Journal of Cleaner Production 264 (2020) 121582

Contents lists available at ScienceDirect

Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Review

A critical evaluation of potential routes of solar hydrogen production

for sustainable development
Faran Razi*, Ibrahim Dincer
Faculty of Engineering and Applied Science, Ontario Tech University, 2000 Simcoe Street North, Oshawa, Ontario, L1H 7K4, Canada

a r t i c l e i n f o a b s t r a c t

Article history: This paper provides a comprehensive review on the various techniques and routes of solar hydrogen
Received 17 February 2020 production. The solar energy options considered are thermal energy, electrical energy, photonic energy,
Received in revised form and hybrid options. The hybrid option includes thermal and electrical, electrical and photonic,
31 March 2020
biochemical and thermal, and biochemical and photonic energies. Some relevant literature review with
Accepted 6 April 2020
Available online 13 April 2020
their key findings, conclusions, and suggestions is presented. Various methods of solar energy-based
hydrogen production are explained and briefly discussed. The technologies available for realizing
Handling editor: Sandro Nizetic these methods are also presented. Some recent advances in solar hydrogen generation is also presented
in which some novel techniques are discussed. Some plant configurations are also discussed and
Keywords: compared to consider the factors which influence the cost of hydrogen. This review article also aims to
Hydrogen comparatively assess and evaluate the several routes of producing hydrogen using solar energy. The
Solar energy comparative evaluation is performed using two sets of criteria. Criteria set 1 consists of environmental
Sustainable development impact and cost of hydrogen production. Criteria set 2 comprises energy and exergy efficiencies, sus-
Photonic energy
tainability indices and hydrogen production rates. High-temperature energy methods show much better
Efficiency
efficiencies and hydrogen yield while at the same time are more environmentally harmful. Photonic and
Environment
biochemical energy routes are more environmentally friendly and sustainable, but have low efficiencies.
© 2020 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
2. Methods of solar hydrogen production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3. Novel techniques of producing solar based hydrogen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
4. Factors influencing the cost of hydrogen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
5. Comparative evaluation of methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
5.1. Environmental impact and cost comparison . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
5.2. Efficiency, sustainability index, and production capacity comparison . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
6. Commercialization potential in the near future . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
7. Global sustainability measures . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
8. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
Nomenclature . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9

1. Introduction

* Corresponding author. With the increase in the utilization of fossil fuels as a primary
E-mail addresses: [email protected] (F. Razi), [email protected] source of energy generation and its economic as well as
(I. Dincer).

https://doi.org/10.1016/j.jclepro.2020.121582
0959-6526/© 2020 Elsevier Ltd. All rights reserved.
2 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582

environmental consequences, the production of green fuels has area of solar energy aided thermochemical processes based on
been the topic of much interest for quite a long time now. In light of experimental studies, cost, lifecycle, and thermodynamic analyses.
the increasing greenhouse gas (GHG) emissions and fossil fuel Based on their analyses, they observed that thermochemical cycles
depletion, many countries have focused on formulating environ- had lower efficiencies and higher cost of hydrogen production than
mentally friendly energy policies. Moreover, various research or- processes for solar upgrading. Moreover, they claimed that solar
ganizations have turned towards the development of such energy-based methane reforming and lime production methods
innovative systems that are capable of utilizing renewable sources showed greater experimental efficiencies in comparison with other
for generating power and fuels. Of course, the choice of renewable solar thermochemical processes. Said et al. (2016) reviewed various
energy has plenty to do with this research as each source, its solar reforming systems. They discussed the four variations of the
availability and its capacity of power generation and fuel produc- reforming process namely, steam methane reforming (SMR),
tion vary in context of the energy demands which need to be met. autothermal reforming, partial oxidation, and dry reforming. Ac-
Scientists and engineers across the globe have been making cording to them, SMR using Nickel-based catalyst showed much
immense efforts to somehow exploit renewable energy sources promise with regards to cost-effectiveness and efficiency in
most efficiently and economically for decades. However, various hydrogen and synthesis gas (syngas) production when compared
challenges need to be addressed to utilize these green energy with other processes. Apart from SMR, they claimed that the rest of
sources. One of the fundamental amongst them is their intermit- the reforming technologies were not suitable for producing
tent availability. This inconsistency in the presence of such sources hydrogen at bulk level. Moreover, they indicated in their review
has been the greatest hurdle in the way of realizing the objective of that solar energy was capable of providing the necessary heat
a green economy. Having said that, amongst all renewable energy required for the reforming process using facilities such as solar
sources, the most compelling choice has always been the solar towers and parabolic dishes. Acar et al. (2016) reviewed various
energy. Relative to other competing sources, solar energy has been photocatalytic water-splitting approaches for hydrogen production
the most promising option as far as its availability and the potential where they analyzed photocatalysis as a green energy solution for
to produce energy. addressing global climate change and environmental sustainability
Around 30% of the solar energy which strikes the surface of the challenges. They comparatively assessed various photocatalysts
earth gets reflected and the remaining of that incident solar energy available in the literature via visible light-based water splitting for
per year (3.9
1024 MJ) is approximately 10,000 times more hydrogen production based on quantum yield, bandgap, rate of
compared with the global energy consumption at present (Joshi producing hydrogen per unit mass of catalyst and rate of producing
et al., 2011). This is an authentication to the aforementioned hydrogen per unit surface area of the catalyst. They reported that
claim about the ability of solar energy for meeting the energy cadmium-sulfide based catalysts on average showed better per-
generation demands as well as fuel production. Solar fuels, such as formance characteristics for all assessment criteria except for
hydrogen, have been a topic of much interest among the scientific quantum yield. On the other hand, zinc oxide/sulfide performed
community and there is plenty of literature available on various better as far as the quantum yield was concerned.
ways of solar hydrogen production. Hydrogen is not only utilized as Numerous studies related to various solar-driven hydrogen
a fuel itself but also helps in the generation of synthetic fuels, in production methods have been performed and published in the
production of ammonia and various fertilizers, in upgrading heavy open literature. Alzahrani and Dincer (2016) conducted a study in
oils such as oil sands and synthesis of other chemicals (Dincer, which they designed and analyzed an integrated system where a
2012). In light of these utilities of hydrogen, especially as fuel, solar tower was utilized for harnessing thermal energy for high-
several countries are trying to shift towards the hydrogen economy. temperature electrolysis to produce hydrogen. Their proposed
According to Monica Nagashima Pereyaslovska, a researcher at the system consisted of a solar tower and a thermal energy storage
Institute of Energy Economics Japan (IEEJ), the Japanese govern- system with a supercritical carbon dioxide Brayton cycle and a
ment has dedicated nearly $1.5 billion over the last six to seven high-temperature solid oxide steam electrolyzer (SOSE). Their
years towards technology R&D and subsidies for supporting the study demonstrated that the integration of solar tower technology
achievement of zero-emission low-cost hydrogen production with high-temperature SOSE has great potential for hydrogen
through fossil fuels or renewable energy electrolysis, infrastructure production. Moreover, the authors concluded that system optimi-
development of import and domestic hydrogen distribution and zation based on the thermal energy storage size could realize a
scaling up hydrogen utilization across different sectors (Nagashima, continuous generation of hydrogen with a solar-to-hydrogen effi-
2018). Some of the European Horizon 2020 projects target at the ciency of around 12.7% which could rise to 56.8% if the heat pro-
development of solar thermochemical technology as a promising vided to the thermal energy storage is taken into consideration.
fuel production pathway at a large scale as well as competitive costs Hinkley et al. (2011) studied the prospects of a hybrid sulfur cycle
(“Sun-to-liquid project pr, 2019). Soon the whole world will even- (a hybrid-thermochemical cycle) solely based on solar operation in
tually have to follow this line of action for meeting the ever- which thermal energy was supplied by concentrated solar energy
growing energy demands while preserving the environment at and PV system was incorporated for providing the electrical input.
the same time. Based on their study, they claimed that when it comes to large scale
Numerous review articles are being published regarding solar production of hydrogen, the hybrid sulfur cycle proves to be one of
hydrogen production in which various options have been discussed. the prime candidates among the various thermochemical water-
Steinfeld (2014) discussed the solar thermochemical ways of splitting cycles. Moreover, using sulfur-dioxide in the electrolyzer
hydrogen production. He reviewed the fundamental concepts and resulted in substantial electrical energy demand reduction in
technological advancements in the domain of solar hydrogen pro- comparison with the orthodox alkaline process. One of their main
duction via concentrated solar energy serving as a source of conclusions was that using only solar energy for thermal and
providing high-temperature process heat. Moreover, he economi- electrical energy input has the potential of zero emissions. Joshi
cally assessed several routes of solar thermochemical processes for et al. (2011) studied solar thermal and photovoltaic (PV) systems.
producing hydrogen. According to his assessment, hydrogen gen- They examined the performance of these systems based on energy
eration by water electrolysis through solar-generated power can be and exergy analysis as well as the sustainability index. They rated
competitive. Yadav and Banerjee (2016) performed a very the exergy efficiency of the solar collector as a significant factor for
comprehensive review that was aimed at the developments in the evaluating the solar thermal hydrogen generation system’s exergy
 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582 3

efficiency because of its fluctuations with solar radiation intensity. photofermentation, high-temperature electrolysis, SeI, and CueCl
Moreover, they concluded that the exergy efficiency of the PV panel thermochemical water-splitting methods, fossil fuel reforming,
also experienced variations with solar radiation intensity as well as biomass, and coal gasification processes. Methods evaluated
ambient temperature. They further concluded that both these through criteria set 2 are: solar thermal power generation and
routes of solar hydrogen production were environmentally friendly electrolysis, solar high-temperature electrolysis, solar water-
and the systems’ energy efficiency was higher than their exergy splitting thermochemical and hybrid thermochemical cycles, pho-
efficiency. They further added that higher exergy efficiency of the tocatalytic or PEC process, biophotolysis, artificial photosynthesis,
systems ensured a higher sustainability index. In comparison be- photofermentation, solar thermochemical H2S splitting, anaerobic
tween the two systems considered in their study, they reported the digestion and solar thermal fossil fuel cracking.
sustainability index of the solar thermal energy-based hydrogen In the following section, we provide an overview of the various
production system to be higher than PV based hydrogen generation processes and available technologies of solar hydrogen production.
system since the former had a higher value of exergy efficiency than Section 3 presents some of the novel techniques employed for
the later. Ozalp et al. (2018) conducted a study in which they generating hydrogen through solar energy. Section 4 discusses the
assessed the viability of solar thermal cracking of natural gas as an factors which influence the cost of hydrogen production by
alternate option for solar hydrogen production. They concluded considering plant data for various methods. In section 5, we
that with the amalgamation of Hydrogen Fuel Cell (HFC) and Car- comparatively evaluate the considered methods based on several
bon Fuel Cell (CFC), solar natural gas cracking offers an encouraging factors. Section 6 provides a discussion regarding the potential of
alternative of conventional power generation cycles. Furthermore, commercialization of the various processes of solar hydrogen pro-
they added that solar natural gas cracking for energy production duction. In section 7, we briefly discuss some of the necessary
through both CFC and HFC to charge the battery of an electric global sustainability measures and efforts. Section 8 provides the
vehicle demonstrates way higher well-to-wheel efficiency in conclusion of this paper.
comparison with solar thermochemical cycles and solar reforming
for syngas generation followed by a synthetic liquid fuel process. 2. Methods of solar hydrogen production
Acar and Dincer (2014) conducted a study in which they concep-
tually developed and performed thermodynamic analysis on a Hydrogen production methods have been classified into four
continuous type hybrid photoelectrochemical (PEC) system for categories based on the option of solar energy being utilized as
hydrogen generation. The hybrid system consisted of PV panels shown in Table 1. These categories are listed as: (1) thermal energy-
with a PEC system and a dielectric mirror was placed such that it based methods (2) electrical energy-based methods (3) photonic
would allow a specific solar spectrum to the PEC cell for photo- energy-based methods and (4) hybrid options which include
catalytic water-splitting and the part of the spectrum which could electrical with thermal energy, electrical with photonic energy,
not be exploited for photocatalysis was sent to the PV panels for biochemical with thermal energy and biochemical with photonic
electricity generation which ultimately aided the electrolysis. energy-based methods. The solar-to-hydrogen (STH) conversion
During the presence of sunlight, the system took advantage of both efficiencies of the various methods are also comparatively pre-
photocatalysis as well as photoelectrolysis while when there was sented in Table 1.
no sunlight, the system was only electricity dependent for pro- All the routes included in the thermal energy option utilizes the
ducing H2 gas along with Cl2 gas and NaOH. One of the major ad- thermal potential of the solar irradiation entering the Earth’s at-
vantages of the proposed system as reported by the authors was mosphere. As mentioned in the introduction section, the thermal
that it could effectively neutralize hydroxyl ions into useful com- energy of the sun can be exploited for various heat-driven pro-
modities for industries. Moreover, by converting such by-products cesses without depleting fossil fuels and also avoiding the resulting
into NaOH and chlorine gas, the system enhanced its utility and GHG emissions. These thermal energy-based methods are further
efficiency. divided into two groups. The first group comprises of all those
According to the literature review, various reviews regarding methods which utilize solar thermal energy for either water or
solar hydrogen production have been published. Most of those re- hydrogen-sulfide splitting/cracking to produce hydrogen. The sec-
views were focused on particular pathways of generating solar- ond group consists of those processes in which solar heat is
based hydrogen such as thermochemical, photocatalytic and fossil employed for hydrogen production involving the utilization of
fuel reforming, etc. Some reviews were performed considering all fossil fuels. In electrical energy option, solar energy is first con-
renewable sources (including solar energy) for producing verted into electricity. This electricity is then supplied in an elec-
hydrogen. However, there has been no review available in the open trolyzer where water is electrochemically split into hydrogen and
literature focusing on all possible ways of exploiting solar energy oxygen gases via electrolysis. The routes considered in the photonic
for hydrogen production. Such a review and comparative evalua- energy option utilizes the photo-effect of the Sun which drives
tion is very essential for providing useful recommendations about many light-dependent processes resulting in hydrogen production.
future research directions for sustainable and environmentally Several methods fall under the category of hybrid options. Methods
friendly hydrogen production. This paper comprehensively reviews that use a combination of electrical and photonic energies work in a
all routes of solar hydrogen production. The main objectives of this way that they utilize photonic energy for electrolysis by incorpo-
particular study are to (a) identify potential solar hydrogen pro- rating certain materials for electrodes that are photosensitive and
duction methods for application in various sectors, (b) categorize undergo certain changes when a specific wavelength of sunlight
these potential methods for various applications and possibilities falls upon them to eventually produce hydrogen. Electrical and
under various conditions, (c) discuss the challenges and opportu- thermal energies are used together where the process involves
nities as well as future directions of the considered methods, and electrolysis as well as heat for either driving thermochemical re-
(d) comparatively evaluate several solar energy-based hydrogen actions or a heat engine which converts a part of the provided
production processes based on two sets of criteria. Criteria set 1 thermal energy into mechanical work that is transformed into
include environmental impact and cost comparison while criteria electricity and then supplied to an electrolyzer. The synergy of
set 2 include efficiency, sustainability index, and hydrogen pro- biochemical and thermal energies is realized such that biomass
duction rate comparison. Methods assessed through criteria set 1 digestion is carried out through low-grade heat energy to produce
are: PV-electrolysis, photoelectrolysis, biophotolysis, hydrogen. Methods that use biochemical and photonic energies
4 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582

Table 1
Solar energy routes and various processes of hydrogen production.

Thermal Energy Solar only Water Thermolysis (STH ¼ 1e2% (Tuller, 2017))
Thermochemical cycles (STH ¼ 20% (Pregger et al., 2009))
H2S Splitting
Thermocatalytic H2S cracking
Hybrid with fossil fuels Reforming (Require CO2 sequestration)
Gasification (Require CO2 sequestration)
Cracking (Require C sequestration)
Electrical Energy PV-Electrolysis (STH ¼ 40% (Rajeshwar et al., 2008))
Photonic Energy Photocatalysis (STH ¼ 0.2% (Tuller, 2017))
Photoelectrochemical (STH ¼ 12% (Tuller, 2017))
Hybrid options Electrical with thermal energy Steam/High Temp. Electrolysis (STH ¼ 35e40% (Rajeshwar et al., 2008))
Hybrid thermochemical water-splitting cycles
Solar thermal power generation & Electrolysis
Electrical with photonic energy Photoelectrolysis
Biochemical with thermal energy Thermophilic digestion
Biochemical with photonic energy Artificial photosynthesis
Photofermentation
Biophotolysis

together work in various ways such as induction of microbes and summarized in Tables 2e4. Table 2 presents the technologies in
bacteria for photo-generation, light assisted fermentation process current use for realizing the thermal energy-based processes of
and bio-imitation of natural photosynthesis for the generation of hydrogen production. In Table 3, the available technological path-
hydrogen. ways are presented with respect to electrical and photonic energy
The various technological pathways undertaken for the solar routes. In Table 4, the technologies for exploiting several hybridized
energy exploitation routes for hydrogen production are routes of solar energy are presented for hydrogen generation.

Table 2
Thermal energy-based routes and the available technologies used for their exploitation.

Routes Available Technologies

Water Thermolysis Heating mechanism:

Directly irradiated reactors
Indirectly irradiated reactors
Gas separation mechanism:
At high temperatures by microporous refractory membranes
By electro-diffusion membranes semipermeable to oxygen
By metallic membranes
By centrifugation
In supersonic jets

Thermochemical water-splitting Cycles (Volatile) Directly irradiated non-structured reactors: Rotating cavities entrained beds
Directly irradiated structured reactors: Moving fronts
Indirectly irradiated non-structured reactors: Aerosols
Indirectly irradiated structured reactors Sintered plates

Thermochemical water-splitting Cycles (Non- Directly irradiated non-structured reactors: Packed Beds, Spouted Beds, Moving Beds
Volatile) Directly irradiated structured reactors: Honey Combs, Foams, Rotary cylinders, Rotary fins
Indirectly irradiated non-structured reactors
Packed Beds
Indirectly irradiated structured reactors

Reforming Indirectly heated reformer

Tubular reformer-receiver
Windowed/volumetric reformer

Gasification Countercurrent fixed bed “up-draft” gasifier

Co-current fixed bed “down-draft” gasifier
Fluidized bed reactor
Entrained flow gasifier

Fossil Fuel Cracking Directly irradiated reactors: Vortex flow

Particle flow
Tornado flow

Indirect irradiated reactors: Entrained flow tubular

Fluid wall aerosol

Thermolysis and Thermocatalysis of H2S Pure Thermal Catalytically enhanced thermal Thermal with equilibrium shift Oxidative and integrated Claus
Processes
 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582 5

Table 3
Electrical and photonic energy-based routes and the available technologies used for their exploitation.

Routes Available Technologies

PV-Electrolysis Electrolyzers:
Alkaline
Proton Exchange Membrane (PEM)
PV Cells:
Wafer-based cell:
Crystalline Silicon/Gallium Arsenide

Commercial thin film:

Amorphous Silicon/Cadmium Telluride/Copper Indium Dallium Di-selenide
Emerging thin-film:
Perovskite/Organic/Quantum Dot

Photocatalysis Photoelectrochemical cell

Photoelectrochemical

Table 4
Various hybrid options and the available technologies used for their exploitation.

Routes Available Technologies

Solar thermal power Generation & Various configurations of thermodynamic systems for converting thermal energy into mechanical energy (Rankine cycle, Brayton
Electrolysis cycle, etc.)
Electrolyzers:
Alkaline
Proton Exchange Membrane (PEM)

Hybrid thermochemical water- Directly irradiated non-structured reactors Directly irradiated structured reactors
splitting cycles Indirectly irradiated non-structured reactors
Indirectly irradiated structured reactors

Steam Electrolysis Solid Oxide Electrolytic cell (SOEC) Solid Oxide Fuel Cell (SOFC)

Photoelectrolysis Photoelectrochemical cell

Thermophilic Digestion Liquid waste:

Covered lagoon digester/Up-flow anaerobic sludge blanket/Fixed Film
Slurry waste:
Complete mix digester
Semi-solid waste:
Plug flow digester

Biophotolysis Tubular Photo-bioreactors Christmas tree Photo-bioreactors Plate Photo-bioreactors Horizontal Photo-bioreactors Foil Photo-
Photofermentation bioreactors Porous substrate bioreactors
Artificial Photosynthesis

3. Novel techniques of producing solar based hydrogen simultaneous direct production of hydrogen and electricity. The
HPEV cell has the potential to avoid the issue of mismatched tan-
Recently, there has been some very interesting research going dem component performance through the addition of a third
on which is focused on novel approaches of producing hydrogen. electrical terminal at the bottom junction which allows photo-
Some of those techniques will be discussed in this section. generated charge carriers, which are not consumed during the re-
Heremans et al. (2017) for the first time demonstrated a vapor-fed action, to get collected as electric current. As a consequence,
solar generator with KOH doped poly-vinyl-alcohol anion exchange electricity is generated simultaneously with hydrogen. Moreover,
membrane (AEM). The vapor-fed-based electrolysis device is the amount of required output products between hydrogen and
coupled with silicon solar cells. In their system, lower current electricity can also be tuned/controlled i.e. when the demand for
densities were generated (10 mA cm2) resulting in low Ohmic the electricity is high, the hydrogen output can be conveniently
losses in the electrolysis device under direct illumination. Accord- reduced to provide more supply of current to be harvested as
ing to them, the water-vapor content in air is adequate for feeding electrical power. As per the authors’ claim, the proposed device has
such solar-based hydrogen generator with water molecules even the promise of drastically augmenting the energy return on the
through natural convection. The authors claim that their device and supplied energy for PEC systems.
technique is capable of producing hydrogen with a STH efficiency of Tembhurne et al. (2019) presented a concept in which a PEC
15.1% over 1500 s at room temperature and a relative humidity of device was operated using concentrated solar thermal energy for
95%. Along with better efficiency, their device is capable of pro- hydrogen production through thermal integration, optimization of
ducing hydrogen at a better cost since it employs earth-abundant mass transport and a close electronic integration between the
catalysts. electrocatalyst and the photo absorber. According to the authors,
Segev et al. (2018) proposed a new category of devices classified the proposed concept can achieve high current densities while
as the hybrid photoelectrochemical and -voltaic cell (HPEV) for simultaneously maintaining high energy conversion efficiency,
6 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582

which is a fundamental challenge that the PEC method faces to production capacity demonstrated to have lower hydrogen costs
improve its competitiveness. An irradiation concentration of per kg.
around 474 kW/m2 for attaining high current densities of up to 0.88
A/cm2 was used by the authors along with an efficient thermal 5. Comparative evaluation of methods
management for ensuring better resistance towards degradation
and high energy conversion efficiency. They employed active The comparative evaluation is performed using two sets of
thermal management technique to facilitate conduction as well as criteria. Criteria set 1 comprises of cost and environmental impact
forced convection for cooling the photo absorber and providing comparisons. Criteria set 2 consists of exergy and energy effi-
thermal energy to the catalytic sites to enhance the overall per- ciencies, sustainability indices and rates of hydrogen production
formance. Based on their study, they claim that this approach has comparisons. The methods included for comparative evaluation in
the capacity of producing hydrogen at costs that seem to be criteria set 1 are PV-electrolysis, photoelectrolysis, biophotolysis,
competitive with those of traditional fuels thereby providing an photofermentation, steam or high-temperature electrolysis, SeI
encouraging route for a renewable hydrogen-based future. thermochemical cycle, CueCl thermochemical cycle, fossil fuel
reforming, biomass, and coal gasification processes. In criteria set 1,
4. Factors influencing the cost of hydrogen the thermochemical, reforming and gasification processes dis-
cussed are not solar-based due to lack of data availability of these
Various processes of solar hydrogen production using different methods. However, the data gives an insight into how these values
solar energy sources have been discussed in this section. The data would vary if these routes are solar energy driven. The methods
for production capacity, STH efficiency and cost of hydrogen is selected for comparative evaluation in criteria set 2 are PV-
€
taken from reference (El-Emam and Ozcan, 2019) and presented in electrolysis, solar thermal power generation and electrolysis, so-
Table 5. From the table, we can see the two fundamental factors lar steam or high-temperature electrolysis, solar water-splitting
which have been observed to influence the cost of hydrogen pro- thermochemical and hybrid thermochemical cycles, photo-
duction i.e. plant production capacity and solar technology incor- catalytic or PEC method, biophotolysis, artificial photosynthesis,
porated. The higher the capacity, the lower was the cost. Among all photofermentation, solar thermochemical H2S splitting, anaerobic
the processes considered herein, overall, the hybrid sulfur ther- digestion and solar thermal cracking of fossil fuels.
mochemical water-splitting method produces the most cost-
effective hydrogen while the algal method, which is a hybrid 5.1. Environmental impact and cost comparison
(biochemical and photonic) method, results in the most expensive
hydrogen. CO2 emissions, due to their deleterious environmental impact,
Even though, the concentrated solar thermal energy-based are considered the most fundamental of the GHGs and their
considered HyS plant had smaller capacity, it resulted in lower minimization is an issue that is supposed to be addressed by the
hydrogen production cost. Moreover, for other routes as well, when future energy carrier (Dincer and Acar, 2014). Methods such as CO2
concentrated solar thermal energy was employed for providing capture and sequestration (CCS) or utilization of the carbon dioxide
heat like in high-temperature steam electrolysis, the hydrogen as a commodity or waste in any industrial process have been widely
production cost was minimum. Furthermore, when considering the known to manage the GHGs in an effective way (Acar and Dincer,
systems using the same sources, the plants having higher 2015). The Global warming potential (GWP) and acidification

Table 5
Cost of hydrogen for various routes and plant capacities of hydrogen production.

Route Option/source with H2 prod. Solar-to- Cost of H2 ($/kg) Corrected Cost Cost of solar components
reference capacity (t/ hydrogen of H2 ($/kg in
day) efficiency (%) 2020)

PEM Solar PV (Choi, 2005) 1200 e 9 e e

Solar PV (Shaner et al., 10 9.76 12.1 (based on economic assumption values from 13.22 $210 ($229 in 2020) per
2016) U.S market & dollar value of 2014) m2 of solar collection
area
High- Concentrated Solar thermal 38 14 4.7 (based on H2A economic guidelines) e 385.3 M$
temperature (Kolb et al., 2007)
steam Stirling dish (Glatzmaier 1.3 20 10.5 (based on H2A economic guidelines) e e
electrolysis et al., 1998)
Concentrated Solar thermal 63 20 6.4 (based on H2A economic guidelines) e e
(Glatzmaier et al., 1998)
Zn/ZnO cycle Concentrated Solar thermal 6 20.8 7.98 (55 MW) and 14.75 (11 MW) (based on H2A e 2.7 M$
(Charvin et al., 2008) economic guidelines & dollar value of 2030 as
start-up)
HyS Concentrated Solar thermal 38.3 20 3.0 (based on H2A economic guidelines) e 314.6 M$
(Kolb et al., 2007)
Concentrated Solar thermal 100 40 3.2 (based on H2A economic guidelines & dollar 4.24 312.6 M$ (414.04 M$ in
(Corgnale and Summers, value of 2005) 2020)
2011)
Chassis Solar PV (Shaner et al., 10 9.76 11.4 (based on economic assumption values from 12.46 $40 ($43.7 in 2020) per
Membrane 2016) U.S market & dollar values of 2014) m2 of solar collection
electrolyzer area
CSPV (Shaner et al., 2016) 10 20 9.2 (based on economic assumption values from 10.05 $132 ($144.23 in 2020)
U.S market & dollar values of 2014) per m2 of solar collection
area
Algal method Solar Photonic (Amos, 0.3 e 13.5 e e
2004)
 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582 7

potential (AP) are the selected environmental impact categories

_
mLHV
according to the operational guide of the ISO standards to define h¼ (19)
the Life cycle assessments (LCA) procedures (JB, 2001). GWP is the E_in
measure of CO2 emissions and AP represents the SO2 discharge on
soil and into water (Ozbilen et al., 2011). where m_ represents the mass flow rate of hydrogen produced, LHV
In criteria set 1, the AP and GWP LCA results presented in abbreviates the lower heating value of hydrogen which is 121 MJ/kg
(Bhandari et al., 2014) and (Ozbilen et al., 2013) are utilized as the and E_ in is the input energy rate. Similarly, the exergy efficiency is
foundation of comparing environmental impact. Among the represented by the following equation:
various methods considered, fossil fuel reforming, coal, and
biomass gasification are the three hydrogen production processes _ ch
mex
j¼ _ (20)
with the highest AP and GWP while biophotolysis, photo- Exin
electrolysis and photofermentation exhibit the lowest GWP and AP
based on the data reported in references (Bhandari et al., 2014) and where exch is the chemical exergy of hydrogen and Ex_ is the input
in
(Ozbilen et al., 2013). Thus, it can be concluded that photonic exergy rate.
energy-based methods are the most environmentally benign pro- Based on the data presented in reference (Dincer and
cesses to generate solar hydrogen. On the contrary, gasification, and Zamfirescu, 2012), amongst the methods selected for criteria set
fossil fuel-based methods are of more harm to the environment. As 2, solar thermal energy-based water-splitting thermochemical cy-
stated previously, the data considered for reforming, thermo- cles, hybrid thermochemical cycles and solar fossil fuel cracking
chemical and gasification processes are not solar-based due to show the highest exergy and energy efficiencies. On the other hand,
limited data availability. However, if solar energy is utilized for PEC or photocatalytic methods are the least efficient methods of
supplying the required process heat, the environmental impact of hydrogen production.
the reforming and gasification processes will significantly reduce. The sustainability index (SI) is used for determining the sus-
With regards to the production cost of hydrogen, there are al- tainability of the considered routes of solar hydrogen production
ways certain ambiguities and uncertainties associated as it is based on exergy efficiency and is defined as:
influenced by various parameters and factors such as the cost of
feedstock to be used as an input, the advancement or maturity level SI ¼ 1  j (21)
of the production technology and the availability of current infra- The data used for exergy efficiencies (based on reference (Dincer
structure (Acar and Dincer, 2015). and Zamfirescu, 2012)) are used here for comparison of the SI.
Based on the data presented in Table 6, coal and biomass gasi- According to the data, processes having higher exergy efficiencies
fication, SeI and CueCl thermochemical cycles and biophotolysis result in lower SI values. Amongst the methods considered, pho-
are the most economical methods of producing hydrogen whereas tocatalysis or PEC and PV-electrolysis have the highest SI values
PV-, photo- and high-temperature electrolysis are the most whereas, solar thermochemical and hybrid thermochemical cycles
expensive routes of solar hydrogen production. As future work, exhibit the lowest SI values.
plenty of research is required for bringing down the cost of The hydrogen production capacities in MW for various methods
hydrogen through water electrolysis with respect to the exploita- considered in criteria set 2 are based on the data reported in
tion of solar PV/T. The cost of material (PV cells and electrolyzer), reference (Dincer and Zamfirescu, 2012). According to the data,
installation and maintenance all contribute towards the overall cost methods that utilize the solar thermal energy results in a much
for generating hydrogen. higher yield (except for solar cracking) in comparison to the pho-
tonic energy and biochemical energy-based methods, which have
extremely low rates of hydrogen production due to their lower STH
conversion efficiencies. Amongst the solar thermal-based methods,
5.2. Efficiency, sustainability index, and production capacity thermochemical water-splitting processes stand out as they have
comparison the highest hydrogen production capacities. The solar HTSE also
exhibits high production capacities as well as solar thermal power
This section compares and discusses the energy and exergy ef- generation and electrolysis. With further efforts, these values have
ficiencies, sustainability indices and capacities of hydrogen pro- the potential to jump further up as well.
duction of the various methods considered in criteria set 2. Overall, the processes which utilize high thermal energy
Efficiency, as defined in reference (Dincer and Acar, 2014), is the demonstrate higher efficiencies in producing hydrogen in com-
beneficial output by consumed input. The following equation is parison with the low-temperature methods. The photonic and
used to express the energy efficiency of a hydrogen generation biochemical methods of hydrogen production are more sustainable
process: but have lower efficiencies. Moreover, the solar thermal methods
are more suitable for hydrogen production at higher capacities
since they have much higher yields of hydrogen. Plenty of research
Table 6
Hydrogen production costs of various methods considered in criteria set 1.
is required for increasing the yield of these low temperature pho-
tonic and biochemical processes.
Methods Cost of hydrogen ($/kg) Reference

PV Electrolysis 5.78e23.27 Calise (2019)

Photoelectrolysis 10.36 6. Commercialization potential in the near future
Biophotolysis 1.42e2.13
Photofermentation 2.83
In this section, we will discuss about the current stage of tech-
High-temperature electrolysis 5.1e10.49
Fossil Fuel Reforming 2.08e2.27 nological development of various solar based hydrogen production
Biomass gasification 1.77e2.05 processes and the potential of their commercialization in the
Coal Gasification 1.34e1.63 coming future. Various factors play their part when it comes to the
Sulfur Iodine TC cycle 1.9 Ozbilen et al. (2013) commercialization of sustainable energy sources among which the
Copper Chlorine TC cycle 1.8
globally implemented energy policies play a vital role. Over the past
8 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582

decade, sustainability and environmental preservation have moved potential to become a low-cost pathway of storing electric power
up the priority list in the context of policy formulation among the for longer durations. This potential of hydrogen could be exploited
developed countries. Such policies help in regulating the costs only through collaborative global efforts for ensuring the conve-
associated with the commercial implementation of these sustain- nient transportation of hydrogen (as a fuel) from regions of abun-
able energy sources such as hydrogen. Another important factor is dant solar resources to energy scarce parts of the world. Moreover,
the technological and infrastructural readiness and process effi- the price of hydrogen for consumers is a function of hydrogen de-
ciencies of such systems having the potential and promise of livery per day and its utilization frequency. Regulating its price
replacing conventional methods. As discussed in the earlier sec- would require long term planning and strong collaborations be-
tions of this paper, some of the methods of solar hydrogen pro- tween industry, investors, and governments to present hydrogen as
duction are more efficient (thermochemical cycles, HTSE, etc.), an attractive alternate fuel for consumers to ensure sustainability.
some are more environmentally friendly (artificial photosynthesis, Furthermore, the implementation of effective global carbon taxing
photocatalysis, etc.) and some are more cost-effective (reforming, could greatly reduce GHG emissions (Metcalf, 2019) and could help
gasification, etc.). Photonic energy-based routes are the most support the cause of achieving sustainability on a large scale. Some
environmentally benign ways of producing hydrogen however, useful recommendations for scaling up hydrogen according to
they have lower production rates and conversion efficiencies which reference (“The future of hydrogen:, 2019) include establishing the
is why they are not a feasible option to be implemented for com- role of hydrogen in long-term energy policies and strategies,
mercial purposes as of now and in the near future. However, among stimulating commercial demand of green hydrogen, supporting
all photonic routes, PV electrolysis is a method having much higher R&D for bringing down costs and eliminating redundant regulatory
STH efficiency and is technologically mature as well. If the cost of hurdles.
the material associated with this method is regulated properly, it
can be commercialized soon for production at higher capacities. 8. Conclusions
Within the methods exploiting solar thermal energy, solar and
hybrid thermochemical water-splitting processes have the most This review discusses the different options and routes of solar
potential of commercialization readiness. They have been studied hydrogen production. Some literature review has been presented
extensively in the open literature. They have higher energy (38%) with their key results, conclusions, and recommendations. Several
and exergy (35%) efficiencies as well as better STH efficiencies methods and routes of solar hydrogen production are presented
(18%), better SI values (0.65) and can produce hydrogen at capac- along with the available technologies for their realization. More-
ities ranging between 75 and 400 MW. Since this method has over, some novel techniques and recent advances in solar-based
relatively lower thermal energy requirements, the material selec- hydrogen generation are presented. We also discussed some plant
tion and cost are also not a big constraint in its commercialization. configurations taking various ways of harnessing solar energy as
Moreover, a wide range of solar thermal options can be considered well as different routes. A couple of factors that seem to influence
for exploiting heat energy. However, material, installation and the cost of hydrogen production are the plant capacity to generate
maintenance cost of components associated with harnessing solar hydrogen and the solar technology incorporated for supplying
thermal energy may result in increasing the cost of per kg hydrogen either thermal, electrical or photonic energy. Based on the data and
produced. Hence, the regulation of all these costs is an essential configurations considered, the hybrid sulfur thermochemical
part of commercializing solar thermochemical processes. SMR, as water-splitting cycle stands out as the most cost-effective meth-
mentioned earlier, is the most commonly utilized method of odology of obtaining hydrogen by employing concentrated solar
hydrogen production industrially since it produces hydrogen at thermal energy. The prime objective of this review is to compara-
higher efficiencies and capacities. At the same time, its increased tively evaluate the various processes of solar hydrogen production.
rate of methane utilization for providing process heat and as a Two sets of criteria have been considered for evaluating those
feedstock makes it a non-sustainable and non-environment methods. Criteria set 1 include environmental impact and cost of
friendly method of producing hydrogen. However, modification in production. Criteria set 2 include exergy and energy efficiencies,
this process by using concentrated solar thermal energy instead of sustainability index and hydrogen production rate. The methods
methane combustion can certainly make this method more sus- selected for criteria set 1 and 2 are different based on the available
tainable and environmentally benign than its conventional version. data. According to the overall comparison of criteria set 1, photonic
Solar driven HTSE has also demonstrated technological maturity energy-based methods and thermochemical CueCl and SeI water
and commercialization potential based on various investigations in splitting cycles are the most environmentally benign (GWP ranging
open literature and data provided in Table 5. Due to its higher STH between 0.4 and 2 kg CO2/kg H2 and AP ranging between 0.8 and
efficiency and lower electrical power consumption, it is one of the 2.5 g SO2/kg H2) whereas coal gasification is the most cost-effective.
most promising green methods of hydrogen production and a However, if coal gasification is provided solar thermal energy as
prime candidate for large scale commercial implementation. heat input, its cost-effectiveness and environmental impact could
improve much more. Moreover, high-temperature processes have a
7. Global sustainability measures more detrimental effect on the environment due to higher GHG
emissions. From the overall comparison of criteria set 2, high
Each of the methods considered for solar hydrogen production thermal energy-consuming processes are more energetically and
in this study possesses the capability of contributing towards exergetically efficient, however, at the same time, less sustainable
achieving sustainability through the generation of hydrogen as a in comparison to the lower efficiency photonic and biochemical
sustainable and cleaner fuel. However, other measures for sus- energy-based processes. Furthermore, solar thermal routes of
tainable development are also required to be taken in this regard. hydrogen production are more suited for large scale production due
According to reference (“The future of hydrogen:, 2019), the cost of to their higher hydrogen production rates.
hydrogen production using electricity from renewables (including As a recommendation for future work, further investigations
solar energy) could reduce by around 30% by 2030 due to the cost with regards to solar-based SMR, solar biomass gasification and
declination of renewables. Components such as electrolyzers, fuel solar coal gasification systems need to be performed along with
cells, and refueling kits could benefit if manufactured in bulk. As cost analysis so that realistic data can help compare these processes
one of the leading options for energy storage, hydrogen has the with and without solar thermal energy. This would help in a more
 F. Razi, I. Dincer / Journal of Cleaner Production 264 (2020) 121582 9

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Choi, J.H., 2005. Hydrogen Production Costs of Various Primary Energy Sources.
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