Energy Conversion and Management 134 (2017) 125–134

Contents lists available at ScienceDirect

Energy Conversion and Management

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

Potential for greenhouse gas emission reductions using surplus

electricity in hydrogen, methane and methanol production via
electrolysis
Ville Uusitalo a,⇑, Sanni Väisänen a, Eero Inkeri b, Risto Soukka a
a
Lappeenranta University of Technology, School of Energy Systems, Laboratory of Sustainability Science, P.O. Box 20, 53851 Lappeenranta, Finland
b
Lappeenranta University of Technology, School of Energy Systems, Laboratory of Thermodynamics, P.O. Box 20, 53851 Lappeenranta, Finland

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

Article history: Using a life cycle perspective, potentials for greenhouse gas emission reductions using various power-to-
Received 15 September 2016 x processes via electrolysis have been compared. Because of increasing renewable electricity production,
Received in revised form 1 December 2016 occasionally surplus renewable electricity is produced, which leads to situations where the price of elec-
Accepted 12 December 2016
tricity approach zero. This surplus electricity can be used in hydrogen, methane and methanol production
Available online 23 December 2016
via electrolysis and other additional processes. Life cycle assessments have been utilized to compare
these options in terms of greenhouse gas emission reductions. All of the power-to-x options studied lead
Keywords:
to greenhouse gas emission reductions as compared to conventional production processes based on fossil
Surplus electricity
Life cycle assessment
fuels. The highest greenhouse gas emission reductions can be gained when hydrogen from steam reform-
GHG emissions ing is replaced by hydrogen from the power-to-x process. High greenhouse gas emission reductions can
PtX also be achieved when power-to-x products are utilized as an energy source for transportation, replacing
Electrolysis fossil transportation fuels. A third option with high greenhouse gas emission reduction potential is
methane production, storing and electricity conversion in gas engines during peak consumption hours.
It is concluded that the power-to-x processes provide a good potential solution for reducing greenhouse
gas emissions in various sectors.
Ó 2016 Elsevier Ltd. All rights reserved.

1. Introduction The same also happened in Scotland during 2016 [56]. It is likely
that similar challenges will also appear in other regions in the near
Climate change due to increased greenhouse gas (GHG) emis- future.
sions is one of the greatest global environmental challenges. According to Plessmann et al. [45] global 100% renewable
Energy production by fossil fuel combustion is the most significant decentralized electricity supply scenario is feasible at decent cost
source of GHG emissions, comprising approximately 65% of global but requires electricity storages. The chief problem is that renew-
GHG emissions [17]. Various targets have been set for overcoming able electricity production peaks occur only temporarily and sepa-
the problems, such as the EU 20-20-20 target for reducing GHG rately from consumption peaks. Therefore, the price of electricity
emissions, increasing the use of renewable energy and to improve may drastically fall during those surplus electricity production
energy efficiency [16]. This has led to rapidly increasing production hours. Also, storage resources or dispatchable generation methods
of renewable energy. are needed in order for grid operators to balance demand and sup-
Increased renewable energy production may in turn lead to sit- ply on a real-time basis [34]. This surplus electricity can be stored
uations where electricity production is occasionally at a higher and used in several ways, depending on the energy form required
level than electricity consumption. This has already happened for as an outcome of the storage. When it is desirable to use surplus
instance in Germany, Scotland and Denmark, where there is rela- electricity later in the form of electricity, it can be stored in
tively high capacity for producing both wind and solar power. pumped hydro storages, compressed air storages or batteries.
According to Neslen [41] on windy conditions Denmark have been These processes are more detailed explained by Sternberg and Bar-
able to exceed domestic electricity consumption with wind power. dow [52], Beaudin et al. [4] and Ma et al. [35]. However, battery
technology is not yet where it needs to be for storing electricity
and balancing energy systems on a large scale [29]. A new solution
⇑ Corresponding author.
could be to produce liquid or gaseous fuels by means of using sur-
E-mail address: [email protected] (V. Uusitalo).

http://dx.doi.org/10.1016/j.enconman.2016.12.031
0196-8904/Ó 2016 Elsevier Ltd. All rights reserved.
126 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134

Nomenclature

CH3OH methanol H2O water

CH4 methane EC European Commission
CO2 carbon dioxide ISO International Organization for Standardization
EPA U.S. Environmental Protection Agency LCA life cycle assessment
GaBi LCA software MEA monoethanolamine
GHG greenhouse gas O2 oxygen
H2 hydrogen PtX power-to-X

plus electricity via electrolysis. These fuels could provide a large unclear. Oliveira et al. [44] did an LCA comparison of various elec-
energy storage capacity and an option to move energy from the tricity storage methods. Their conclusion is that from climate
electricity markets to other sectors, such as transportation. A change perspective electricity production methods have the high-
recent techno-economic comparison of different energy storage est contribution to the results. Spath and Mann [51] studied GHG
options have been carried out by Amirante et al. [2]. The study emissions from hydrogen production via electrolysis utilizing
shows rapid development in different storage options. renewable electricity. Their conclusion was that in the operational
The production of hydrocarbons and hydrogen would allow for phase, emissions are minimal, and that the majority of emissions
the use of hydrogen storage options and hydrogen utilization are related to the construction phase. Galindo et al. [23] compared
instead of direct electricity storing and power-to-power options. the economy of conventional methanol production with that of
Further, hydrogen production also facilitates the production of methanol production from CO2, and they concluded that conven-
other chemicals, such as methane and methanol, which have even tional methanol production is less expensive. They also collected
better storage characteristics [53]. All these options to produce data from previous studies on the GHG emissions of methanol pro-
something from renewable electricity via electrolysis and addi- duction from CO2. According to the previous studies, 1 kg of
tional processes are referred to as PtX (Power-to-X) in this paper. methanol produced from CO2 leads to 0.8 kg of CO2 emissions.
In addition to balancing electricity systems, hydrogen, methane Since then, development has occurred in the methanol conversion
and methanol have multiple utilization alternatives for energy, process. Schaaf et al. [48] conclude that methane production from
transportation, fertilizers and materials. Global markets for these surplus electricity and storage in natural gas grids enables a high
commodities are tremendous [18,37]. balancing option for the electricity system. Clemens et al. [10] have
Hydrogen can be produced through various types of electrolysis studied photocatalytic methane and methanol production from
processes. At the moment, the focus of research is on reducing cap- CO2. The weak point of this process is the high water consumption,
ital costs and integrating the compression of hydrogen into an elec- which may limit its use, especially in dry regions. There may also
trolysis process [57]. Methane can be produced via a be economic limitations as Bydny et al. [8] study shows that PtX
thermochemical catalytic or biological methanation of hydrogen. options cannot be operated profitably for bridging the balancing
Thermochemical catalytic methanation has been viewed as a more markets for power and gas currently without subsidizes.
potential option in the near future. Etogas started a 6 MW thermo- Due to the various utilization options and PtX routes, deciding
chemical catalytic methanation process in 2013 in Germany, which how surplus electricity should be utilized is challenging. We still
can be regarded as mature technology [47]. The good availability of lack knowledge about the ways and means that hold the most
natural gas, have been seen to limit large scale methanation plants potential for utilizing surplus electricity via PtX routes especially
[25]. Methanol can be produced with the hydrogenation of carbon compared to traditional production ways. In this paper, our focus
monoxide and carbon dioxide by using catalysts, which is also is on GHG emission reductions from these routes. Some are more
mature technology [3]. Various pilot-scale demonstration plants direct, such as conventional hydrogen, methane, and methanol
have confirmed the possibility to produce methanol from CO2 replacement with PtX products. However, backed by political deci-
captured from flue gas, and H2 from electrolysis [54]. In addition, sions and economic support, these fuels could also be utilized as
Mitsui Chemicals is working with a 100,000 t methanol plant that replacement of fossil-based transportations fuels or in various
uses CO2 from flue gas and H2 from the photochemical splitting of energy production options. The aim of this research is fourfold:
H2O [38]. (1) to calculate the GHG balance for various PtX options; (2) to
There are relatively few life cycle assessment (LCA) studies compare, for the same products, GHG emissions from PtX methods
related to surplus electricity utilization in different products and to GHG emissions from alternative production methods; (3) to pro-
energy options. Denholm and Kulcinski [13] have compared differ- vide recommendations for how PtX processes should be utilized in
ent electricity storage options from a life cycle perspective. Their order to gain the highest GHG emission reductions; and (4) to dis-
conclusions is that electricity generation method have the highest cuss the potential of PtX commodities for replacing conventional
contribution on climate change. However they did not include PtX fossil fuel-based systems globally.
processes in their study. The most thorough study has been carried This paper gives novel information related to GHG emission
out by Sternberg and Bardow [52], who have compared GHG emis- reductions for PtX processes and products compared to those pro-
sions results from various PtX processes. They found that the high- duced by fossil energy. The conclusions of the paper can help
est GHG emission reductions can be achieved by surplus electricity researchers, companies and decision makers to develop more sus-
use in heat pumps or in electric vehicles. However, they did not tainable electricity systems that are linked to fuel production.
include hydrogen compression electricity consumption in their
study, and there are various options for heat recycling also not
2. Materials and methods
included in their study. One of the key process steps of PtX is
CO2 capture. Sternberg and Bardow [52] did not include CO2
In this chapter at first general principles for the life cycle assess-
capture-related GHG emissions in the overall emissions of PtX
ment model have been presented. The second part of this chapter
products. Therefore, its importance from a GHGs standpoint is
presents detailed assumptions and data used in the model.
 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134 127

2.1. The LCA model transportation to replace other transportation fuels; however, it
is unclear which fuels they are actually replacing. Methane can
The core method of this research is life cycle assessment, which directly replace natural gas in gas-operated vehicles, but it could
has been carried out according to the instructions of the ISO 14040 also substitute for fossil fuel (petrol or diesel) if political decisions
[30] and 14044 standards. In addition, GaBi 6.0 [22] software and and economic support are directed towards higher amounts of gas-
databases have been applied for modelling. Additional data has operated vehicles or to the conversion of cars from petrol-operated
also been collected from relevant literature. The literature is pre- to gas-operated. Similarly, electricity produced from methane may
sented in a chapter ‘‘data and assumptions”. A model have been replace marginal electricity production methods if the methane
created to calculate the carbon footprints of different PtX products electricity production is adjusted to peak production hours.
and to compare these to similar products produced by conven-
tional processes. This research has been carried out in the EU oper- 2.2. Data and assumptions
ational environment. The functional unit used is 1 MJ of surplus
renewable electricity produced by wind power. Wind power was This section of the paper provides the data utilized in the mod-
chosen for the study because it holds the highest potential for pro- elling. The values in parentheses represent the potential variation
ducing surplus electricity in the EU [12]. of values, which have discuss later in the sensitivity analysis. The
The LCA model was created so that hydrogen, methane and model has mainly been created so that the PtX processes are mod-
methanol production via PtX could be compared to alternative elled based on values from the literature. The replaced conven-
options for producing these products (Fig. 1). tional processes and energy production processes have been
In addition, the products can be used to replace other fuels and modelled based on GaBi 6.0 [22] database values. Direct surplus
energy systems indirectly, for instance in the transportation sector. electricity use in heat pumps or electric vehicles is excluded from
These comparisons have been classified into two options: (1) this study because this has already been studied by Sternberg and
primary product replacement, and (2) secondary use replacement. Bardow [52].
In the case of the first option – primary product replacement – Electrolysis is the first step in transforming surplus electricity
hydrogen, methane and methanol directly replace hydrogen, into different commodities. In the electrolysis process, H2O is sep-
methane and methanol from alternative production processes. This arated into H2 and O2 with the use of a direct electric current. There
substitution may be well-justified because it does not require any are three main electrolysis methods available: (1) alkaline electrol-
additional uncertain assumptions which could be related to the ysis cell (AEC), (2) proton exchange membrane electrolyzer (PEM),
secondary use replacement. Justifying the second option – sec- and (3) high temperature electrolysis. For the purposes of this
ondary use replacement – is more complicated. To illustrate, all research, proton exchange membrane technology has been
of the products under study can be used as energy sources for selected. This is because in comparison to the other production

PRIMARY PRODUCTS SECONDARY USE

OXYGEN FROM
O2 CRYOGENIC AIR
RENEWABLE SURPLUS ELECTRICITY SEPARATION

HYDROGEN FROM STEAM

ELECTROLYSIS H2 REFORMING

HYDROGEN VEHICLES FOSSIL PETROL

H2
H2
GAS VEHICLES FOSSIL PETROL

CO2 METHANATION CH4 NATURAL GAS

HEAT PRODUCTION
GAS ENGINE
FROM NG

ELECTRICITY
PRODUCTION

METHANOL FROM GAS

CO2 METHANOL CONVERSION CH3OH SYNTHESIS
ELECTRIC VEHICLES FOSSIL P
PETROL
ETROL

METHANOL VEHICLES FOSSIL PETROL

PROPYLENE
LURGI MTP PROCESS
PRODUCTION

PRODUCTION OR UTILIZATION PROCESS

PtX PRODUCT

CONVENTIONAL PRODUCTION PROCESS

Fig. 1. LCA model for PtX processes, primary product replacement and secondary use replacement.
128 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134

methods, the slightly higher efficiency and shorter startup time most potential in the near future [47]. This technology is still under
improve the usability of this electrolyzer when a variable electric- development. The methanation process is exothermic, thus provid-
ity source is used in production [20]. According to Sternberg and ing heat in addition to main products. Reaction (R2) presents the
Bardow [52] 1 MJ electricity can produce approximately 0.0052 methanation process [25]. It is assumed that the conversion pro-
(0.0050–0.0061) kg of H2. Based on Reaction (R1), this requires cess for methanation is 95% [52]; therefore, a little unconverted
0.046 kg of H2O and also produces 0.041 kg of O2. H2 and CO2 remain in the product gas. The methanation process
is further described in Helmeth.
1 1
H2 O ) H2 þ O2 ðR1Þ CO2 þ 4H2 ) CH4 þ 2H2 O DhR ¼ 165 kJ mol ðR2Þ
2
In addition to hydrogen, production of hydrocarbons requires In the methanol conversion process, CO2 and H2 are converted
carbon feed for the process in the form of CO or CO2. In this study, into methanol and water via chemical reactions in the presence
carbon is taken from the flue gas of a combustion plant as CO2, of the catalyst. The reaction is exothermic as well and is presented
because worldwide, there are tremendous amounts of CO2 avail- in Reaction (R3) [52]. The methanol conversion process produces a
able. There exist various methods for separating CO2 from the flue mixture of gas, which is cooled down in order to condense the
gases. This separation can be based on absorption, adsorption, formed methanol and water. The unreacted CO2 and H2 are cycled
membranes, or other physical and biological separation methods back into the process, whereas the methanol is separated from the
[1]. Monoethanolamine (MEA) absorption is a commercially avail- water and purified. Evald et al. [19] very high selectivity, i.e. near
able and commonly utilized separation method for CO2 in biogas 100%, has been attained for methanol using a SiO2-modified Cu/
production [46]. In addition it can also be used in power plants ZnO catalyst [54]. Methanol conversion is described in more detail
to capture CO2 as is presented by Fytianos [21] and Abu-Zahra in Suhas et al. [54].
et al. [1]. Thus, that technology was chosen for this study. MEA 1
CO2 þ 3H2 ) CH3 OH þ H2 O DhR ¼ 49 kJ mol ðR3Þ
has a strong affinity for CO2, but the regeneration process requires
high temperatures and therefore thermal energy use [1]. A small Based on Reactions (R2) and (R3), inputs and outputs for metha-
proportion of MEA has to be constantly removed from the process nation and methanol conversion processes can be calculated. The
and replaced with new MEA due to the MEA degradation. MEA results and additional data are presented here in Table 1.
degradation leads to problems with corrosion, among other things. Additionally, different ratios have been presented for the
MEA degradation and resulting problems are further described in methanol conversion process. Evald et al. [19] present that the
Fytianos [21] and Zhou [62]. Fig. 2 presents modelling of MEA pro- CO2:H2 ratio can be approximately 1:3, and that energy consump-
duction and CO2 capture processes. After capture, CO2 is com- tion in the process is much higher than assumed. This is probably
pressed for storage before the hydrocarbon production. The due to rapidly developing technology. In this case, a relatively high
electricity consumption in CO2 compression is assumed to be amount of extra CO2 is added to the process, but the carbon
0.61 MJ kg1 of CO2 [61]. amount in the methanol produced is similar whether extra CO2
In the methanation process, CO2 can be converted to methane is added to the process or not. Capturing and storing extra CO2 nev-
via chemical reactions. A thermochemical catalyst was selected ertheless leads to additional GHG emissions, especially in electric-
for this study because it has been viewed as the method with the ity consumption.

THERMAL ENERGY
CO2 ABSORBTION ELECTRICITY
PRODUCTION BY
PRODUCTION
NATURAL GAS
2280 MJ 695 MJ
FLUE GAS CO2 1000 kg
MEA 20000 kg
CO2 1000 kg
ABSORPTION REGENERATION

FLUE GAS MEA 20000 kg MEA 1.5 KG

THERMAL ENERGY
PRODUCTION BY MEA PRODUCTION
NATURAL GAS EMISSIONS TO AIR:
3 MJ AMMONIA 0.00237 kg
CO2 0.03975 kg
ELECTRICITY
PRODUCTION 1
1.8
.8 MJ MEA 1.5 KG
MEA PRODUCTION
AMMONIA
1
1.182
.182 kgg
PRODUCTION WASTE HEAT 1.8 MJ

ETHYLENE OXIDE 1.224 kg

PRODUCTION SYSTEM BOUNDARY

Fig. 2. Monoethanolamine (MEA) absorption process for CO2 and the MEA production process [1,32]. Production of process inputs are presented as boxes with dash line and
actual processes of CCS as boxes with solid line.
 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134 129

Table 1 Table 2
Inputs and outputs for methanation and methanol conversion processes [19,31,52]. Initial data related to vehicle use of various PtX processes [39,52].

Methanation Methanol conversion Energy Vehicle type Tank-to-wheel

source efficiency,
Inputs Outputs Inputs Outputs
MJ km1
CO2 (kg) 2.89 0.14 1.38 0
Hydrogen Fuel cell vehicle 1.30
H2 (kg) 0.53 0.03 0.19 0
Methane Gas-operated vehicle developed for natural 1.87 (2.3)
CH4 (kg) 0 1 0 0
gas
CH3OH (kg) 0 0 0 1
Methanol Traditional petrol cars in small portions or 1.58 (2.5)
H2O (kg) 0 2.25 0 0.56
in cars developed for methanol use
Electricity (MJ) 1.19 0 4.78 0
Electricity Electric vehicles 0.65 (0.40–0.79)
Heat (MJ) 0 10.53 0 1.23

Various utilization options exist for hydrogen, as it can be used production methods in the EU. For reference processes, GaBi
directly in hydrogen-operated vehicles or as a chemical. The major databases have been utilized. In addition, for methanol
chemical applications for hydrogen are fuel production processes production from fossil syngas, GHG emissions are approximately
and ammonia production. Traditionally, hydrogen has been pro- 1 kg CO2 kg CH3OH1 [36]. Higher GHG emission factors
duced from natural gas with a steam reforming process. This pro- have been presented for methanol production, varying from
cess leads to relatively high GHG emissions because carbon from 3.8 kg CO2 kg CH3OH1 (coal) to 1.6 kg CO2 kg CH3OH1 (natural
the methane reacts to CO2 [58]. Hydrogen utilization requires com- gas), but in this paper, the lower value has been utilized [23].
pression or liquefaction of hydrogen. Both consume relatively high Electricity and heat production from methane requires the use
amounts of electricity depending on the length of the storage per- of gas engines or gas turbines. Due to its high electricity-
iod [26,58]. For the purposes of this paper, it is assumed that the production efficiency, a gas engine has been chosen for this study.
hydrogen production is at close range from its utilization; thus, An example gas engine used in the model is TCG 2020 V16. The
no long-term storage would be needed. Compression for low pres- electricity and heat production efficiencies for the gas engine are
sure and for the methanation or methanol conversion processes both 0.42 [15]. The calculations have also been carried for lower
requires only about 1% of hydrogen energy content [6]. electricity production efficiency (35%) if for example gas turbines
In addition to hydrogen, electrolysis also produces oxygen. Pure are utilized. Use of Organic Rankine Cycle technology could slightly
oxygen is used in numerous industries for a variety of reasons and increase electricity production capacity, but this option has not
also in medicine, aircraft and submarine applications. Oxygen can been studied in this paper [11].
be produced with certain processes, such as cryogenic separation
and pressure swing adsorption; or by using membranes and pass-
ing air through a membrane filter [50]. Oxygen is also formed as a 3. Results and discussion
by-product from processes where nitrogen is produced from air
[55]. In some cases, oxygen use may not directly replace oxygen In this section, the GHG emissions for various PtX products and
produced by a cryogenic process. In the majority of oxygen- their uses as well as the GHG emissions from alternative produc-
consuming processes, such as combustion and aeration in waste tion methods have been presented. In addition, the applicability
water treatment, oxygen is added as air. However, if pure oxygen of PtX for different sectors have been discussed. The GHG balance
from electrolysis is available, there can be various advantages over results for the production of H2, CH4 and CH3OH is presented in
air use. This is because there is 78% nitrogen in air, leading to Fig. 3. Similar products can be further directed for secondary use.
unnecessary electricity use in compression and to unnecessary GHG emissions for transportation uses are presented in Fig. 4.
capacity investments, for example. The first bars in the figures present GHG emissions and sources
Methane can be used in various energy production processes from PtX processes. The second bar summarizes these GHG emis-
developed for natural gas. In addition, methane is utilized for sions. The third bar presents GHG emissions from reference cases.
instance as feedstock in hydrogen production via steam reforming. The reference case bar also includes an option to replace reference
There is tremendous demand for methane, and EU28 natural gas oxygen production with oxygen produced in electrolysis.
consumption alone was 18,000 TJ in 2014 [18]. As can be seen in Fig. 3, with the use of a PtX process, hydrogen
Methanol is a feedstock for various chemical applications. It can can be produced with very low GHG emissions. Emissions from
be utilized in plastic and paint production, for example. It is also an hydrogen production are mainly related to renewable electricity
energy carrier and can be employed for energy production or as a production. The renewable electricity utilized in electrolysis was
transportation fuel. Worldwide, 180,000 t of methanol is used daily assumed to be produced by wind power. If the electricity had been
[37]. produced by solar power, the GHG emissions from this phase
Distributing hydrogen, methane, methanol or electricity for would be slightly higher [40]. In addition, changes in electrolysis
transportation use requires compression and pumping processes. efficiency would either improve or weaken GHG emission perfor-
For vehicle use, hydrogen must be compressed to approximately mance of PtX solutions, compared to the alternative production
600 bars of pressure [9]. The compression consumes approxi- methods. However, changes in electrolysis efficiency do not affect
mately 11% of hydrogen energy content [6]. According to Uusitalo the order of different PtX routes in terms of GHG emissions. The
et al. [59], methane compression and distribution in 55 bars of electricity production method could also be something else, but
pressure consumes 0.71 MJe kg1 methane. In addition, compression to in the cases here, the GHG emissions are directly linked to the pro-
250 bars, which is the tank pressure of the vehicle, requires an addi- duction method. The electrolysis process is assumed to have no
tional 0.29 MJe kg1
methane electricity. Methanol refueling consumes direct GHG emissions. Methane and methanol production lead to
0.07 MJe kg1
methanol electricity [5]. negative GHG emissions, due to the CO2 capture. The majority of
For secondary use, comparisons of tank-to-wheel efficiencies of GHG emissions from these processes are related to the electricity
different vehicle types play an important role. Data related to vehi- use in the CO2 and H2 compressions as well as in the methanation
cle use is presented in Table 2. and methanol conversion processes. Methanol conversion results
For the purposes of this paper, it is assumed that all electricity in higher GHG emissions than methanation because the electricity
consumed in the processes is produced by average electricity consumption is approximately four times higher in the former.
130 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134

Fig. 3. A comparison of GHG emissions from H2, CH4 and CH3OH production, according to PtX route used or alternative production method used.

Fig. 4. GHG emissions from PtX products and reference fuels in the transportation sector.

Evald et al. [19] have presented an even much higher electricity leads to the lowest GHG emissions of the studied options. How-
consumption for methanol conversion, which would significantly ever, alternative methane production methods (natural gas) have
increase methanol conversion bar in Fig. 3. Methane production relatively lower GHG emissions than alternative H2 and CH3OH
 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134 131

production methods. The highest GHG emission reduction can be duty vehicles. Electricity is applicable only in light-duty vehicles
achieved by replacing H2 from steam reforming with H2 from due to limitations of battery technology. There are 0.7 million elec-
PtX. In Fig. 3, GHG emissions from methane or methanol combus- tric vehicles globally, and they represent only 0.08% of all vehicles.
tion are not included, but the combustion emissions are similar, Nevertheless, in some locations, such as in Norway, the share of
whether they come from conventional production routes or from electric vehicles is as much as 12% [27,28]. There are only a little
PtX routes. over 10,000 hydrogen-operated vehicles worldwide. One of the
There are also other developing options to utilize renewable biggest challenges with hydrogen-operated vehicles is the com-
surplus electricity in methane and methanol production which pression requirements for hydrogen fuel. Methanol is one option
are not included in this study. Some methanogen microorganisms for future synthetic fuel, and it is currently used in cars with high
can metabolize electricity into chemical energy in the form of compression engines (e.g. race cars) for performance and safety
methane. These methanogens require also CO2 which can be cap- reasons. Methanol can be blended with fossil-fuel petrol, but any
tured from flue gas or from the atmosphere. However there are still amount of ethanol in the fuel will further limit blending options.
challenges with large scale process [49]. This process is more Also, higher methanol blends are possible alongside engine modi-
detailed described by Deutzmann et al. [14]. fications, but currently, the global amount of methanol vehicles
Amine technology was utilized to capture CO2 from flue gas is marginal. Methanol has fire-safety advantages over petrol, and
flow. With this technology, electricity and heat production pro- vehicle motor and fuel systems in current use can be converted
cesses result in relatively high GHG emissions: GHG emissions to utilize methanol relatively easily. The use, handling and distri-
are 9% from electricity use and 16–17% from heat use. With the bution processes of methanol resemble in large part those of petrol
use of other CO2 capture technologies, electricity and heat con- [43]. One drawback for methanol use in transportation is low
sumption could be lower, but amine technology was chosen for energy density – only half that of petrol. This means that more
this study because it is commercially available. Attractive options methanol needs to be distributed and used on a weight basis. On
for obtaining CO2 could also be biogas plants or biofuel production the other hand, compared to hydrogen, methanol requires less vol-
incorporating hydrotreatment. These processes produce almost ume for the same energy content [43].
pure CO2 that could be applied in PtX processes [59,60]. Fig. 5 presents the GHG reduction potential of electricity pro-
Fig. 4 presents a situation where PtX products are directed to duction using methane as compared to average and marginal elec-
transportation use. As the figure illustrates, all of these options tricity production. Particularly high GHG reductions can be
lead to GHG emission reductions as compared to fossil petrol achieved if the methane is stored and utilized for electricity pro-
use. The reductions with transportation use are even higher than duction during peak production hours. For the purposes of this
those for primary product replacement, which confirms the con- paper, the electricity produced from methane is assumed to
clusions of Sternberg and Bardow [52]. Methanol use leads to replace marginal electricity produced by coal. However, most of
lower reductions than the other options because of the higher fuel the variation between electricity consumption and production is
emissions from methanol combustion. The life cycle GHG emis- adjusted by hydropower. Therefore, the peaks from the utilization
sions for methanol are approximately at the same level as those of fossil fuel-based marginal electricity may become rarer in the
presented previously by Galindo et al. [23]. Methane and methanol future. If a gas turbine or a gas engine with a lower efficiency
use in vehicles leads to the release of CO2 captured in the MEA pro- would have been used instead of the chosen gas engine type espe-
cess. The highest GHG emission reductions would be achieved with cially the amount of electricity produced could have been dropped.
hydrogen use. However, it is important to note that the vehicle In this case a smaller amount electricity could have been replaced.
engine efficiencies and the assumptions related to the engine effi- In Fig. 5 GHG emissions from the replaced processes are displayed
ciencies have significant impacts on the results. For example, a 10% also when electricity production efficiency is 35%. As can be seen in
reduction or improvement in engine efficiency would decrease or the figure reductions in electricity production efficiency also
increase the reference petrol use bar by 10%. Therefore, in real reduce GHG emissions reduction potential. However the process
decision-making situations, attention should be paid to the vehicle still leads to GHG emission reductions.
types chosen for the study. There are also opportunities for heat integrations and heat uti-
Globally, there are 20 million gas-operated vehicles [42]. Petrol- lization in PtX processes. CO2 capture requires heating, which in
operated vehicles can be modified to use gaseous fuel at relatively this paper was assumed to be produced by natural gas. In addition,
low costs. In addition, methane is also an applicable fuel for heavy- both methanation and methanol conversion processes produce

0.08
0.07
0.06
0.05
kgCO2eq

0.04
0.03
0.02
0.01
0.00
-0.01
-0.02
CH4 CHP Total Reference Reference Reference Reference
average el. marginal el. average el. marginal el.
(42%) (42%) (35%) (35%)

PtX process Fuel emissions Total Reference electricity Reference heat from NG

Fig. 5. Comparison of GHG emissions from PtX methane production and from further electricity production from methane with those of average electricity and marginal
electricity (coal based) production. Electricity production efficiency is displayed in parenthesis (42% and 35%).
132 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134

0.04 Table 3
Sensitivity analysis of initial data.
0.03
Initial data Effect on GHG reduction (%)

0.02 Initial data Initial data

10% +10%
kgCO2eq

0.01 Primary use

H2
0.00 Emissions factor of wind power +0.4 0.4
Electrolysis efficiency 9.6 +9.6
a a
Emissions factor of H2O production
-0.01
CH4
-0.02 Electricity consumption in methanation +0.9 0.9
CH4 (PtX) total Reference CH3OH (PtX) total Reference Electricity consumption in CO2 capture +1.3 1.3
Heat consumption in CO2 capture +2.2 2.2
PtX Natural gas producon Oxygen producon Heat producon Electricity consumption in CO2 +1.3 1.3
compression
Fig. 6. Comparison of GHG emissions from methanation and methanol processes Methanation efficiency 14.2 +7.1b
a a
with the reference processes when heat is utilized. MEA production
a a
H2 compression
Electrolysis efficiency +8.7 8.7
CH3OH
heat because they are exothermic processes. Heat integration Electricity consumption in methanol +4.6 4.6
could be carried out by directing heat from methanation or metha- conversion
nol conversion processes to CO2 capture. It is also possible to use Electricity consumption in CO2 capture +0.9 0.9
Heat consumption in CO2 capture +1.6 1.6
heat from these processes in other heat-consuming applications
Electricity consumption in CO2 +0.8 0.8
that are available at close range. Methanation produces more heat compression
(0.10 MJ) than required for the CO2 capture (0.06 MJ), but all the Methanol conversion efficiency c
7
a a
heat from the methanol conversion process (0.03 MJ) could be uti- MEA production
a a
H2 compression
lized in CO2 capture (0.09 MJ). Fig. 6 presents the effects of heat
Electrolysis efficiency +9.6 9.6
utilization on GHG emissions.
Secondary use
Further on a sensitivity analysis have been carried out for differ-
Hydrogen vehicle efficiency 11.3 +11.3
ent factors in the model. Analysis have been carried out so that ini- CH4 vehicle efficiency 14.0 +14.0
tial data values have been modified at a range from 10% to +10%. Electric vehicle efficiency 12.8 +12.8
Effects of variation are presented in Table 3. Methanol vehicle efficiency 18.3 +18.3
As can be seen Table 3. Production efficiencies in electrolysis, a
Factors that lead less than 0.001 kg CO2eq emissions are discarded from the
methanation and methanol conversion have the highest effect on sensitivity analysis.
the results. In addition vehicle efficiencies have high impact on b
Methanation efficiency can be improved only by 5%.
c
secondary use options. Other factors and initial data assumptions Methanol conversion efficiency cannot be improved anymore.
have minor impact on the results.
Potential for PtX products can be roughly estimated by calculat-
Table 4
ing how many different products could be produced if a 3 MW
Product potentials when a 3 MW wind turbine produced electricity for electrolysis.
wind turbine with an operational period of 2200 h were to produce
electricity for the electrolysis process. Annually, 20 million t of Product t a1 Vehicle use km a1 Cars

hydrogen is utilized for ammonia production worldwide, H2 123 H2 car 11,380,000 632
360,000 t of hydrogen are consumed in the EU, and over 1 million O2 974 CH4 car 6,230,000 346
CH4 233 CH3OH car 8,270,000 459
gas-operated vehicles are used in the EU [42,18]. In reality, only a
CH3OH 656 Electric car (CH4) 7,560,000 420
portion of electricity produced by wind power is actually surplus Electric car (direct) 36,550,000 2031
electricity. Table 2 shows the potential of each product (H2, O2,
CH4, and CH3OH) to produce different PtX products, if all the elec-
tricity from a 3 MW wind turbine were utilized. Table 4 also shows
the potential for direct electricity use in electric vehicles. Accord- rently the most economic option but PEM electrolysis could be bet-
ing to both Table 4 and to the total consumptions provided above ter suited for PtX processes due to its better performance in
in the text, there is a huge potential for production of all the PtX transient operation. Their study also show that catalytic methana-
products, so production should be directed towards those path- tion requires smaller reactor size and is more efficient than biolog-
ways that pose the highest potential for GHG emission reductions. ical methanation. However biological methanation has a higher
One of the major technical challenge related to PtX processes is tolerance for impurities. According to the study none of the pro-
that wind power production is intermittent. Therefore there may cesses is competitive with natural gas or biomethane production.
be challenges on how electrolysis, methanation and methanol con- Hydrogen production cost dominates the whole process costs.
version can be applied. It is likely that electrolysis process can be For feasibility different services such as mobility, electricity grid
adjusted based on wind power availability but a more stable driv- balancing and CO2 services have to be combined. Breyer et al. [7]
ing would be needed for methanation and methanol conversion found out that PtX integrated to an existing pulp mill is already
[20]. To create smooth operational conditions a hydrogen storage profitable. At the moment there are various projects going on to
may be required. However this issue should be further studied. combine operations of renewable electricity production, electroly-
There are still challenges in feasibility and technical operations sis, CO2 capture and methanation process. For example a test facil-
of renewable electricity, electrolysis and methanation or methanol ity will start operation in Finland in 2017 [33].
conversion combinations. Götz et al. [24] compared various elec- In the future, more research is required to determine how GHG
trolysis and methanation processes from technical and economic emissions from different sectors could be most effectively
perspectives. According to their study alkaline electrolysis is cur- decreased. This paper demonstrates the GHG reduction potential
 V. Uusitalo et al. / Energy Conversion and Management 134 (2017) 125–134 133

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