3 and nutrients such as nitrogen
and phosphorus are also prevalent in dairy wastewater [52]. The key factors that influence
the composition and concentration of dairy wastewater are the operations performed, the
processing of different dairy products, the water-management strategies implemented, and
the design of the dairy industry. Typically, the dairy industry uses the CIP scheme for
washing equipment and tools by employing caustic soda, sodium hypochlorite solutions,
acids such as nitric acid, etc.; all of these chemicals end up in the wastewater [3]. These
reagents affect the quantity and pH of the wastewater and also contribute about 10% to
the wastewater COD. Further, the inclusion of different operations such as cheese making,
butter production, etc., in a factory can result in the production of wastewater with varied
characteristics. However, dairy effluent can be majorly divided into three main categories
based on its source and contents; these will be described subsequently.
A huge amount of water is employed in chilling warm milk or other dairy products
by means of condensers or chillers, which results in the formation of process water. This
process water also includes the condensates produced after the evaporation of milk or
whey at various stages. These condensates, which are one of the least polluted wastewaters
generated in the dairy industry, contain a few dairy drops collected from evaporators along
with a few volatile compounds such as decanoic acid, octanoic acid, etc. [42,56]. Broadly
speaking, the process water contains negligible organic contaminants and with minimum
pretreatment, the effluent can either be reused for chilling or can be safely discharged into
Energies 2022, 15, 9084 8 of 34

the environment. Classic reuses this water include the production of steam and washing of
membranes used in membrane separation processes such as reverse osmosis, nanofiltration,
etc. [57]. Further, the liquid used for the chilling of products throughout the sterilization
and the condensates produced during thermal evaporation can be reused for irrigation,
cleaning of rooms, etc. [58].
Cleaning wastewater commonly originates from scrubbing and cleaning apparatus
and tools that are in contact with milk or processed food. Cleaning wastewater consists
of CIP discharges; milk and dairy product residues such as cheese, yogurt, etc.; and some
byproducts such as whey or whey permeates that are formed during cheese making. More
than 90% of the cleaning effluent comprises milk because the loss of milk during operations
is 2.5% of the processed milk and sometimes can be as high as 4% [2]. This wastewater
is generated in huge volumes and is highly contaminated with organics and nutrients;
therefore, it requires an effective treatment before disposal.
Sanitary wastewater in the dairy industry is the wastewater released from sanitary
conveniences such as toilets, lavatories, etc. It is pumped out into the sewage-collection
system because it has similar characteristics to those of municipal wastewater. Further,
sanitary wastewater can be employed as a nitrogen source to balance the nitrogen deficit
present in dairy wastewater when it is subjected to aerobic treatment. However, in an
investigation by Danalewich and co-workers, a survey of a few milk-processing plants in
various places in the USA, such as Minnesota, South Dakota, etc., regarding the mixing
of both sanitary and dairy wastewater was conducted [59]. The study proved that the
separation of sanitary wastewater from dairy wastewater during treatment assisted in
reducing the concern with the disposal of produced sludge that contained pathogenic
microbes. Hence, it is advisable to separate sanitary wastewater from dairy wastewater
and opt for onsite treatment of the same.
The other option for effective dairy wastewater treatment could be to incorporate a
separate collection system for byproducts such as whey and whey infiltrates, as they are
the primary pollutants of the industry [60,61]. The critical contaminant in dairy effluent
is the whey produced during cheese making, which is remarkably high in both organic
and volumetric load. Thus, whey being a nutrient-rich effluent can cause eutrophication
and excessive oxygen depletion when released into the environment without appropriate
treatment. Typically, whey alone comprises lactose of around 4–5%, proteins and lactic acid
together of around 1%, fats of less than 0.5%, and a varied salt content of 1.5 to 3% [12,62].
Since the BOD5 /COD ratio for whey is higher than 0.5, whey can be treated using biological
processes. However, without a proper control of biological processes employed for whey
treatment, the decomposition of proteins can result in a foul odor. Therefore, understanding
the characteristics of milk and dairy products can abet a better estimation of the organic
load present in dairy wastewater and further guide in designing the required treatment
units. Although dairy plants produce wastewater that is equivalent in characteristics to
the milk and dairy products manufactured, every single process discharges effluent with
unique characteristics and quantity, which calls for a specially designed treatment scheme
prior to its disposal (Table 2).
Among the vital parameters, an optimal pH for effective wastewater treatment is
imperative. Though most of the operational units in the dairy industry produce neutral
pH effluents, the plants with a whey discharge tend to create wastewater with an acidic
pH of less than 6, which is due to the acidic coagulation process incorporated in cheese
making, from which whey is generated as a byproduct. Further, if a sudden hike in pH
up to 10 is observed in the effluent, it can be attributed to the discharge of detergents and
disinfectants after cleaning the equipment. Further, a longer retention of dairy effluents in
the sewerage system creates an anaerobic environment, which helps in the fermentation of
lactic acid, thus resulting in a reduction in pH from basic to acidic.
Energies 2022, 15, 9084 9 of 34

Table 2. Characteristics of dairy effluent at various stages of milk processing.

Stages in
the BOD5 COD TSS
Sources of Wastewater pH TN (g/L) TP (g/L) References
Processing (g/L) (g/L) (g/L)
of Milk
a. Poor drainage facility
Milk
b. Cleaning of units
receiving 7.18 0.8–5 2.54–10 0.65–3 - - [43,45]
c. Spillage and overflows
stage
d. Foaming
a. Vacreation process
(pasteurisation by
vacuum methods)
Butter
b. Use of salts increases 0.22– 8.93–
production 12.08 0.7–5.07 - - [45,63]
salinity and ions such as 2.65 10.2
process
Na+ and Cl−
c. Cleaning and washing
operations
a. Whey separation
b. Cleaning and washing
operations
Cheese c. Usage of salts tends to
3.38-9.5 0.59–5 1–63.3 0.19–2.5 0.018–0.83 0.005–0.28 [45,50,64]
making increase ionic
concentration and
suspended solids
d. Spillages and leaks
a. Plant and tank
Ice cream clean-up
production b. Backflushing water 5.1–6.96 1.8–2.45 4.94–5.2 1.1–3.1 0.014–0.06 - [43,62,65]
process c. Pasteurizer and chiller
flush-out
BOD5 : 5-day biochemical oxygen demand, COD: chemical oxygen demand, TSS: total suspended solids, TN: total
nitrogen, TP: total phosphorus.

The presence of higher settleable solids, which arises mostly from butter and cheese-
making processes in the dairy industry, might also result in the clogging of sewage pipes. In
addition, the molecular protein formation and deposition of fats along the walls of the pipes
that carry dairy wastewater requires regular cleansing with necessary chemical solutions.
This increases the maintenance cost of the conveyance system that is employed for the
transportation of dairy effluent. Furthermore, different concentrations of total nitrogen
(TN) and total phosphorus (TP) are also observed in distinct types of dairy wastewater due
to the existence of amino acids and inorganic phosphates in milk. However, the presence of
these levels of TN and TP values are dependent on biological processes; thus, METs can
also be employed for the treatment of dairy wastewater with the concomitant recovery
of valuables.

5. Current Treatment Approaches for Dairy Wastewater

Dairy wastewater significantly affects the quality of the receiving environment due to
the high volume of the effluent, which is loaded with heavy organic loads and has a fluctu-
ating pH. These issues entail effective and economic effluent-management technologies that
can safeguard the environment. In this regard, the present section elucidates the application
of various chemical, physicochemical, and biological processes for the treatment of dairy
effluent.

5.1. Chemical Treatment

Chemical treatment is executed by adding oxidants to dairy effluent and then blend-
ing it vigorously using rapid mixers. Chemical treatment employs either oxidation of
Energies 2022, 15, 9084 10 of 34

the targeted pollutant using reagents or pH alteration to facilitate removal. When FeSO4
and H2 O2 were used as chemical reagents to treat cheese wastewater, an 80% fat-removal
efficiency was obtained with an initial fat concentration of 1.93 g/L [66]. An extreme pH of
the dairy effluent of under 6.5 or over 10 can accelerate the deterioration of piping tubes
and can be highly pernicious to the microbiome employed in biological procedures. Thus,
this extreme pH must be adjusted to diminish these repercussions. In the case of using dis-
solved air flotation, pH regulation is an obligatory stage to attain the optimum results [67].
Nevertheless, coagulants perform outstandingly in lower pH environments, which necessi-
tates a consequent pH tuning to the required level before additional treatment [12]. Due to
the use of chemicals for dairy effluent treatment, it is always appropriate to employ self-
reliantly utilized CIP effluents and discharge them continuously in an effluent-treatment
plant. Although the contaminants are removed efficiently in this mode of treatment, the
accumulation of sludge creates a significant problem, and the prerequisite of chemicals also
makes the treatment quite expensive [42,68].

5.2. Physicochemical Processes

Physicochemical processes such as coagulation–flocculation, adsorption, membrane
technologies, etc., emphasize the removal of colloidal substances from dairy wastewater.
Some physicochemical techniques employed for the treatment of dairy wastewater are
discussed below.

5.2.1. Coagulation–Flocculation
Coagulation and flocculation are employed to eliminate suspended, colloidal, and
dissolved materials from dairy effluent. These processes aid in precipitating inexplicable
compounds such as phosphate as a mode of tiny constituent parts, which then bulk into
bigger flocs. The bulkier flocs settle in clarifiers as a core sludge, while clear seepage
is discharged into other reactors for subsequent treatment. This phase decreases the
suspended and colloidal constituents that are accountable for the turbidity of the liquid and
aids in decreasing the organic matter, thus diminishing the COD and BOD [69]. Usually,
coagulation in dairy effluent can be accomplished via explicit lactic acid microbes. These
microbes help to ferment the lactose, thereby converting the lactose into lactic acid and
lowering the pH, which concentrates the proteins with the combination of flocculants,
causing the denaturation of water-soluble proteins in the dairy effluent. In this regard,
different coagulants such as chitosan, carboxymethylcellulose, etc., were employed to
enhance the coagulation process. A study reported that the use of chitosan achieved a
COD removal efficiency of 82%, whereas the employment of carboxymethylcellulose as
a coagulant obtained a COD reduction of around 78% [70]. However, irrespective of the
excellent removal efficiencies obtained, the higher sludge generated and the requirement
of chemicals for pH adjustment makes the technology of coagulation and flocculation
ineffective for treating dairy wastewater.

5.2.2. Adsorption
Amid the various physicochemical approaches, adsorption remains a unique method
for eliminating organic matter from dairy effluents. For effective dairy wastewater treat-
ment, activated carbon (AC) is utilized the most compared to other adsorbents due to its
high surface area and possession of excellent porosity. However, a few other adsorbents
such as fly ash that are economical can also be employed in the treatment of dairy effluent.
Rao et al. applied powdered AC (PAC) as an adsorbent for dairy-wastewater treatment
and compared it with different low-priced adsorbents such as straw dust, coconut coir,
etc., to lower the total solids concentration [71]. Another study reported a maximum COD
removal efficiency of 92.5% using rice husk as an adsorbent to treat dairy wastewater with
a dose of 5 g/L at an acidic pH of 2 [72]. Moreover, the downside of adsorption processes
such as the separation of the adsorbent from the pollutant, a weak selectivity, and an excess
Energies 2022, 15, 9084 11 of 34

generation of waste products has led researchers to deeply question the applicability of
this technology for dairy-wastewater management.

5.2.3. Electrocoagulation
Electrocoagulation (EC), which can be another practical alternate approach to treat-
ing dairy wastewater, has recently gained a great deal of consideration due to its easy
installation and functioning and lack of chemical requirements. The technology of EC
involved the development of an electrolysis method that aids in the removal of soluble
organic matter, turbidity, colloidal matter, and color through the passage of electric current
through the dairy wastewater via electrodes. Sengil et al. applied the EC method to remove
COD and oil/grease from dairy effluent using mild steel electrodes and obtained COD
and oil/grease removal efficiencies of 98% and 99% with a pH and electrolysis time of 7
and 1 min, respectively [73]. Another study outcome specified that EC could effectively
attain removal efficiencies of 98.8%, 97.9%, and 97.75% for COD, BOD, and TSS using
dairy effluent, respectively, with 60 V of applied cell potential in 60 min of reaction time
with aluminium electrodes [74]. Although this method is an effective solution for treating
dairy wastewater, this technology has a few significant drawbacks such as higher energy
requirements and recurrent restoration of electrodes to minimalize the formation of the
passivation layer, which elevates both its operative and maintenance costs.

5.2.4. Membrane Treatment Technologies

Membrane technologies such as microfiltration, nanofiltration, ultrafiltration, reverse
osmosis, and electrodialysis have appeared as alternative treatment technologies for manag-
ing dairy effluent due to higher pollutant removal efficiencies with no additional chemical
requirements. A higher degree of targeted-pollutant removal can be achieved with the
operations mentioned above, and the final effluent generated is of an excellent quality that
can be used straight in the process, thus exemplifying a zero-liquid discharge. Frappart
et al. described that the recovery of lactose and milk proteins and an ion reduction of up
to 80% was possible using dynamic nanofiltration equipped with a rotating disc unit [75].
Another study reported the treatment of dairy wastewater by employing RO; a maximum
of 90 to 95% water recovery was accomplished with a permeate flux of 11 L/h.m2 and a
concomitant 99.8% total organic carbon removal [76].
Recently, a study by Kumari et al. was aimed at improving the water recovery
rate via the comprehensive elimination of organic matter and total solids from dairy
effluent with a membrane bioreactor (MBR) [77]. The study achieved removal efficiencies
of 99.8%, 98%, 40%, 80%, and 98.7% for COD, BOD, total dissolved solids, NH4 -N, and
PO4 3- , respectively, via the integration of MBR with a polyvinylidene membrane [77].
Therefore, the above-mentioned study emphasized the fact that membrane technologies
can be operative in removing contaminants from dairy effluent. Nevertheless, despite the
effectual management of dairy wastewater with membrane operations, the fouling and
scaling of membranes disturbs the enduring steadiness of the membranes and results in a
further rise in the maintenance cost of the process.

5.3. Biological Treatment

The consistent treatment approaches for dairy wastewater are microbial methods that
can adapt to all dairy wastewater constituents, but they still prevalently use solvable com-
posites and minor colloids as a substrate, hence removing them from the wastewater [36].
Furthermore, due to their wild adaptation abilities, these methods can be conjointly em-
ployed with several arrangements for the effective component-degradation needs [42,78].
Biological-treatment processes have two different classifications based on oxygen supplies:
aerobic and anaerobic processes, both of which are employed in the treatment of dairy
wastewater.
Currently, many dairy-effluent-treatment units are adapting aerobic processes; how-
ever, these are not highly effective, mostly due to the filamentous development and
Energies 2022, 15, 9084 12 of 34

quick acidification triggered by greater lactose values and lower aqua-buffering capa-
bilities [52,68,79]. The difficulties usually met in activated sludge processes (ASPs) are
the bulking of sludge, sludge foaming, ionic precipitation, extra biomass generation, and
inefficient treatment efficiency at colder temperatures. The sharp O2 exhaustion (greater
than 3 kg of oxygen required per kg of BOD5 consumed) necessitates enormous energy
requirements throughout the aerobic treatment of dairy effluent [42]. A study reported
that when synthetic dairy wastewater with an initial concentration of 4 g/L of COD was
treated using an ASP in continuous mode, a COD removal efficiency greater than 96%
was obtained, which provided an optimistic response [80]. Another study done by Russell
revealed that with the use of a milk–butter mixture effluent for an ASP, reliable COD and
TN removals of more than 90% and 65% could be achieved [81]. However, to improve the
removal efficiency of an aerobic system, an appropriate pretreatment or acceptable effluent
dilution needs to be provided.
A sequencing batch reactor (SBR) is often chosen to treat dairy wastewater due to
its extravagant loading abilities and flexible nature in treating wide varieties of effluents.
The management of dairy wastewater was demonstrated by Britz et al., who reported
that maximum COD and TN removal efficiencies of 97% and 38%, respectively, could be
obtained via an SBR [42]. Further, a recent examination demonstrated that the SBR is a
notable technology for merging the activated-sludge granulation in the management of
milk effluent. Maximum removal efficacies of 90% for COD, 80% for TN, and 67% for TP
were obtained in an eight-hour reaction time for soluble dairy effluent [82].
Anaerobic approaches are very appropriate for the treatment of complex dairy effluent
and are also very economical than aerobic systems. If suitably operated, these processes
do not generate any undesirable smells, which increases their applicability in residential
areas [42,68]. The primary complications of anaerobic processes comprise an extensive start-
up time due to the presence of complex matter; the performance and generation of methane
are affected by pH variation, sludge floating, etc. [83,84]. Nevertheless, the evidence on the
industrial-level application of anaerobic processes using whey wastewater revealed a COD
removal efficacy of about 75% at around a 10 kg/day.m3 organic-loading rate.
Dairy wastes are treated in traditional single-phase anaerobic processes such as in
an upflow anaerobic sludge blanket (UASB) reactor. Earlier, lab-scale UASB reactors for
cheese whey permeate treatment were designed and employed for an effluent with an
initial COD ranging between 0.2 and 10.4 g/L of wastewater under a hydraulic retention
time (HRT) of 0.4 to 5 days [85,86]. A comparative investigation of the prospect of flocculent
sludge with granular sludge under diverse HRTs between 6 and 16 h on a UASB was made;
approximately 80% of COD and VFA removal for each and an almost 60% fat removal were
obtained with the flocculant sludge at an HRT of 12 h [87].
The above deliberation exposed that there are critical restrictions for different treat-
ment technologies such as EC, as they need an extremely conductive effluent in order
to minimalize the ohmic resistance between the cathode and anode to bring down the
energy consumption for an efficient performance. Likewise, membrane scaling, fouling,
and maintenance costs are the main disadvantages of membrane-based techniques (Table 3).
Therefore, to circumnavigate these bottlenecks, minimal energy-concentrated and effective
technologies such as METs are mandatory for generating the self-sustainable energy associ-
ated with value-added product retrieval. Like MFCs, METs possess a smaller land footprint
when compared to ASPs, and self-sustainable usable energy also can also be yielded with
MFCs. Furthermore, compared to EC, in which toxic intermediates can be generated, METs
have been proven to be amazingly effective in the overall mineralization of pollutants.
Hence, METs can be used as a credible counterfeit of the existing treatment options for the
treatment of milk-processing effluent.
Energies 2022, 15, 9084 13 of 34

Table 3. Treatment of dairy wastewater using different treatment techniques.

Treatment Technology Process Conditions Treatment Efficiency Drawbacks Reference

Polyacrylamide and polyferric • Chemical requirement

Coagulation and 95% turbidity removal
sulfate as coagulants, pH = 7.5, • Sludge management [88]
flocculation 82% COD removal
coagulant dose = 20 mg/L

Synthesized copper oxide • Weak pollutant

nanoparticles coupled with selectivity
Sophora Japonica fruit as 77 to 95% COD • Separation of
Adsorption [89]
adsorbent, contact time = removal pollutants from the
120 min, temperature = 25 ◦ C, adsorbent
pH = 7.5, adsorbent dose = 1 g/L

Six aluminium electrodes in • Higher energy

98.84% COD removal requirement
parallel connection, voltage
Electrocoagulation 97.95% BOD5 removal • Passivation layer on [74]
input = 60 V, maximum current
97.75% TSS removal electrodes
= 5 A, HRT = 60 min

• Membrane scaling
RO membrane area = 540 m2 , • Fouling of
95% Water recovery membranes
Reverse osmosis transmembrane pressure = [76]
99.8% TOC removal • Higher maintenance
20 bar
costs

MBR with PVDF membrane of 99.8% COD removal • Higher capital and
0.2 to 0.3 µm pore size, water 98% BOD5 removal operational costs
Membrane bioreactor flux = 4 to 7 L/h, HRT = 6 h, 40% TDS removal • High membrane [77]
organic loading = 20 to 22 g/L, 80% NH4 -N removal cleaning and
pH = 6.5–7 98.7% PO4 removal replacement costs

80.2% COD removal • Higher oxygen

63.4% TS removal requirement
Sequencing batch Initial COD = 20,000 mg/L, • Sludge bulking
66.2% VS removal [90]
reactor HRT = 2 days • Poor activity at low
75% TKN removal
38.3% TN removal temperature

• Long start-up period

Organic loading rate = 6.2 g • Extensive pH
Upflow anaerobic variations
COD/L.day, reactor volume = 98% COD removal [85]
sludge blanket reactor • Improper sludge
10 L, HRT = 6 day
settling

BOD5 : 5-day biological oxygen demand, COD: chemical oxygen demand, TSS: total suspended solids, TN: total
nitrogen, TP: total phosphorus, TOC: total organic carbon, TDS: total dissolved solids, TS: total solids, VS: volatile
solids, TKN: total Kjeldahl nitrogen, NH4 -N: ammonium nitrogen, PO4 3− : phosphate, HRT: hydraulic retention
time.

6. Microbial Electrochemical Technologies: Introduction and Working Principle

The METs are promising innovative technologies that employ microbes to catalyze
different electrochemical reactions to produce value-added products from different waste
streams [91]. The different variants of METs that are employed to recover valuables from
waste are MFCs, MECs, microbial desalinization cells (MDCs), and MCCs. In METs,
wastewater that is rich in organics is used as the fuel or substrate by the anaerobic microbes
residing on the anode, whereas oxygen is used as the terminal electron acceptor that facili-
tates the oxygen-reduction reaction in the cathodic chamber [92]. The microbes cultured in
METs are electroactive in nature, and those that transfer electrons to the anode are known
 Energies 2022, 15, 9084 14 of 34

as exoelectrogens; these microbes function as biocatalysts for the conversion of waste

to valuables [93]. The inventive METs possess the potential to synthesize several types
of valuables such as bioelectricity, hydrogen, methane, biofuels, etc., with concomitant
wastewater treatment or brackish-water desalination [94]. As a result, these technologies
have drawn considerable attention from researchers due to their inherent demonstration of
a circular economy by converting waste into resources. A more detailed explanation and
the working principle of diverse types of METs are elucidated subsequently.

6.1. Microbial Fuel Cell

An MFC is a promising technology that exemplifies wastewater treatment with simul-
taneous bioelectricity production by converting the chemical energy present in the chemical
bonds of organic matter present in wastewater directly to bioelectricity with the assistance
of the catalytic activities of microorganisms [95]. A typical MFC consists of two chambers,
namely the anodic and cathodic chambers, which are partitioned by a proton-exchange
membrane (PEM). The electrodes housed in the respective chambers are connected via
an external circuit through which reusable electricity can be harvested [92]. The microbes
present in the anodic chamber produce electrons and protons from the organic matter
present in the wastewater. The electrons are transferred to the cathodic chamber via the
external load, thus completing the circuit. On the other hand, the protons produced in the
OR PEER REVIEW anodic chamber pass through the PEM that separates the chambers and reach15the of cathode.
36
In the cathodic chamber, the protons and electrons combine with oxygen, which leads to
the formation of water through an oxygen reduction reaction (ORR) (Figure 1) [96].

Figure 1. A schematic diagram of a typical dual-chamber microbial fuel cell.

Figure 1. A schematic diagram of a typical dual-chamber microbial fuel cell.
The anodic microbes in an MFC are strictly anaerobic in nature and as a result, the
presence
The anodic microbes in of oxygen
an MFC in the
areanodic chamber
strictly can inhibit
anaerobic the generation
in nature and as of electricity;
a result, however,
the
aerobic conditions must be maintained in the cathodic chamber to facilitate the ORR [97].
presence of oxygen in the anodic chamber can inhibit the generation of electricity; how-
The oxygen required for the ORR is provided in either an aqueous form (in the case of
ever, aerobic conditions
aqueousmust be maintained
cathode MFC) or can be in consumed
the cathodicfromchamber to as
the air (such facilitate the ORRMFC
in an air-breathing
[97]. The oxygen required for the ORR
or single-chamber MFC)is provided
[98]. in either
This emerging an aqueous
technology of the MFCform (inemployed
can be the casein the
of aqueous cathodedairy
MFC) industry
or can forbe
theconsumed
treatment of dairy
fromeffluent
the airin(such
the anodic
as inchamber, which will reduce
an air-breathing
the organic
MFC or single-chamber MFC) load[98].
that reaches the subsequent
This emerging treatment unit,
technology of thethusMFC
reducing
canthebeoperational
em-
costs [99]. Further, the energy recovered from the operation of an MFC that employs dairy
ployed in the dairywastewater
industry can forbethe treatment
used to provideof dairy effluent
electricity to low-power in the anodic
sensors, which chamber,
are employed
which will reduce the
in quality controls [100]. The technology of the MFC possesses the advantage ofre-
organic load that reaches the subsequent treatment unit, thus power
ducing the operational costsfrom
recovery [99]. Further,
waste; the the
however, energy
amountrecovered
of power from the via
recovered operation of an for
MFCs is inferior
MFC that employs dairy wastewater can be used to provide electricity to low-power sen-
sors, which are employed in quality controls [100]. The technology of the MFC possesses
the advantage of power recovery from waste; however, the amount of power recovered
 Energies 2022, 15, 9084 15 of 34

medium/large-scale applications, and the exorbitant fabrication cost of scaled-up MFCs

makes this technology infeasible for practical applications [101]. Hence, to commercialize
this novel technology, researchers are toiling hard to synthesize low-cost electrode and
membrane materials that would not only reduce the capital investment, but would also
improve the power generation of a scaled-up MFC.

6.2. Microbial Electrolysis Cell

A MEC is a derivative of the MFC that is employed to produce hydrogen, methane,
hydrogen peroxide, etc., from the organic matter present in wastewater, with the application
of a minute amount of imposed potential depending upon the targeted product [102]. The
operation of the anodic chamber of an MEC is like that of a MFC, in which electrons
and protons are produced during the decomposition of the organic matter present in
wastewater [102]. The electrons from the anodic chamber are drawn to the cathodic
Energies 2022, 15, x FOR PEER REVIEW 16 of 3
chamber via an externally connected potentiostat; the protons reaching the cathode through
the PEM are reduced by these electrons to produce hydrogen (Figure 2).

Figure2.2.AAschematic
Figure diagram
schematic of a of
diagram microbial electrolysis
a microbial cell. cell.
electrolysis

If suitable cathode catalysts and catholyte are employed in an MEC, other value-
If suitable cathode catalysts and catholyte are employed in an MEC, other value
added products such as hydrogen peroxide, acetic acid, etc., can be produced through this
added products
innovative such[103].
technology as hydrogen
A scaled-upperoxide,
MEC can acetic acid, etc.,
be installed candairy
in the be produced
industry through
that thi
innovative technology [103]. A scaled-up MEC can be installed in the
could treat the effluent in the anodic chamber with concurrently produced hydrogen or dairy industry tha
couldcommodity
other treat the chemicals
effluent in the These
[104]. anodic chamber
products canwith concurrently
be further used in theproduced hydrogen o
dairy industry
otherthus
itself, commodity chemicals
exemplifying [104].
a circular These [105].
economy products can bethe
However, further used of
technology inthe
theMEC
dairy indus
also suffers from similar drawbacks to those of MFCs, which include
try itself, thus exemplifying a circular economy [105]. However, the technology inferior yields of of th
valuables and higher fabrication costs; hence, researchers are attempting to circumnavigate
MEC also suffers from similar drawbacks to those of MFCs, which include inferior yield
these drawbacks
of valuables andbyhigher
integrating other biotechnologies
fabrication with MECs. are attempting to circumnav
costs; hence, researchers
igate
6.3. these drawbacks
Microbial byCell
Desalinization integrating other biotechnologies with MECs.
An MDC is a type of MET that is primarily employed for the removal of salts from
6.3. Microbial
brackish water Desalinization
with concomitantCellwastewater treatment and bioelectricity recovery [106].
An MDC
Typically, an MDCis aconsists
type ofofMET
threethat is primarily
chambers with anemployed
additional for the removal
desalination of salts from
chamber
sandwiched between the cathodic and anodic chambers (Figure 3) [107].
brackish water with concomitant wastewater treatment and bioelectricity recovery [106]
Typically, an MDC consists of three chambers with an additional desalination chambe
sandwiched between the cathodic and anodic chambers (Figure 3) [107].
 6.3. Microbial Desalinization Cell
An MDC is a type of MET that is primarily employed for the removal of salts from
brackish water with concomitant wastewater treatment and bioelectricity recovery [106].
Typically,
Energies 2022, 15, 9084 an MDC consists of three chambers with an additional desalination chamber
16 of 34

sandwiched between the cathodic and anodic chambers (Figure 3) [107].

Figure 3. A schematic diagram of a microbial desalinization cell.

Figure 3. A schematic diagram of a microbial desalinization cell.
The working principle of the anodic and cathodic chambers of an MDC is similar to
The working that
principle of the
of an MFC; anodic
however, the and cathodic
movement chambers
of ions of an MDC
from the additional is similar
desalination to
chamber
to the anodic and cathodic chambers is the only difference [108]. The AEM separates
that of an MFC; however, the movement of ions from the additional desalination chamber
the anodic chamber from the desalination chamber, which also facilitates the movement
to the anodic and cathodic chambers
of anions from is thewater
the brackish onlypresent
difference
in the [108]. The AEM
desalination separates
chamber the
to the anodic
anodic chamber fromchamberthe [109].
desalination chamber,
Alternatively, which alsomembrane
the cation-exchange facilitates the that
(CEM) movement of
separates the
cathodic chamber from the desalination chamber facilitates the
anions from the brackish water present in the desalination chamber to the anodic chamber movement of cations from
the brackish water present in the desalination chamber to the cathodic chamber, thus
[109]. Alternatively, the cation-exchange membrane (CEM) that separates the cathodic
demonstrating the successful desalination of the brackish water [110]. Instead of a single
desalination chamber, an MDC can have multiple desalination and concentrate chambers
to increase the quantity of saline water getting treated; however, in that case, the internal
resistance of the system rises, thus considerably affecting the power generation [105]. An
upscaled MDC can be employed in the dairy industry to treat saline water before sending
it to the RO system, thus increasing the longevity of the RO membranes. However, the
build-up of salinity and pH in the concentrate chamber, membrane fouling, and a lower
yield of bioelectricity are also some of the major challenges in the use of this technology.

6.4. Microbial Carbon Capture Cell

An MCC is a modified version of an MFC in which carbon capture is accomplished by
algae cultured in the cathodic chamber of the MCC [111]. Further, these algae growing in the
cathodic chamber can be harvested to produce biodiesel and other valuable products such
as carotenoids [112]. The anodic chamber of an MCC functions similarly to that of an MFC;
however, in the cathodic chamber, algae provide the oxygen required for the ORR instead
of the external aeration used in MFCs (Figure 4) [113]. An MCC can be employed to remove
the nutrients present in dairy effluent by using them for the growth of algae, which can
produce biodiesel when harvested; this produced biodiesel can be further used to produce
in-house power in the dairy industry [114]. An MCC can demonstrate carbon capture
and sequestration by capturing CO2 from the dairy emissions, which also aids in tackling
global warming, climate change, and air pollution [115]. However, culturing of algae
via industrial effluents, sluggish reduction kinetics, and an inferior yield of byproducts
are some of the major challenges of this technology that must be overcome prior to its
successful commercialization.
 ther used to produce in-house power in the dairy industry [114]. An MCC can
strate carbon capture and sequestration by capturing CO2 from the dairy emissions
also aids in tackling global warming, climate change, and air pollution [115]. H
culturing of algae via industrial effluents, sluggish reduction kinetics, and an inferi
Energies 2022, 15, 9084 of byproducts are some of the major challenges of this technology that17 must
of 34 be ov
prior to its successful commercialization.

Figure 4.4.AAschematic
Figure diagram
schematic of a microbial
diagram carbon capture
of a microbial carboncell.
capture cell.
7. Dairy Wastewater Treatment Utilizing METs
7. Dairy Wastewater
Recently, Treatment
the concurrent Utilizing
dairy wastewater METsand energy production by METs
treatment
have Recently,
fascinated investigators and have
the concurrent massive
dairy considerations.
wastewater METs areand
treatment an exceptional
energy produc
technology that integrates biotic and electrochemical pathways for simultaneous dairy
METs have fascinated investigators and have massive considerations. METs are an
effluent management with simultaneous energy generation and recovery of valuables such
tional technology
as H2 [116]. that the
In this context, integrates
subsequent biotic and
section willelectrochemical pathways
elucidate the comprehensive for simul
mech-
dairy
anismseffluent management
and applications of diversewith
METs simultaneous energy
for dairy-effluent generation
management. and recovery
Depending on o
the configuration, function, and type of valuables produced, METs are further
bles such as H2 [116]. In this context, the subsequent section will elucidate the com categorized
into MFCs, MECs, and MDCs. The term MXC was newly composed for the technologies
sive mechanisms and applications of diverse METs for dairy-effluent managem
mentioned earlier, where X denotes the diverse categories of METs and their operations [19].
pending on the
In recent years, theconfiguration, function,
notion of MES, which andmode
is another typeofofmicrobial
valuables produced,was
electrocatalysis, METs are
categorized into
familiarized for MFCs,
carbon MECs,
dioxide and toMDCs.
recycling valuableThe term MXC
commodity was The
products. newly composed
process
adopted in MES is quite the opposite of MFCs, in which the oxidation of organic matter
triggers the microbial transfer of electrons to an anode. Therefore, an MES does not generate
electricity but produces valuable chemicals along with the microbial conversion of CO2
through the electrotrophic microbes cultured in the cathodic chamber of the MES [21].
Numerous operative variations between these METs varieties can be recognized and are
deliberated with their features below (Table 4).

7.1. MFCs for Bioelectricity Generation using Dairy Effluent

MFCs typically use microbes as biocatalysts to change the form of the chemical energy
to electrical energy through degradation of the organic matter present in the wastewater.
As an evolving process, MFCs are getting an incredible amount of attention because their
potential contribution to simultaneous power generation and treatment of wastewater
such as dairy effluent is comprehended. In this regard, the treatment of dairy industry
effluent was perceived in a catalyst-less and mediator-less membrane MFC (CAML-MMFC).
A maximum coulombic efficiency and voltage of 37.16% and 0.856 V, respectively, were
achieved at a corresponding organic loading rate (OLR) equal to 17.74 kg COD/m3 .day
and 53.22 kg COD/m3 .day with five days of HRT through the CAML-MMFC [117]. During
another investigation, real dairy wastewater with 8000 mg/L of initial COD was fed
continuously in a single-chamber MFC with a 0.2 L working volume for 15 days. In
the investigation, the maximum current density and power density were observed to be
141 mA/m2 and 50 mW/m2 , respectively, with a simultaneous COD removal efficiency of
92.21% [1].
Energies 2022, 15, 9084 18 of 34

In a fascinating study, a single-chamber MFC inoculated with a mixed culture was fed
with real dairy wastewater and operated continuously for 264 h. The system demonstrated
outstanding results with a coulombic efficiency of 31.58% and a maximum COD removal
efficiency of 95.31%. The peak power density and optimum cell voltage of the MFC were
shown to be 62.27 mW/m2 and 0.48 V, respectively [5]. Similarly, dairy effluent was used
as the substrate to understand the long-term performance of an air-cathode single-chamber
MFC that was operated for 95 days. The maximum removal efficiencies for COD and
nitrate of the MFC were observed to be 93% and 100%, respectively, along with a power
density of 0.48 W/m3 [118]. Therefore, these investigations proved that the MFC provides
a multifaceted waste-handling opportunity for dairy effluent; nevertheless, additional
research needs to be performed that focuses on the advances in affordable and steady
electrocatalysts to improve the lethargic oxygen reduction reaction (ORR) kinetics, which
would further enhance its energy generation.

7.2. MECs for Simultaneous H2 Evolution and Dairy Wastewater Treatment

The use of MECs is a new-fangled processes that aids in the oxidation of organic
compounds with the assistance of exoelectrogenic microorganisms that exist in the anodic
compartment to generate H2 , H2 O2 , etc. [21]. Nevertheless, the production of H2 via a
reduction process is not spontaneous due to the lower reduction potential; hence, MECs
necessitate an external voltage source > 0.2 V of external potential for the reduction reaction
to take place [101]. Furthermore, CH4 is frequently found in MECs with H2 generation due
to the reception of electrons by electromethanogenic microbes in the cathode compartment
if functioning in biotic environments. Moreover, if suitable metallic catalysts are employed
in MECs, chemicals such as H2 O2 can also be recovered that can be directly used in
the industry.
With the increasing global energy demand, the utilization of biofuels can diminish the
ingestion of non-renewable fuel sources, thereby lowering greenhouse gas emissions and
eventually limiting global warming and the associated climate change [119]. Henceforth,
the evolution of alternate energy sources is imperative for self-sustainable development
and the attainment of sustainable development goals. In a prior investigation, a single-
chamber MEC was fed with dairy wastewater with 6000 mg/L of initial COD and operated
under optimized conditions such as an HRT of two days and an applied cell voltage of
0.8 V. The findings showed a COD removal efficiency of 95% along with H2 generation
of 32 mL/L.day [120]. Likewise, the treatment of dairy effluent combined with landfill
leachate was studied in a membrane-less batch-fed MEC operated at an applied cell voltage
of 0.8 V with an HRT of 48 h. A sustained functioning of the MEC at an OLR of 24 g
COD/m3 .day for 10 operation cycles resulted in a maximum COD removal of 73% and H2
generation of 15 mL/L.day [121]. Therefore, the above discussion exposed that an MEC can
professionally manage dairy effluent and valuables such as bio-hydrogen can concurrently
be retrieved during the treatment process.
The key benefits of MECs comprise the biotransformation of waste into valuable prod-
ucts when linked with dark fermentation that uses complex carbohydrates to produce green
hydrogen. In contrast, MECs use various organic substrates for H2 evolution. Furthermore,
H2 generation in MECs occurs via organic matter oxidation, which necessitates a low redox
potential when associated with water oxidation in the usual electrolysis. Irrespective of
these advantages, the main limitation of MECs is their lower rate of H2 production, which
restricts their real-life applications. Hence, imminent studies need to be conducted to
elucidate the complicated associations amid the diverse working parameters of MECs and
their H2 production rate.

7.3. MDCs for Water Desalination and Dairy Wastewater Treatment

The application of MDCs in the desalination process was presented in 2009 by Cao
et al. [122]. The fundamental basis of MDCs is to exploit the natural electric potential created
between the electrodes; i.e., the anode and cathode, to initiate the on-site desalination
Energies 2022, 15, 9084 19 of 34

process [123]. Contrary to METs, MDCs adopt a tertiary compartment for desalination
by installing both an AEM and a CEM across the anodic and cathodic compartments.
MDCs often are employed as either a self-standing technology for concurrent organics
degradation and desalination with power generation or as a pretreatment process for
traditional salt-removal technologies such as reverse osmosis (RO) to decrease the salt
load, thereby reducing the scaling and fouling of the RO membrane and minimizing the
power ingestion.

Table 4. Treatment of dairy wastewater using different METs.

Wastewater Power Density Treatment

Type of MET Reference
Used (W/m2 ) Efficiency
Air-cathode
Real dairy COD removal of
single-chamber 0.005 [1]
wastewater 92.21%
MFC
COD removal of
Catalyst-less and
Dairy 90.46%
mediator-less 0.062 [117]
wastewater BOD5 removal of
membrane MFC
81.72%
Combined
Membrane-less leachate and COD removal of
800 [121]
MEC dairy 73%
wastewater
Single-chamber Dairy COD removal of
1520 [120]
MEC wastewater 95%
Three-chamber Salt removal rate of
Dairy effluent 0.0020 [124]
MDC 0.341 g/L.day
MFC: microbial fuel cell, MEC: microbial electrolysis cell, MDC: microbial desalination cell, COD: chemical oxygen
demand, BOD5 : 5-day biochemical oxygen demand.

In an exciting study, dairy effluent with COD of 1000 mg/L was applied as feedstock in
the anodic chamber with a Chlorella Vulgaris-inoculated biocathode in an MDC. Continuous
experimental trials were executed by consuming a saline solution with a concentration of
15 g/L and 35 g/L in two MDCs while the rate of salt removal and the power density were
constantly scrutinized. A maximum salt removal rate of 0.341 g/L.day with a maximum
power density of 20.25 mW/m2 was noticed in the MDC with a 35 g/L salt content
compared to the MDC with a 15 g/L salt concentration [124]. These studies showed that
due to the insignificant energy contribution needed for the concurrent treatment of dairy
effluent and salt removal by an MDC, it can be foreseen as an energy-competent and
reasonably economic process.
The other substantial benefits of MDCs include a low energy consumption, an effective
salt removal rate, additional energy generation, and concurrent wastewater treatment.
Nevertheless, apart from these extraordinary benefits, the main drawback of MDCs is
the scaling and fouling of membranes caused by the existence of different ions such as
sodium, calcium, etc., present in the salt solution. Scaling further results in the inhibition of
the movement of ions and raises the overall resistance of an MDC, thus diminishing the
power generation [107]. Henceforward, supplementary research is needed to explain the
inhibition of the movement of ions, which would aid in minimizing the maintenance costs
and improve the performance of MDCs.

7.4. Valuables Recovered through MES using Dairy Wastewater

The technology of MES is an evolving one in bioelectrochemical research; it utilizes
the electrons resulting from the cathode to reduce CO2 and other compounds into different
chemicals [125]. The benefits of MES include not only CO2 sequestration and chemical
production, but also address the harvesting, storing, and circulation difficulties linked
Energies 2022, 15, 9084 20 of 34

with energy, as the electrons harvested can be from any sustainable source [126]. As this
technology is still in its embryonic form, there has been limited research conducted on it and
that also employing dairy wastewater. In a recent finding, CO2 was converted to CH4 using
membrane-less MES inoculated with anaerobic granular sludge to treat dairy wastewater.
The MES experiments were performed for 144 days; i.e., about six cycles, and the CH4 was
steadily collected in the serum bottles. A maximum CH4 level of about 46% was observed
in the second cycle within 16 days of operation. Bacterial data examination exhibited that
the Methanobacterium was the utmost leading group of microbes in every experimental
sample [127]. Therefore, as deliberated earlier, the MES conveys boundless potential,
but there also are few challenges involved such as a low product yield, separation and
purification of the obtained products, etc., which must be resolved before commercializing
the technology.

8. Strategies to Improve the Performance of METs

The execution and economics of METs are connected to the employment of appropriate
materials for membranes and electrodes and an efficient system architecture. METs char-
acterize a ground-breaking technology for simultaneous dairy wastewater treatment and
valuables recovery that can be chosen for numerous environmentally based concerns [128].
Harvesting energy and value-added products through METs is not restricted by the Carnot
cycle because it is a rudimentary translation of biochemical energy deprived of limited
heat losses [129–131]. Therefore, they can deliver a higher rate of energy alteration in the
range of 70%, similar to traditional fuel cell technologies [132]. In addition, the efficacy
and operations differ depending on the feedstocks and bacterial catalysts employed. To
improve METs’ efficiency and commercialize them, advancements in electrode materials,
membranes, the biocatalysts employed, and the architecture of METs are elucidated be-
low [133]. The integrated-system approach to METs for augmenting wastewater-treatment
efficacy is also deliberated in detail.

8.1. Electrode Modifications

The constitutional and constructural properties of electrode materials impact MET
functionality. For anodes, the influence is on the adhesion of microbes and the potency of the
coalescent electron transfer from microorganisms to anodes [134]. These structural abilities
are related to the electron-transfer efficiency and can be increased by increasing the specific
surface area to enhance biofilm development. Furthermore, the microbe’s metabolism rate
can also be amended by anodic constituents that provide an anaerobic terminal electron
acceptor for breaking down the organic compounds in dairy wastewater [135]. In a recent
investigation, a batch-fed dual-compartment MFC was studied using three diverse anodes
(a graphite rod, graphite felt, and carbon cloth) and that employed dairy effluent as
feedstock with an initial COD of 1357 mg/L. In this investigation, the maximum open
circuit voltage and power density of 0.847 V and 1.36 W/m2 , respectively, resulted from
the carbon cloth, along with a COD removal efficiency of 91.3% [136].
During another study, an anode adorned with copper-doped iron oxide nanoparticles
(Cu-FeO) was utilized to treat proteins and lipids present in dairy effluent through an MFC.
The operation of the MFC showed an improved power density of 161.5 mW/m2 for the Cu-
FeO anode along with a COD removal of 75% [137]. The Cu-FeO-coated anode exhibited
an outstanding performance due to its better hydrophilic nature and reduced resistance,
which were confirmed by the wettability and an electrochemical impedance spectroscopy
analysis. More recently, in a study by Mahdi Mardanpour et al., a stainless-steel spiral
anode coated with graphite was employed in a single-annular-compartment MFC for dairy
wastewater treatment. The study’s findings showed a maximum coulombic efficiency and
COD removal efficiency of 26.8% and 91%, respectively. Further, a 20.2 W/m3 peak power
density was achieved, which demonstrated the effectiveness of using a spiral anode in the
MFC due to the better attachment of microbes to the anode [138]. Henceforth, choosing
suitable anode materials and their alteration is obligatory to intensify MET performance.
Energies 2022, 15, 9084 21 of 34

Not only the anode but also the MET efficiency in terms of energy and valuables recov-
ery along with concurrent dairy effluent treatment is affected by cathodic materials as well
because they affect the reduction reaction kinetics [139,140]. The typical cathodes employed
in METs such as platinum, etc., have limitations comprising cost-intensity, the tendency
for bacterial fouling, and intoxication of microorganisms for biotic cathodes [141,142]. Due
to these concerns, several low-priced and inert bacterial constituents with higher electro-
catalytic capabilities have been discovered to boost the performance of METs. Affordable
chemical cathodic modifications help to enhance the adsorptive and electrochemical activi-
ties of METs by changing the cathodic exterior to cultivate the inert bacterial features.
In a study by Veeramani et al., the researchers synthesized cobalt oxide (CoO) from
cobalt nitrate and sodium hydroxide and exploited it as cathode material in an MFC for
energy recovery from dairy effluent by coating CoO on carbon cloth. A maximum open
circuit voltage of 630 mV was obtained along with a peak power density of 80 mW/m2 [143].
Another interesting study was executed by opting for a copper-blended 3D cathode (Cu-
blended 3D cathode) in an air-cathode MFC fed with dairy wastewater. The peak power
density and COD removal efficiency achieved with these Cu-blended 3D cathodes were
14.4 W/m3 and 88.1%, respectively [144]. Henceforward, the performance of METs can be
significantly improved via the modification of the electrode materials, thereby paving the
way toward real-world implementation and commercialization for energy recovery and
dairy effluent treatment.

8.2. Membrane Modifications

In a typical MET, membranes aid in transporting the ions and separating the anodic
and cathodic compartments. Furthermore, the membrane is vital in the interception of
coupling between the anodic and cathodic sides exclusively by dairy wastewater, CO2 ,
and O2 [145,146]. For the selection of membranes, aspects such as the resistance, feed
uptake, membrane fouling, and O2 dispersion are considered for justification. Several
types of membranes were established for H+ transport in METs [147,148]. Characteristically,
polymer membranes are categorized as perfluorinated polymer membranes, hydrocarbon
polymer membranes, and hybrid membranes. Mostly, DuPont™ Nafion® membranes
under perfluorinated polymer membranes are applied as PEMs in METs due to their
excellent H+ conductivity [146]. However, the downsides of using this type of membrane
are the cost intensity and non-biocompatibility.
To counter the cost concerns, numerous polymers and chemical-based additives such
as TiO2 , etc., were presented to formulate a competent PEM for MET applications. In a
study by Ayyaru et al., the authors employed sulphonated polyether ether ketone (SPEEK)
as a PEM in a single-chamber MFC to treat dairy and domestic wastewater; this was
further correlated with a Nafion® 117 membrane. The MFC-containing SPEEK membrane
generated 55.2% greater power when compared to the Nafion® 117 membrane. In obtaining
the oxygen mass transfer coefficients, SPEEK and Nafion® 117 demonstrated 2.4 × 10−6
cm/s and 1.6 × 10−5 cm/s, respectively, resulting in lowered oxygen diffusion [149].
During another investigation, TiO2 nanofillers were added to SPEEK to synthesize the
TiO2 -SPEEK membrane for application in an MFC. Different weight percentages of TiO2
that varied from 2.5 to 10% were studied to understand the membrane performance; a 5%
TiO2 –SPEEK membrane generated a peak power density of 1.22 W/m2 and a voltage of
0.635 V, which were higher than those of the Nafion [150].

8.3. Different Configurations Employed

A large variability in MET architectures is being fathomed for explicit applications and
to enhance METs’ functionality by minimalizing system losses. In this regard, a few note-
worthy illustrations comprise single-chamber METs, air-cathode single-chambered METs,
upflow tubular METs, etc. [129,133]. Nevertheless, the most frequently described configu-
rations are the dual-chamber METs; despite their lower voltage generation, they have been
Energies 2022, 15, 9084 22 of 34

the utmost expedient to optimize METs’ performance with component modifications and
additional functional circumstances.
Firstly, the air-cathode single-chamber METs are the effectual configuration system
for better optimal performance. The purpose of the air cathode is to opt for the freely
available oxygen from the environment as a terminal electron acceptor for the reduction
reaction [133]. Therefore, the oxygen requirement for aeration is reduced, thereby improv-
ing the system’s sustainability. In a study, dairy wastewater with an initial COD in the
range of 900 to 1500 mg/L was fed into single-chamber MFCs with an HRT of 2.4 days.
A peak power density of 170 mW/m3 and a coulombic efficiency of 12.8% were attained
with a simultaneous COD removal efficiency of 71.1% [151]. During another investigation,
single-chamber MECs were fed with dairy wastewater operated for two days at an applied
voltage of 0.8 V. The results demonstrated that a COD removal efficiency of 95% along with
a maximum H2 generation of 32 mL/L.day [120].
Now, the other configuration is the most suitable and simpler version of METs; i.e.,
dual-chamber METs. These reactors comprise two different compartments separated by
the membranes and tightly sealed with the assistance of a gasket. This model is the most
appropriate reactor for laboratory trials because it is not affected by cathode fouling due
to separation. In an investigation by Cecconet et al., the researchers fabricated a dual-
chambered MFC for dairy effluent treatment that was run continuously for 96 days. The
average feeding rate for the MFC was 1 L/day and the maximum CE and COD removal
efficiency obtained were 30.4% and 80.9%, respectively. Moreover, the average produced
power density was 12.21 W/m3 throughout the operational period of 96 days [152]. Apart
from the exceptional outcome of dual-chambered reactors, single-chamber reactors are the
most preferred ones to fulfil the needs for upscaling of the reactor.
A conventional three-chambered MDC is constructed by placing the additional com-
partment between the two compartments of a typical dual-chambered MFC and separating
the anode with an AEM and the cathode with a CEM. The membrane positions can also be
altered by placing an AEM near the cathode and a CEM near the anode. In a fascinating
study, dairy effluent was applied as a substrate in the anodic chamber in a biocathode
MDC. The middle chambers were filled with salt concentrations of 15 g/L and 35 g/L in
two different MDCs, and the rate of salt removal and the power density were noted. An
extreme salt removal rate of 0.341 g/L.day with a peak power density of 20.25 mW/m2
was found in the MDC with a 35 g/L salt content compared to the MDC with a 15 g/L salt
concentration [124].
Tubular air-cathode MFCs are intended to function in a constant mode of operation.
Typically, in a tubular MFC, the anode is positioned at the bottom of the tubular reactor, and
the cathode is attached to the PEM to form a membrane electrode assembly (MEA). A study
recently described the advancement of an upflow tubular air-cathode MFC fed with dairy
effluent. Maximum COD and BOD removal efficiencies of 96% and 97%, respectively, were
obtained along with a peak power density of 3.5 W/m3 [153]. The above results specified
that the different METs built have an outstanding potential in dairy effluent treatment,
valuables recovery, and energy recovery.

8.4. MET-Based Integrated Systems

The combination of various treatment processes assists in attaining a greater removal
efficacy compared to the stand-alone process and further aids in reaching the levels of
the discharge standards, specifically for an intricate effluent such as dairy wastewater.
Nevertheless, limited integrated-system approaches have been undertaken to date in dairy
wastewater treatment. In a recent fascinating study [154], MFCs were coupled with a
dark-fermentation hydrogen-generation reactor to treat complex cheese whey wastewater.
A peak power density of 439 mW/m2 was achieved from the effluent after the fermentation
process, which was almost 1000 times better than that when using cheese whey alone in the
MFC. The above results demonstrated that MFCs could be an important part of the process
Energies 2022, 15, 9084 23 of 34

to obtain additional chemical energy from cheese whey wastewater when they follow the
dark-fermentation process.
A study was made by coupling the electro-Fenton process with an MFC, renowned
as a bio-electro-Fenton MFC, for dealing with combined dairy and oil wastewater by
employing an AEM in the reactor. The authors observed a COD removal of 77% and
a maximum power density of 260 mW/m2 with voltages up to 2.3 times better than
that of the conventional system [155]. During another investigation, integrating an MFC
with a microalgal approach such as a photobioreactor system can aid in reducing GHG
emissions from dairy wastewater treatment plants, thereby sequestrating CO2 released from
industries. The MFC-PBR configuration used an industrial dairy effluent as the anolyte;
the COD removal efficiency was constantly noted and finally shown to be 99% [156].
These research findings exposed that the amalgamation of METs with supplementary
technologies such as dark fermentation and PBR (Table 5) improves the removal efficacy,
valuables recovery, and bioelectricity generation of METs. Therefore, combining METs with
progressive approaches can support overcoming the boundaries of stand-alone approaches
and hence can result in clean water for discharging or recycling purposes. In addition, the
above discoveries demonstrated that METs can be established as a self-sustainable way to
manage dairy effluent and also aid in reducing operational costs by recovering bioenergy
and valuables.

Table 5. Strategies for improving the performance of METs.

Modification of
Strategy Type of MET Power Density Removal Efficiency Reference
Material/System
Anode decorated with
Dual-compartment
copper-doped iron oxide 161.5 mW/m2 COD removal of 75% [137]
MFC
Electrode nanoparticles
modification
Copper-blended 3D
Air-cathode MFC 14.4 W/m3 COD removal of 88.1% [144]
cathode
Sulfonated polyether
Single-chamber MFC 5.7 W/m3 COD removal of 75% [149]
Membranes ether ketone
TiO2 -SPEEK membrane Dual-chamber MFC 1.22 W/m2 COD removal of 90% [150]
Air-cathode-single
- 170 mW/m3 COD removal of 71.1% [151]
chamber MFC
Configurations - Dual-chamber MFC 12.21 W/m3 COD removal of 80.9% [152]
Conventional-three Salt removal rate of
- 20.25 mW/m2 [124]
chamber MDC 0.341 g/L.day
Integration with dark
Single-chamber MFC 439 mW/m2 COD removal of 42% [154]
fermentation
Integrated systems
Integration with
Dual-chamber MFC 260 mW/m2 COD removal of 77% [155]
electro-Fenton process
MFC: microbial fuel cell, MEC: microbial electrolysis cell, MDC: microbial desalination cell, COD: chemical oxygen
demand, MET: microbial electrochemical technology.

9. Water Reuse and Circular Economy via METs in the Dairy Industry and Real-Life
Applications
Conventionally, a linear economy is being engaged to harvest energy and resources
that generate beneficial products by utilizing limited supplies and sending the waste aris-
ing from the process to the landfill. This plan, which uses a ‘take-make-disposal’ policy,
creates a significant quantity of factory-made and domestic waste. Further, these wastes
are inevitable and detrimental to the environment because they are incinerated or dumped
in landfills [80,157]. Meanwhile, the rising greenhouse gases (GHGs) produced during
several waste disposal/remediation activities are responsible for global warming condi-
tions. Therefore, ecologically beneficial and continual economic models are recommended
Energies 2022, 15, 9084 24 of 34

for the recycling of waste generated with the potential recovery of resources [158,159].
The circular economy is one such model that aids in the augmentation of salvaging and
recycling existing waste materials for harvesting varied materials and power by exploiting
environment-friendly methods.
The notion of circularity, which was instigated by industrialized ecosystems, targets
the diminishment of resource depletion and discharges/emissions into the environment by
completing the circuit of constituents [160]. On the downside of these criteria, material loss
needs to be mitigated and can be regenerated either for recycling or reusing. In agreement
with the above-stated basis, rallying in the direction of a circular economy infers probing
for sustainable practices or technologies. Furthermore, circularity can circumnavigate
the issue of limited supplies by boosting the usage of recovering resources and further
preventing the escape of native resources such as nutrients in the form of nitrogen (N),
phosphorus (P), carbon (C), and water from the ecological system [161]. This idea aids in
encouraging the reuse and reclaiming of the loss of specific resources that can complement
their significance to the ecosystem. Briefly, for a circular economy, wastes are converted into
resources through the implementation of different sustainable technologies and strategies,
which is imperative in the conservation of natural resources and in alleviating emerging
environmental challenges.

9.1. Circular Economy in METs in the Dairy Industry

Several investigations have scrutinized resource recovery from dairy wastewater
effluent via METs, and many encouraging yields were deliberated. Although further
comprehensive studies and analyses of the upscaling of METs must be made to demon-
strate future opportunities. Innovative METs are highly capable of being part of a circular
economy because they function to recover energy and produce valuable commodity chemi-
cals along with simultaneous dairy wastewater treatment [101,162,163]. The wastewater
employed as a substrate in METs undergoes biological degradation to generate energy
and new materials concurrently. As in a typical MET, aerobic wastewater treatment is
not obligatory, and the energy consumption for the process is significantly alleviated. In
addition, extensive self-sustainable systems can be attained by pairing METs with other
popular energy sources such as solar, tidal, etc. [164].
Both MFCs and MECs are alleged to be self-sustainable podiums for recuperating
energy from waste because they can break down the organic matter present in dairy
wastewater along with an additional production of electricity or clean fuel such as H2 [7,
164]. Similarly, MCCs that employ algal cells assist in the recycling of CO2 into biomass,
resulting in the sequestration of CO2 [165]. Although CO2 is discharged as one of the
byproducts in the above process, due to the biological degradation of organic matter, it can
be further utilized for algal growth, which exemplifies METs as carbon-neutral systems.
Moreover, salt elimination and water reclamation are critical issues in dairy plants that
can be solved by applying MDCs, which are a type of MET. Compared to the traditional
treatment technologies, these METs use less energy and instead reasonably yield power
under anaerobic conditions, thus accomplishing sustainability.
Among the METs, MESs have captured immense attention in the sequestration of
CO2 with concomitant beneficial biochemical production in which microorganisms exploit
CO2 as the carbon source. A recent study reported the conversion of CO2 to CH4 using a
membrane-less MES incorporated with carbon-cloth electrodes functionalized with copper
nanoparticles for different cycles. A maximum energy efficiency of 46% within 16 days was
reported for methane production in the second cycle. However, the system performance
declined with the continual process cycles due to the decreased hydrogen production,
which resulted in decreased methane generation [147]. Similar valuable substances such as
the methane produced above can be utilized either for straightaway uses or as reactants
for other chemical processes. This CO2 closed-loop plan through METs can be envisaged
as a potential part of a circular economy by achieving a self-sustainable waste-to-valuable
chemical platform, thereby making the system economical.
Energies 2022, 15, 9084 25 of 34

Recently, a database of the biochemical components of milk foods revealed that numer-
ous organic composites such as nutrients, organic acids, conjugated linoleic acids, volatile
fatty acids, etc., originate from milk, cheese, and other dairy products [166]. The retrieval
of nutrients such as N and P from dairy effluent will permit the ecological protection of
the marine environment and aid in creating biofertilizers through the waste-to-fertilizer
platform. Mansoorian et al. reported nutrient recovery from dairy wastewater with higher
elimination efficacies of about 69.43% for ammonia nitrogen (NH4 + -N) and 72.45% for
phosphorous with an HRT of 6 days [117]. Similarly, lactic acid, an exciting organic acid
usually observed in dairy wastewater, can be employed as an effective substrate in METs
for energy generation. Lactic acid recovery/removal can be accompanied by utilizing it as
a source of electrons in the METs [167]. In addition, retrieving VFAs from dairy effluent is
another excellent pathway that is being studied in the domain of METs [168]. Therefore,
through the implementation of METs representing the above-mentioned technologies, a
circular economy can be demonstrated in the dairy industry.

9.2. Circular Economy in the Dairy Industry via Other Technologies

Many sustainable approaches strive to recover resources from dairy wastewater as
part of a circular economic plan. Among them, nutrient recovery through struvite pro-
duction from dairy wastewater has been studied and can be easily adapted for real-life
applications [169,170]. A few other investigations on the production of biogas employing
anaerobic digestion from dairy wastewater also were demonstrated recently. According to
a recent study, the rate of CH4 generation in anaerobic digestion could be enhanced via the
application of various conductive substances such as Fe2 O3 [171], nanomagnetites [172],
etc. Microalgae harvesting is also one of the alternative methods for producing biofuels
with the parallel removal of nutrients from dairy wastewater [173]. In this veneration,
D˛ebowski et al. studied the usage of a dairy wastewater digestate as a growth medium
for microalgal cells to produce biofuels that contained a greater content of oleic acid [174].
Nevertheless, this method of producing biofuels is not yet applied in a commercialized way
since a detailed examination and preliminary testing still need to be performed extensively.

9.3. Real-life Applications of METs for Dairy Wastewater Treatment

Laboratory and benchtop studies of METs are very prevalent in the literature. However,
there are a minimal number of articles on the commercialization and real-life applications of
METs for dairy wastewater treatment. For example, a long-term pilot plant functioned for
65 days with an MFC with a capacity of one litre per day for simultaneous organic matter
elimination and energy recovery [175]. The above work proved that dairy wastewater could
be successfully treated by an MFC and showed an average COD removal of 82% along
with the recovery of a maximum power density of 26.5 W/m3 in a field-scale investigation.
A maximum CE of 24% was obtained at an OLR of 3.7 kg COD/m3 .day; this was further
reduced to 5% when the OLR was increased. Likewise, another pilot-scale study of an MFC
with a 3 L volume of dairy effluent in an anodic chamber was also demonstrated [176].
The maximum removal efficacies attained by this field-scale MFC under the optimum
conditions were about 93.9%, 90.6%, and 72.6% for parameters such as COD, BOD, and
TDSs, respectively. As a result, based on the above-cited studies, we concluded that
METs are highly proficient in treating dairy wastewater with concomitant real-time energy
retrieval.

10. Environmental Impact Assessment and Techno-Economic Assessment of METs

A careful examination to identify savings in energy and emissions from various kinds
of dairy wastewater treatment and plausible valuable recovery through METs must be
conducted to expedite the commercialization thereof. In this regard, a technoeconomic
analysis (TEA) and an environmental impact assessment might prove to be valuable tools
in gauging the sustainability of dairy effluent treatment through METs because they would
assist in deciding whether METs should be investigated further or possess any feasible
Energies 2022, 15, 9084 26 of 34

field applicability [177]. The economic assessment of dairy wastewater treatment via
METs and other technologies such as aerobic digestion can be compared, whereas a life
cycle assessment (LCA) would shed some light on the environmental impacts that could
arise from the traditional technologies or METs employed during the treatment of dairy
wastewater [178]. However, to the best of our knowledge, there are no previous articles
that pertained to the LCA and TEA of METs employed in the treatment of dairy wastewater.
However, a few investigations briefly and critically explained the TEA and LCA of METs;
these are explained subsequently. An investigation conducted by Trapo et al. (2017)
showed that MFCs were economically beneficial (EUR 1700–2300 per year) compared to
the conventional activated-sludge process (EUR 8166 per year) when no replacement of
the electrode or membrane was required because the capital cost of MFCs is higher than
the operating cost due to the use of expensive membranes and electrodes in METs [179].
However, few pilot- and field-scale experiments on METs have been investigated, which
restricts a better understanding of the long-term economic feasibility of METs.
Similarly, an LCA aids in the evaluation of the positive and negative effects of products
on human health, the environment, and the depletion of sources. An experiment revealed
that the environmental benefit of valuables recovered from wastewater was only 0.01–7% of
the overall environmental impact of METs [180]. Another investigation revealed that METs,
especially MFCs and MDCs, would only become environmentally sustainable if their power
density rose to at least 500 W/m3 from the present maximum of 20 W/m3 [181]. Similarly,
MECs will become only beneficial if hydrogen production contributes to environmental
benefits; this will be possible if the produced hydrogen can be used as a biofuel in vehicles
and industries. The TEA and LCA can provide a better understanding of the economic and
environmental impact of the METs employed for dairy wastewater treatment [182]. There-
fore, investigations pertaining to the TEA and LCA of METs in treating dairy wastewater
should be conducted for the better understanding of the applicability of METs for dairy
wastewater treatment.

11. Challenges Involved and Future Prospects

METs have a wide opportunity for application in treating dairy wastewater with
simultaneous resource recovery. Further, METs are promising technologies that have the
competence to resolve the problems of energy requirements and environmental pollution.
In this regard, numerous investigations have demonstrated resource recovery from dairy
wastewater via METs [183]. However, there are a few challenges that are impeding progress
toward the commercialization of these technologies. Still, many unanswered questions
remain regarding the implementation of METs at a pilot or field scale for industrial wastew-
ater treatment, such as the cost of installation and operations, energy requirements, and
efficacy [8]. The operation of METs is beneficial in the short term; however, research should
be directed toward determining their long-term suitability for the generation of valuables
from waste.
Understanding the cell microbiome can also be beneficial when suggesting operational
strategies for the improvement of the activity of electroactive microbes, which in turn will
increase the yield of valuables recovered [184]. In addition, a better understanding of
these aspects can be achieved with more field-scale investigations. However, the upscaling
of METs from lab to pilot or field scales is still one of the serious challenges, although
dairy wastewater has been proven as an ideal substrate in the application of these tech-
nologies [185]. Further, design and material issues interfere with the practical application
because the increase in the volume or size resulted in a decline in performance and efficiency.
Therefore, MET technologies are not fully ready at this moment for real-life application;
however, they might become a valid alternative to conventional technologies soon.
In METs, electrode materials and membranes play vital roles and are the major reasons
for the high fabrication costs of the said technologies [22]. Usually, the raw materials
utilized for electrode fabrication in METs are expected to demonstrate an exceptional
stability, superior conductivity, a mass transfer ability, a high porosity, a greater surface
Energies 2022, 15, 9084 27 of 34

area, biocompatibility, and a capacity to scale up. Nevertheless, materials with the above-
mentioned characteristics such as platinum are presently very expensive, which hinders
the scalability along with the technical feasibility of METs. Additionally, the application of
membranes that serve as a separator between the anodic and cathodic compartments in
METs is hindered by several drawbacks such as a decreased proton permeability, substrate
loss, and oxygen dispersion into the anodic chamber. Further significant barriers to mem-
brane employment in METs involve membrane fouling and increased resistance. Therefore,
the implementation of an appropriate membrane is challenging and poses technological
obstacles to the configuration, efficacy, and real-life application of METs.
Furthermore, METs are exceedingly temperature-sensitive, which can further affect
the efficacy and power output and may reduce the potential life of METs in field-scale
operations. This is majorly due to the inability of METs to operate at minimal temperatures
due to the lethargic biological responses in such circumstances. Additionally, overpotential
losses at electrode surfaces, architectural design and operations, low efficiency, and poor
power output are also factors behind the challenges leading to the upscaling of METs [186].
To navigate these challenges encountered in dairy wastewater treatment via METs, fur-
ther interdisciplinary research is necessary to determine the complexities and schematic
approaches that can be employed to overcome the challenges faced during the upscaling of
METs, which would move these novel technologies toward commercial applications.
The prospects of METs are significant in numerous potential functions that extend from
power generation to wastewater treatment. The extremely well-studied purpose of METs is
the use of microorganisms to produce electrical energy. A few other findings emphasized
the possibility of hydrogen evolution from METs. Recent studies emphasized the fact that
hydrogen can be competently generated from bacterial reactions using dairy wastewater
through a fermentation process with or without expensive membranes. An additional
vital function of METs is in dairy wastewater treatment, for which several investigations
examined the prospects of METs. Moreover, the investigators revealed that METs can be
applied in the field of water treatment involving a desalination process. Further noteworthy
uses of METs were seen in different areas such as the lowering of carbon dioxide emissions
and greenhouse gas mitigation.

12. Conclusions
The current review article deliberated the worldwide threats regarding the treatment
of dairy effluent and highlighted the evolving technologies employed for dairy wastewater
treatment. Traditional systems such as coagulation–flocculation, MBR, EC, and aerobic and
anaerobic processes are typically utilized for managing dairy effluent. Nevertheless, the ear-
lier processes are energy-consuming and expensive, yield vast quantities of surplus sludge,
and create toxic products throughout the treatment process. In recent times, METs have
acquired the colossal recognition of researchers due to their effectual effluent-management
competence with the contemporaneous generation of valuables and diminished sludge
generation. However, the use of METs is affected by diverse working/operational pa-
rameters such as membranes, catalysts, the feedstocks exploited, etc., which need to be
optimized to improve the production of valuables to encounter marketable anticipation for
real-world implementations. Consequently, additional investigations must be undertaken
to advance economical electrocatalysts and membranes. Further research in pilot studies
and in experimental laboratory trials will aid in the field-scale propagation of METs.

Author Contributions: A.G.: Conceptualization, Formal analysis, Investigation, Methodology,

Writing—original draft, Writing—review and editing; Y.B.: Validation, Writing—original draft,
Data curation, Writing—review and editing; S.D.: Project administration, Resources, Supervision,
Validation, Writing—review and editing. All authors have read and agreed to the published version
of the manuscript.
Funding: This research received no external funding.
Institutional Review Board Statement: Not applicable.
Energies 2022, 15, 9084 28 of 34

Informed Consent Statement: Not applicable.

Data Availability Statement: Not applicable.
Acknowledgments: We would like to thank IIT Delhi for providing the infrastructure required for
this research.
Conflicts of Interest: The authors declare that they do not have any financial interests or personal
relationships that could be considered as potential competing interests.

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