Sustainable Production and Consumption 30 (2022) 301–315

Contents lists available at ScienceDirect

Sustainable Production and Consumption

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

Environmental impacts of the production of synthetic natural gas from

industrial carbon dioxide
Remi Chauvy a,b, Lionel Dubois c, Diane Thomas c, Guy De Weireld a,∗
a
Thermodynamics and Mathematical Physics Unit, University of Mons, 20 Place du Parc, 7000 Mons, Belgium
b
Environmental Engineering Department, National Cheng Kung University, No.1 University Road, 70101 Tainan City, Taiwan, ROC
c
Chemical and Biochemical Process Engineering Unit, University of Mons, 20 Place du Parc, 7000 Mons, Belgium

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

Article history: Power-to-Gas technologies (PtG) are regarded as promising options to defossilize the energy system by
Received 22 April 2021 converting and storing renewable electricity to gases. When combined with carbon capture and utiliza-
Revised 30 November 2021
tion from large point sources, such as energy intensive and hard-to-abate sectors, where a major part
Accepted 4 December 2021
of CO2 emissions cannot be avoided, PtG technologies can also play a role to mitigate CO2 emissions.
Available online 7 December 2021
However, these technologies have several environmental impacts throughout their lifetimes that must
Editor: Dr. Raymond Tan be assessed, due to the use of resources, materials, and energy, as well as the formation of chemical by-
products. Using a Life Cycle Assessment (LCA) methodology, this paper aims to assess the most significant
Keywords:
Power-to-gas technology environmental impacts of an integrated PtG system including the conversion of renewable energy to hy-
CO2 capture and utilization drogen through water wind-based electrolysis, that is further converted to synthetic natural gas (SNG) by
Techno-economic investigation reacting with captured CO2 from a cement plant flue gas. More precisely, the present work innovates on
Life cycle assessment both the technical and methodological perspectives. An advanced CO2 capture process is implemented,
Uncertainty analysis using mixed amines solvent and innovative configuration to reduce the energy consumption to 2.3 GJ
per tCO2 captured, and include an optimized heat integration with the CO2 conversion step. A hybrid
approach combining physical and economic input data is also considered for the life cycle inventory. Ad-
ditionally, both subdivision and system expansion via substitution approaches are applied to consider the
multi-functionality of the systems. Simulation results show that the PtG process with CO2 captured from
cement plants flue gas reduces the overall GHG emissions by 76%. Similarly, the fossil resource scarcity is
drastically reduced by over 80% thanks to the heat integration between the CO2 capture and the CO2 con-
version processes, but also thanks to the substitution of natural gas by the CO2 -based SNG. Nevertheless,
environmental impacts of PtG are higher than conventional natural gas production for other impact cat-
egories, including freshwater eutrophication, terrestrial acidification, and mineral resource scarcity. Both
data uncertainties, assessing the knowledge base underlying the input data parameters, and sensitivity
analysis, assessing the value range of the parameters respectively to the environmental indicators, are
conducted to test the results and highlight the uncertainty hotspots.
© 2021 Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

1. Introduction

Abbreviation: AC, Acidification; ASU, Air Separation Unit; CC, Climate Change;
CCU, Carbon Capture And Utilization; CCUS, Carbon Capture, Utilization And Stor-
With international climate targets aiming to reach climate neu-
age; CCS, Carbon Capture And Storage; CEPCI, Chemical Engineering Plant Cost In- trality by 2050, renewable energy share is continuously increasing,
dex; DE, Germany; EIO-LCA, Economic Input-Output Life Cycle Analysis; EU, Euro- allowing environmentally friendly power production. Simultane-
pean Union; FCI, Fixed Capital Investment; FE, Freshwater Eutrophication; FS, Fossil ously, the increase of renewable energy involves challenging situ-
Resource Scarcity; GHG, Greenhouse Gases; HT, Human Toxicity; I-O, Input-Output;
ations, especially in power grids management (Gielen et al., 2019).
ICA, Inter-Cooled Absorber; LCA, Life Cycle Assessment; LCI, Life Cycle Inventory;
MDEA, Methyl Diethanolamine; MEA, Mono- Ethanolamine; MS, Mineral Resource It is accompanied by growing issues in terms of transmission
Scarcity; NACE, Nomenclature Statistique des Activités Économiques dans la Com- and distribution loads, where conventional power generation sta-
munauté Européenne; NG, Natural Gas; NR, Natural Resources; PEC, Purchased tions can hardly compensate power output fluctuations of increas-
Equipment Cost; PEM, Polymer Electrolyte Membrane Electrolysis; PtG, Power-to- ing number of wind and photovoltaic technologies (Abdon et al.,
Gas; PZ, Piperazine; RAMON, Reference And Management Of Nomenclatures; RVC,
Rich vapour Compression; SNG, Synthetic Natural Gas; TA, Terrestrial Acidification;
US, United States; WU, Water Use; WW, Water-Wash.
∗
Corresponding author. E-mail address: guy.deweireld@umons.ac.be (G. De Weireld).

https://doi.org/10.1016/j.spc.2021.12.004
2352-5509/© 2021 Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
R. Chauvy, L. Dubois, D. Thomas et al.
2017). Additionally, the ability to respond to fluctuating renew-
able sources is central in order to accommodate multiple grid
services, including spinning reserve, grid stability, and reliability
(Guandalini et al., 2015). Several storage technologies are avail-
able, such as pumped hydroelectric energy storage, compressed air
energy storage, flywheel, batteries, or hydrogen storage technolo-
gies, with different prices, duration, yield, and storage capacities
(Breeze, 2018). However, daily and seasonal fluctuations of renew-
able resources lead to differences in energy demand and renew-
able energy supply, and variations on electrical generation output
(Eveloy and Gebreegziabher, 2018). High penetration of intermit-
tent renewables is likely to require long-term energy storage. In
addition to electricity storage, a promising option is to couple the
electricity and gas sectors by converting renewable electricity to
hydrogen and, in a second step, to synthetic natural gas (SNG)
(Zhang et al., 2020).
Power-to-Gas (PtG) is thus an up-and-coming attractive tech-
nology due to its flexibility; in relation to time, location, and end-
use; to convert electricity to gases for large-scale and long-term
energy storage, and its utilization of existing natural gas infras-
tructure, reducing thus the capital investment. It could be framed
in ambitious plans to defossilize thermal energy consuming indus-
tries, while keeping the majority of current technologies and thus
avoiding, in the short term, significant modifications of processes
consuming fossil-based energy (van Leeuwen and Mulder, 2018).
This technology starts with converting electricity to renewable
hydrogen through water electrolysis (Power-to-hydrogen). Hydro-
gen can be either injected to natural gas network; or used in other
applications that require hydrogen as feedstock or fuel. Renewable
hydrogen can also react with carbon dioxide to produce synthetic
natural gas, containing mainly methane (Power-to-methane), that
is then conditioned to be either injected and stored in the existing
natural gas network, or supplied as fuel to power a vehicle.
Additionally, to face the challenges of climate change and
limit the climate-altering emissions, several international agree-
ments have highlighted that Carbon Capture, Utilization and Stor-
age (CCUS), is essential to reduce CO2 emissions in a sustainable
way (Masson-Delmotte et al., 2018). In a CCUS process, CO2 , cap-
tured from exhaust gases and purified, is either sequestered or
converted to valuable products (Anwar et al., 2020). The growing
recognition of CCUS was underlined by more than 30 events orga-
nized during the recent United Nation climate change conference
COP26, while the main world’s top greenhouse gas (GHG) emit-
ters, United States and China, commit to work together on the de-
ployment and application of these technologies (see the US– China
Joint Glasgow Declaration (US DoS 2021)). Additionally, the use of
alternative low-carbon fuels, including CO2 -derived fuels such as
SNG, to defossilize the already existing gas network and transport,
was intensively discussed in the conference. In the context of the
European Green Deal, which sets an ambitious plan and vision to
make Europe the first climate neutral continent by 2050, a group
of trade associations issued a joint call to include CCUS in the EU’s
Industrial Strategy. In particular, the conversion could drive the
development of novel techniques, products, and industries, while
achieving emission cuts especially in hard-to-abate sectors.
As highlighted by Müller et al. (2020), instinctively Carbon Cap-
ture and Utilization (CCU) may be expected as technologies with
potentially zero emissions or net-negative emissions over the en-
tire life cycle. In theory, it can be carbon neutral if direct air cap-
ture or fossil point sources are considered for CO2 capture together
with permanent sequestration or CO2 permanently stored in the
product, assuming all other emissions are null over the life cycle.
CCU technologies may even have negative emissions if overall life
cycle GHG emissions are lower than the amount of CO2 fixed. In
other cases, CCU have positive emissions over the entire life cy-
cle, even though they can be lower than conventional processes.
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Sustainable Production and Consumption 30 (2022) 301–315
In the transition phase to a low-carbon future, sources of unavoid-
able CO2 (e.g., CO2 coming from the decarbonation of limestone in
production of cement) should be considered (Meylan et al., 2017).
To this extent, the environmental performances of PtG tech-
nologies, examined through the Life cycle assessment (LCA)
method, must be evaluated before large-scale deployment. In the
existing literature, the environmental performance has been typ-
ically assessed for the GHG emissions, considering system varia-
tions (electricity supplies, electrolysis technologies, CO2 sources)
or limited applications of the final SNG produced. Based on
Thonemann (2020), an overview of the LCA studies focusing on PtG
technologies is carried out in the Supporting Information (see SI.1).
Sternberg and Bardow (2015) highlight that PtG demonstrates
environmental benefits if the hydrogen used is produced via
water electrolysis from so-called excess renewable energy. The
benefits related to the use of surplus energy is concurred by
Meylan et al. (2017), as the electricity production would other-
wise be curtailed. Zhang et al. (2017) highlight that these envi-
ronmental benefits are also highly reliant on the reference pro-
cesses. As the main contributor to the environmental impact is
the electricity source, the type of electricity supply is essential
(Sternberg and Bardow, 2016). The use of electricity mainly gen-
erated from fossil resources leads to a higher environmental im-
pact of PtG systems compared to fossil reference processes, and is
therefore not recommended (Reiter and Lindorfer, 2015). Further-
more, PtG demonstrates the highest reduction of GHG emission if
biogenic CO2 sources are used for methanation (Zhang et al., 2017).
It is also noticed that amine-based post-combustion technologies
have strong dominance to capture CO2 from flue gas stream, re-
gardless the source of CO2 (except for direct air capture), which
is related to the fact that these technologies present the highest
level of maturity (Zhang et al., 2020). Hoppe et al. (2018) also ar-
gue that better environmental performance are obtained when the
CO2 content in the flue gas is higher, as the energy demand for CO2
recovery is lower. Additionally, heat management, especially heat
integration between the different units involved in PtG, appears
to be a key point to lower the overall energy consumption, influ-
encing the environmental impacts of process chains, and improve
economic efficiency of a PtG plant (Thema et al., 2019). Regarding
some methodological aspects, the literature review (see SI.1) also
shows that construction, manufacturing and decommissioning of
the PtG plant are rarely considered within the system boundaries,
which may have critical contribution when the associated impact
of electricity is low (Zhang et al., 2017).
In the present work, the investigated PtG technology chain con-
sists of several units, an electrolysis to produce renewable hydro-
gen, an advanced amine-based CO2 capture process, a CO2 metha-
nation process, a SNG upgrading unit, as well as an optimized
heat management system allowing to recover and use waste heat.
Most of the published research on PtG and SNG production focuses
on plant design and techno-economic aspects, and addresses envi-
ronmental perspectives separately. Conventional amine-based (e.g.,
MEA) absorption-regeneration systems are often considered, and
very few papers include the SNG upgrading unit (see SI.1).
To this extent, this work aims to assess and compare life cy-
cle emissions of a complete and integrated PtG technology chain
to the natural gas production, using a hybrid LCA approach. The
contributions to the environmental impacts of the PtG technology
chain over the life cycle are analysed allowing to identify the main
hot spots to reduce environmental impacts, applying a process-
based attributional LCA. LCA is a well-established methodology
which allows evaluating the environmental impacts of a product
over its whole life, from raw material extraction, production, use,
to end-of-life treatment, including recycling and final disposal, and
identifying the main sources of pollution. The LCA study is then
hybridized by filling data gaps with Economic Input-Output data
R. Chauvy, L. Dubois, D. Thomas et al.
Fig. 1. Framework to evaluate the life cycle emissions combining conventional LCA and EIO-LCA.
to quantify the emissions related to the construction, manufactur-
ing and decommissioning of the PtG plant (EIO-LCA), maintaining
completeness of the system under study.
This integrated PtG technology chain is thus investigated
through process modelling, using the AspenTech’s software. Based
on the modelling results, an economic evaluation was carried out
to investigate the capital investment. The results are used to evalu-
ate the environmental impacts of the construction and decommis-
sioning based on the EIO-LCA, avoiding then the underestimation
of related impacts. The techno-economic models are thus used to
develop the life cycle inventory in order to perform the environ-
mental assessment considering several impacts categories, such as
climate change, fossil resource scarcity, and water use. Both sub-
division and system expansion via substitution approaches are un-
dertaken to quantify the environmental impacts of the suggested
PtG system. Finally, an uncertainty assessment and a sensitivity
analysis are carried out to strengthen the robustness of the results.
2. Materials and methods
In this paper, life cycle emissions are assessed applying a hybrid
approach (Crawford et al., 2018). It combines process-based attri-
butional LCA for the evaluation of emissions occurring during the
CO2 capture and conversion processes, and the Economic Input-
Output LCA (EIO-LCA) approach to assess the environmental im-
pacts due to the construction and decommissioning of the infras-
tructure (see Fig. 1). LCA, conducted according to the framework
outlined by ISO 14040:2006 (International Organization for Stan-
dardisation, 2006), is performed using SimaPro v9 as LCA software,
coupled with the EcoInvent database v3 for the background life cy-
cle inventory and life cycle impact assessment analyses, together
with simulation data results, obtained from previous process mod-
elling using the AspenTech’s software (Chauvy et al., 2020). In line
with the ISO guidelines, LCA consists of four phases, including goal
and scope definition, inventory analysis, impact assessment and re-
sults interpretation.
2.1. Goal and scope definition
This study is built on a case study conducted by
Chauvy et al. (2020), which proposed the techno-economic
investigation of an integrated PtG system. The main objective
is to assess the environmental impact of PtG system generated
during the life cycle stages of the production of SNG. The life cycle
impacts are compared with fossil reference systems.
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Sustainable Production and Consumption 30 (2022) 301–315
The proposed PtG system is dimensioned to use large-scale 90-
MW multi-electrolysers operating with wind-based electricity to
generate 40 ton per day of renewable H2 . It is assumed that the
use of this electricity does not compete with utilization in applica-
tions leading to lower net CO2 emissions. The system enables the
synthesis of H2 and CO2 to SNG (so-called Sabatier reaction). The
source of CO2 is coming from the flue gas generated by a conven-
tional cement plant equipped with best available technologies. The
content of NOx and SOx in the flue is assumed to be reduced be-
yond the permitted emission limits, to limit solvent degradation
in the subsequent CO2 capture unit (Voldsund et al., 2019). 30 0 0
tons of clinker per day are produced, corresponding to a total flow
rate of 250,0 0 0 m³/h at 1.20 bar and 40 °C, after efficient desulfur-
ization, denitrification, dedusting and cooling. With a CO2 content
of 20 mol.%, it generates 2475 ton of CO2 per day (Meunier et al.,
2020). Based on a H2 /CO2 stoichiometric ratio of 4, about 10% of
the cement plant flue gas is treated assuming a CO2 capture ra-
tio set to 90%, representing a CO2 production of about 219 ton per
day. In many cases, the gas stream leaving a catalytic methanation
reactor does not meet the quality specifications of the natural gas
grid (Schildhauer and Biollaz, 2016). The produced raw gas is then
upgraded. The final composition of the produced SNG is 92.9 mol.%
methane, together with 3.7 mol.% CO2 , 3.4 mol.% H2 , and traces of
CO and water, which is compatible with the existing natural gas
pipeline infrastructures (Fendt et al., 2016). Finally, SNG is then fed
into a 35–100 bar pressure gas pipeline, for which the gas pres-
sure at the PtG plant is enough so that no further compression is
required.
In the underlying investigations, a cradle-to-gate LCA is consid-
ered. The system boundary includes therefore (i) the production of
H2 and O2 through wind-based water electrolysis; (ii) the CO2 cap-
ture unit to separate the CO2 from the other components present
in the cement plant flue gas; (iii) the methanation unit to pro-
duce Raw-SNG from CO2 and H2 ; and (iv) the SNG upgrading unit.
Fig. 2 shows the framework for estimating the life cycle parame-
ters of the alternative SNG production. All processes are considered
on-site thus neglecting the environmental impacts and energy re-
quirements of transports and storage. Oxygen and excess heat are
co-products. Oxygen can be compressed to be reused in industrial
processes, such as in chemical industry, medical applications, or
wastewater treatment, while heat can be recycled to be reused on-
site or it can be injected into a district heating grid (Eveloy and
Gebreegziabher, 2018).
The process inputs for the PtG plant sizing are obtained from
the detailed model discussed in Chauvy et al. (2020). The produc-
tion of one GJ using the lower heating value (LHV) is considered
R. Chauvy, L. Dubois, D. Thomas et al. Sustainable Production and Consumption 30 (2022) 301–315

Fig. 2. Framework for estimating the life cycle parameters of SNG production.

Fig. 3. Technological metrics normalized to the production of one-GJ (LHV-basis).

as functional unit. CO2 -based SNG is benchmarked to one GJ (LHV)
fossil-based natural gas (NG) in Germany. To make the results com-
parable, they are harmonized using their methane content based
on the lower heating value. As the downstream processes are iden-
tical in the comparison of PtG process to conventional NG pro-
cess, the use and end-of-life phases of SNG can be neglected for
the present scope (Zimmermann et al., 2020). The technological
metrics of the integrated process, normalized therefore to the pro-
duction of one-GJ, are displayed in Fig. 3. It can be noted from
Fig. 3 that as the excess heat released by the methanation is also
used for producing electricity, no supplementary electricity needs
to be supplied to this unit, and the need for external electricity is
also reduced for the CO2 capture unit.
This study applies both subdivision and system expansion via
substitution for joint cement, captured CO2 production and O2 co-
production in case of PtG. In order to address the perspective
of the PtG system, cement plant, and oxygen unit operators, the
multi-functional process is divided into separate production activi-
ties (subdivision approach), so that the environmental burdens as-
sociated with the specific products (i.e., cement, SNG, and oxygen)
can be quantified. In this case, CO2, considered as a waste stream,
does not carry environmental credits.
To include the substitution and displacement of alternative
products in the market, the system boundary is expanded. To this
extent, the total environmental impacts of the complete and ex-
panded system, including cement production with CO2 capture and

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R. Chauvy, L. Dubois, D. Thomas et al.
PtG system, are evaluated and compared with the conventional
production of equivalent amounts of cement without CO2 capture,
the conventional production of oxygen from cryogenic air separa-
tion unit (ASU), as well as the conventional production and use of
natural gas when PtG is not in place, as recommended by von der
Assen et al. (2013).
Particularly, the common method to evaluate the climate
change impact (CC), only valid if CO2 is available from point
sources, is to credit the CO2 used by the PtG process, but also bur-
den it with GHG emissions due to CO2 capture and conditioning
impacts (Zimmermann et al., 2020). In other words, all CO2 be-
ing used in the CO2 -based SNG has a negative GHG emission (of
−1 kgCO2 -eq per kgCO2 used), but also a positive GHG emission
mainly related to the energy demand to capture this amount of
CO2 and auxiliary equipment. It is then assumed that the provi-
sion of 1 kgCO2 generates a reduction of 1 kgCO2 emissions only
in the case where no additional energy is required and no indirect
emissions occur; which is very rare, and only possible with some
specific processes (von der Assen et al., 2014), such as mineral car-
bonation using flue gas without preliminary CO2 capture (He et al.,
2020).
2.2. Hybrid inventory analysis
The Life cycle inventory (LCI) phase provides the balance of
resources and emissions upon which the assessment is calcu-
lated. The data include both background data from the EcoInvent
database v3 (Althaus et al., 2007), and foreground data obtained
from process modelling based on previous work (Chauvy et al.,
2020).
Regarding the energy consumption, the data include upstream
processes, such as extraction of resources and raw materials, fuel
processing, and transport, as well as downstream processes, op-
eration, transmission, and distribution. The German grid supply is
chosen for the electricity supply of the different units. In terms of
materials use, the infrastructure construction and decommission-
ing of the PtG plant are considered in this study based on the EIO-
LCA approach. The use of EIO data mainly leads to fill data gaps
in the analysis and reduce errors, providing more complete infor-
mation when compiling the inventory. It is worth noting that this
approach combining process and EIO data is often referred as the
Tiered hybrid analysis (Crawford et al., 2018).
2.2.1. Economic input-output LCA (EIO-LCA)
Based on the economic input-output theory developed by
Leontief (1970), the EIO-LCA model was built by the Carnegie Mel-
lon University (Hendrickson et al., 1998; 2006). While process-
based LCA models list the inputs and outputs, taking a “bottom-up”
approach, the EIO-LCA model takes “top-down” approaches, link-
ing monetary values of the industry sector to their environmen-
tal inputs/outputs, to estimate the total emissions throughout the
supply chain (Azari, 2019). Using both models can therefore com-
prehensively capture the full range of processes within the econ-
omy (Sherwood et al., 2017). This approach represents the inven-
tory stage of the LCA.
The relation between a sector’s output and its inputs is pre-
sented in a matrix constituted by technical coefficients, A. The out-
put needed from each sector X to satisfy an increase in demand Y ,
is expressed by Eq. (1):
X = (I − A )−1Y (1)
where (I − A )−1
is the Leontief Inverse, and I the identity matrix.
More details regarding the matrix definition and calculation are
available in the Supporting Information (see SI.2).
The economic data are linked with resources use and environ-
mental impact categories. Considering B the total vector of the dif-
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Sustainable Production and Consumption 30 (2022) 301–315
ferent impacts, b a matrix of environmental impacts per mone-
tary unit of each sector’s output, the environmental impacts can
be computed by Eq. (2):
B = bX = b(I − A )−1Y (2)
Data are categorized by industry sectors using the Statistical Clas-
sification of Economic Activities in the European Community, com-
monly referred to as NACE (acronym defined from the French term
"nomenclature statistique des activités économiques dans la Com-
munauté européenne"), available in the Reference and manage-
ment of nomenclatures (RAMON) from (Eurostat 2008). They are
founded on numerous sources aggregated by economic sector.
As discussed by Crawford et al. (2018), and illustrated by
Giordano et al. (2018), the EIO-LCA allows to prevent the under-
estimation of related impacts regarding the construction and de-
commissioning system, mainly coming from the lack of data on
materials quantities. Specifically, to account the emissions related
to the construction and decommissioning stages, the emissions per
unit cost are multiplied by the cost of equipment referred to the
functional unit, as previously described.
Economic analysis of the PtG process is carried out using the
factorial method, described in detail by Towler and Sinnott (2013).
The purchased equipment cost (delivered) (P EC) is evaluated, us-
ing the ICARUSTM suite of tools licensed by Aspen Technology Inc.,
based on the equipment sizes and mass and energy balances from
process modelling. Using the factorial method based on the P EC,
the fixed capital investment (F CI) is expressed as the sum of di-
rect and indirect costs. Direct costs include the total cost of de-
signing, constructing, and installing the plant, as well as the asso-
ciated modifications needed to prepare the plant site (Towler and
Sinnott, 2013). These factors do not take into account land pur-
chase and preparation, long pipelines or belt conveyors, work-
shops, warehouse, or office buildings. The indirect costs comprise
costs associated with offsite developments that require the plant
to run, as well as design and engineering costs, and contingency
charges. The typical factors used in this study are presented in the
Supporting Information (see SI.3.1). Costs related to materials re-
placements are evaluated to consider the emissions throughout the
assumed system lifetime of 20 years. The decommissioning costs
are taken into account and estimated as 5% of F CI (Giordano et al.,
2018). All costs are adjusted to the year 2018, using the Chemical
Engineering Plant Cost Index (Shirmohammadi et al., 2021). The
value of CEPCI index for 2018 is equal to 603.1, derived from the
magazine of Chemical Engineering (Jenkins S., 2019). The costs are
estimated with a nominal accuracy of ±30%.
Finally, capital costs for the PtG plant are allocated to different
economy sectors of the multiregional sectorial cash flow EXIOBASE
3 database to evaluate the environmental impacts (Stadler et al.,
2018). The nomenclature of sectors in EXIOBASE 3 relies on the
NACE, with further disaggregation regarding some products, such
as energy, waste treatment, or agricultural and food products.
2.2.2. Hydrogen and oxygen co-production
Regarding the hydrogen supply, water electrolysis using power
from wind turbines is selected as it demonstrates the lowest im-
pact on climate change (von der Assen et al., 2014; Matzen and
Demirel, 2016). Electrolysis using wind emits 0.97 kgCO2 -eq per
kg of H2 , compared with solar electrolysis (2.4 kgCO2 -eq per
kg H2 ) and conventional H2 production in a steam reforming
process with natural gas that emits 11.9 kgCO2 -eq per kg H2
(Cetinkaya et al., 2012). PEM electrolyser is considered, producing
hydrogen at 30 bar with a high purity level of 99.99 vol.%. The op-
erating temperature is typically low (50–100 °C) (Schmidt et al.,
2017). The specific electrical power is estimated at 55.6 kWh per
kg H2 . A production cost of 4 to 5 € per kg H2 , and a total sys-
tem cost, including energy supply and installation costs, of 1200
R. Chauvy, L. Dubois, D. Thomas et al.
Fig. 4. CO2 capture unit flow sheet considering the RVC+ICA+WW configuration.
€ per kW with an operation lifetime of 20 years are considered
(Becker et al., 2018). The H2 production is intended to be ge-
ographically co-located with the electricity from renewable en-
ergy supplies and the source of CO2 , avoiding additional units
and transport needs. LCA aggregated data are used for H2 produc-
tion, based on the comprehensive works of Ghandehariun and Ku-
mar (2016) and Bareiß et al. (2019); the latter providing a detailed
inventory for a PEM water electrolyser system; see the Supporting
Information SI.4.1. Finally, conventional tap water, once treated, is
considered as source for the electrolysis.
Oxygen generated from cryogenic air separation unit is con-
sidered as a benchmark for the co-production of oxygen from
the electrolysis. The environmental impacts of air separation units
are mainly associated with the demand for electricity. The ac-
tual power consumption to produce a 95% purity oxygen (medi-
cal grade oxygen) varies between 184 and 260 kWh per ton O2 ,
but the energy requirement increases beyond a purity level of 95%
(Khallaghi et al., 2020). The conventional ASU process considered
in this work and presented in the Supporting Information (see
SI.4.2), has a power consumption of 290 kWh per ton O2 , as a
higher purity level (approximately 99%) is required for reasons of
system consistency (i.e., the oxygen produced by the ASU must
have the same purity level as the oxygen purity coming from the
electrolyser).
2.2.3. CO2 capture unit
The CO2 capture process was modelled with Aspen Plus, based
on a transposition of the works of Dubois and Thomas (2018a;
2018b), and Chauvy et al. (2020; 2021) performed with Aspen
HYSYS. The CO2 capture plant uses as basis a standard absorber-
stripper configuration (Rochelle, 2009; 2016). It is completed with
a rich vapour compression (RVC) process associated with an inter-
cooled absorber (ICA) and two water-wash operations on both ab-
sorber (WWabs ) and stripper (WWstrip ) for gas polishing, and the
use of a MDEA 10 wt.% + PZ 30 wt.% aqueous blend as the solvent,
as displayed in Fig. 4. The main purpose of these process modifi-
cations is to reduce the energy penalty of the capture process, as
discussed by Shavalieva et al. (2021).
The CO2 -containing feed stream (namely gas to treat) from the
cement plant enters the absorber at a pressure of 1.2 bar. The gas
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Sustainable Production and Consumption 30 (2022) 301–315
contacts the solvent in the counter-current packed absorber, after
which the treated exhaust gas leaves the top of the absorption col-
umn along with some traces of solvent. The rich solvent is pumped
from the bottom of the absorber and enters the internal heat ex-
changer to be preheated by the regenerated lean solvent, before
entering the RVC unit. The RVC configuration, applied to the rich
solution, uses a heat pump effect. As a result of the solvent flash-
ing, the produced gas, mainly composed of CO2 and H2 O, is com-
pressed to the regeneration pressure (5 bar) and sent to the strip-
ping column to reduce the steam requirement at the reboiler. Con-
currently, a second heat exchanger cools down the vapour coming
from the compressor to the same temperature level at the bottom
of the stripper column (140 °C). The gas flow at the top of the
stripper enters a condenser unit where it is cooled down in order
to generate a CO2 flow at 98 mol.% purity. The concentrated CO2
flow is then sent to the CO2 conversion unit, where it is first com-
pressed to reach the pressure required for the conversion.
Table 1 summarizes the techno-economic performance parame-
ters needed to assess life cycle emissions of the CO2 capture unit.
Due to lack of data, the impacts of MDEA and PZ productions are
modelled as those of MEA, since LCI data for MEA can be regarded
as proxy for amine-based solvents (Fernández-Dacosta et al., 2018).
2.2.4. CO2 conversion unit including SNG upgrading
The CO2 conversion unit was modelled with Aspen Plus. The
CO2 captured from the flue gas stream is then fed together with
renewable hydrogen from the PEM electrolysis in the conversion
unit, considering the stoichiometric ratio H2 /CO2 of 4. The process
comprises four multi-tubular adiabatic reactors, in between which
the reaction mixture is cooled down to 350 °C to obtain a high
CO2 conversion rate. The working pressure is 10 bar. A fraction
of the product gas leaving the first reactor is recycled and mixed
with the feed gas to lower the temperature in order to avoid cata-
lyst sintering. A large portion of the reaction water formed is con-
densed and separated from the product gas leaving the fourth re-
actor. The produced Raw-SNG, containing methane (71.44 mol.%),
CO2 (4.15 mol.%), H2 (23.64 mol.%) and remaining water vapour, is
then upgraded considering a membrane system. It includes both
a dehydration membrane and a H2 removal membrane to comply
with the specification of the existing natural gas network, mainly
R. Chauvy, L. Dubois, D. Thomas et al. Sustainable Production and Consumption 30 (2022) 301–315

Fig. 5. CO2 conversion unit flow sheet including the upgrading section.

Table 1
Performance specifications of the CO2 capture unit Based on Chauvy et al. (2020).

Parameters Values Units

Separation performance
Capture ratio 90 %
CO2 output 219 t per day
CO2 purity 98 mol.%

Material requirement
Water 257.51 kg/tCO2
Aqueous blend of amines (solvent) 1.44 kg/tCO2

Energy requirement
Reboiler duty 2.28 GJ/tCO2
Compressor (RVC configuration) 0.91 MWe
Pumps 0.04 MWe
Coolers (incl. condenser, lean solution, absorber, water-wash) - 4.98 MWth

Air emissions (treated exhaust gas)

Flow rate 3065 kg/tCO2
Compositions
−1
H2 O 1.24 10 wt.%
CO2 3.57 10−2 wt.%
N2 7.28 10−1 wt.%
O2 1.10 10−1 wt.%
CO 1.50 10−3 wt.%
SO2 2.66 10−7 wt.%
NO2 2.79 10−9 wt.%
NO 5.71 10−7 wt.%
Solvent traces 1.00 10−16 wt.%

Costs
1. Purchased equipment cost (delivered) (PEC) 7.18 M€
Columns (absorber/stripper) 17.27 % PEC
Compressors 46.80 % PEC
Heat Exchangers (heaters/coolers) 33.43 % PEC
Flash tanks 2.50 % PEC
2. Total direct cost 22.97 M€
3. Total indirect cost 5.02 M€
4. Fixed capital investment (F CI) 27.99 M€

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Table 2 mation (see SI.3.2). The German region is used in the modelling of
Performance specifications of the CO2 conversion unit including the upgrading
the impacts of the infrastructure.
section Based on Chauvy et al. (2020).

Parameters Values Units 2.2.6. Cement plant

Material requirement A representative cement plant is considered, as described by
CO2 2.53 t/t SNG Voldsund et al. (2019) and Gardarsdottir et al. (2019). The ther-
Renewable H2 (99.9 vol.%) 0.46 t/t SNG mal energy input for this plant includes up to 16% of alternative
Catalyst Ni/MgAl2 O4 (Ni 15 wt.%) 4.07 10−4 t/t SNG
fuel and biomass, while the other 84% are coming from coal, natu-
Energy requirement ral gas, refuse derived fuel, solid and liquid hazardous wastes, an-
CO2 Compressor 0.14 MWe imal meal and other carbon-based fuels (ECRA, CSI, 2017). For the
Recycle compressors 0.19 MWe life cycle inventory analysis for the cement plant, LCA aggregated
Membrane compressor 0.36 MWe
data are taken from the EcoInvent database, which were adapted
SNG compressor 0.25 MWe
Pumps 0.07 MWe to consider the German mix and conditions of the German loca-
Turbine - 1.06 MWe tion as close as possible, as energy consumption and alternative
Output fuels are very context specific.
SNG production 87 t per day
SNG purity
CH4 92.93 mol.%
2.3. Impact assessment
CO2 3.69 mol.%
H2 3.38 mol.% The inventories of the PtG system, including emissions and
CO Traces mol.% resource consumption, are then translated into impact indicator
Water Traces mol.%
scores. There are currently a large variety of impact assessment
Oxygen production 3.70 t/t SNG
Water production 2.16 t/t SNG methods. The most updated version of the standard practice Life
Costs cycle impact assessment (LCIA) methodology the ReCiPe Midpoint
1. Purchased equipment cost (delivered) (PEC) 20.96 M€ methods is chosen in this study (Huijbregts et al., 2016), as it sur-
Reactor 16.70 % PEC passes some of the weaknesses highlighted by the review from the
Compressors 29.53 % PEC
Turbine 2.15 % PEC
JRC report (Bareiß et al., 2019). The hierarchical perspective is used,
Heat Exchangers (heaters/coolers) 45.32 % PEC as it is based on the most common policy principles in terms of
Membrane 5.87 % PEC time-frame and other issues. The LCA is conducted on six relevant
Flash tanks 0.43 % PEC impacts indicators, reflecting the goal and scope of the study: cli-
2. Total direct cost 67.07 M€
mate change (CC), fossil resource scarcity (FS), terrestrial acidifi-
3. Total indirect cost 14.67 M€
4. Fixed capital investment (F CI) 81.75 M€ cation (TA), freshwater eutrophication (FE), water use (WU), and
mineral resource scarcity (MS). More details can be found in the
Supporting Information (see SI.4.3). It is worth noting that the en-
vironmental impacts of construction and decommissioning are ag-
the water dew point requirements of the pipelines, corrosion con-
gregated under the category ‘infrastructure’ in the following.
trol and prevention of solid hydrocarbon/water hydrates’ formation
(see Fig. 5) (Chauvy et al., 2020). Subsequently, the SNG product
2.4. Uncertainty and sensitivity analysis
gas is sent to the compression unit for final supply to the natural
gas network.
In a real application, insufficient information of reactions and
The methanation of CO2 being strongly exothermic processes,
kinetic models related to the catalyst, as well as lack of knowledge
releasing 165 kJ of heat/mol, heat management during the reaction
of the components’ physical properties, can be sources of uncer-
is therefore a crucial aspect. Heat integrations between the differ-
tainty (Sharifian et al., 2019). The uncertainty of the proposed PtG
ent units are possible. To this extent, heat recovery is performed
process related to the environmental impacts depends mainly on
to improve the energy efficiency and optimize the use of utilities,
the quality of the techno-economic parameters determined from
lowering thus the costs (Chauvy et al., 2020). The excess heat is
the process modelling, as well as and the quality of the available
used to generate steam which is then expanded in a gas turbine,
data from the database and the literature.
and the mechanical power recovered by this solution corresponds
Uncertainties are identified in this study using predefined pedi-
to the total work required for the compressors in the CO2 conver-
gree analysis from Fernández-Dacosta et al. (2017), detailed as
sion unit including the upgrading section.
well by (van der Spek et al., 2016; 2019) to evaluate the weak-
The performance parameters necessary to assess life cycle emis-
nesses that can arise from the data source, process modelling, and
sions of the CO2 conversion unit, including the upgrading section,
methodologies. These predefined Pedigree matrices are detailed in
are summarized in Table 2.
the Supporting Information (see SI.5). This approach is designed to
The catalyst considered for the CO2 methanation is modelled
provide an indication of the quality of data, as well as the iden-
using the data available for the manufacturing of chemicals re-
tification of poor data quality. The quality is thus appreciated de-
ported in EcoInvent database (Althaus et al., 2007). The spent cat-
pending on how well the data respond to the definition of the pre-
alyst, its recovery and further reuse are not included in the system
defined pedigree indicators. The assigned quality ratings are pro-
boundary. As a result, no emission or credit are accounted for the
cessed to convert them into numerical score and generate data
spent catalyst.
quality indicator (DQI). The following procedure is then used to
characterize data quality uncertainty: 1) build the pedigree ma-
2.2.5. Construction and decommissioning trix for each unit of the PtG plant; 2) build the intermediate DQI
The economic inputs required to use the EXIOBASE 3 database for each unit, performed by summing up the scores of the data
are computed based on the F CI for the different plant processes. quality parameters related to a specific indicator and dividing this
The F CI is allocated to different economy sectors. Table 3 displays figure by the number of data quality parameters, assuming equal
the fractional capital cost distribution by sector for the CO2 capture weights to each parameter; 3) build the final aggregated qualitative
and conversion units. The items and corresponding I-O categories DQI score, i.e. the average of the indicator scores of equal weight-
using the NACE code sectors are presented in the Supporting Infor- ing (Wrisberg et al., 1997). It is worth mentioning that applying

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Table 3
Fractional cost distribution by sector for the PtG process plant infrastructure (excluding
renewable H2 production).

Sector Fractional cost distribution

Manufacture of machinery and equipment 0.51

Manufacture of electrical machinery and apparatus 0.13
Construction 0.22
Intermediation 0.02
Other business activities 0.07
Decommissioning 0.05

an equal weighting for each of the data quality indicators is de-

batable, but initially implicit when the Pedigree method is used
(Edelen and Ingwersen, 2018). Using a weight for DQI to reflect
the inherent characteristics of the model is out of scope of this
study. The data directly extracted from the EcoInvent database are
not assessed as they are considered reliable and globally accepted
(Khoo et al., 2018).
Additionally, the LCA results may lead to incorrect deci-
sions if apparent differences between the two alternatives turn
out statistically insignificant after inclusion of all uncertainties,
as discussed by Huijbregts et al. (2003), and more recently
emphasied by Mendoza Beltran et al. (2018). To this extent,
Jolliet et al. (2016) present some generally accepted default rules
that can be used to take into account uncertainty, based on expert
judgement, especially in the case of a comparative study, where it
is rather difficult to know when the difference between two sce-
narios is significant. Thus, when comparing scenarios, any differ-
ence less than 10% can be considered insignificant at first glance
for energy and CO2 related impacts. For respiratory inorganic ef-
fects, acidification and eutrophication, the difference between two
scenarios should typically be greater than 30% to be evaluated as
significant. For toxicity characterization, the calculation of impacts
often involves more uncertainty, requiring a difference of at least
one to two orders of magnitude between scenarios to be consid-
ered significant (Jolliet et al., 2016). These general rules are there-
fore used to strengthen the LCA conclusions derived from this
present paper.
Complementary to the uncertainty analysis, a sensitivity anal-
ysis is also performed mainly to show the variances of some pa-
rameters on the LCA results. It is performed by changing one in- Fig. 6. Contribution analysis of the main process units (upgrading unit included in
put parameter at the time, considering a minimum and maxi- the CO2 conversion unit).
mum value around the base value with all other input parame-
ters fixed within reasonable technical, physical, or economic con-
straints (Zimmermann et al. (2020) and references herein). Typical
variances are assumed according to the ones reported in literature also denotes a high share, representing for instance 91% of the FE
(Fernández-Dacosta et al., 2017; Schakel et al., 2017). Variances of impact’s contribution.
± 10% are considered for feedstock consumption, ± 25% for energy Fig. 7 shows the breakdown of the environmental contribution
consumption, and ± 30% for the capital investment which is used to the impact categories of the integrated CO2 capture and con-
for the evaluation of the construction and decommissioning envi- version process. It is observed that no external heat demand is
ronmental impacts. In particular, the variance of the capital invest- required due to process-to-process heat integrations between the
ment is in accordance with the AACE international recommended CO2 capture and CO2 methanation units, leading to environmen-
practice related to cost estimation (Christensen and Dysert, 2005). tal benefits compared to a scenario where these units are not in-
tegrated. Except for the MS indicator (reduction of less than 1%),
these are positive on all the environmental impacts, which show
a global reduction of 4% to 75% according to the considered crite-
3. Results and discussion rion. Particularly, the environmental impacts on CC and FS are re-
duced by 39% and 75%, respectively. The remaining treated exhaust
3.1. LCA results gas from the absorber’s top of the CO2 capture unit contributes to
35% of TA and 30% of CC. The infrastructure, including construction
Fig. 6 depicts the contribution analysis, which determines the and decommissioning, accounts for 50% of the mineral resource
contribution that the main process units of the PtG plant make to- scarcity. Amongst all the items considered in the LCI, the analy-
wards the overall environmental impacts. Despite the fact that re- sis of the environmental burdens along the life cycle also shows
newable electricity is used, the contribution made by H2 produc- that a significant fraction of the impacts is generated during the
tion compared to the other units is dominant. It has the highest production of renewable H2 . Additional LCA details are displayed
share in WU, CC, and TA impact categories. The CO2 capture unit in the Supporting information (see SI.4.4).

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Fig. 7. Environmental contribution to the impact categories of the integrated CO2 capture and conversion process including the upgrading unit.

Table 4
LCA Characterization results for both the conventional NG and the CO2 -based SNG productions applying the sub-
division approach.

Impact category Unit Conventional NG production CO2 -based SNG production

Fossil resource scarcity (FS) kg oil eq 27.75 1.20

Mineral resource scarcity (MS) kg Cu eq 1.73 10−2 1.82
Water use (WU) m³ 1.56 10−2 0.37
Terrestrial acidification (TA) kg SO2 eq 3.98 10−2 0.12
Freshwater eutrophication (FE) kg P eq 5.53 10−4 2.58 10−3
Climate change (CC) kg CO2 eq 13.70 18.28

Fig. 8. Comparative LCA environmental impact results in relative% of impact for both the conventional NG and the CO2 -based SNG productions applying the subdivision
approach.

In case of subdivision approach, Table 4 presents the compari-
son between the environmental impacts of the CO2 -based SNG to-
gether with conventional NG as a benchmark. Furthermore, these
results have been represented in Fig. 8 to illustrate their rela-
tive environmental impacts. The impacts of NG are extracted from
the EcoInvent database (Swiss Centre for Life Cycle Inventories).
The impacts of the CO2 -based process are higher than the con-
ventional NG production, mainly due to the additional purification
steps and related infrastructures, except for the FS, that is drasti-
cally reduced. Higher water use is expected since that is the main
source of hydrogen for electrolysis, while natural gas production
requires limited water use. PtG mineral resource scarcity is more
than a hundred times higher than natural gas, as the share for the
construction of the PtG plant, including a complex heat integration
network for heat recovery and electricity production, is only allo-
cated to the PtG plant. Regarding the CC indicator, the CO2 used
by the PtG process is burdened with GHG emissions due to CO2
capture and conditioning impacts, which thus only takes into ac-
count the positive emissions mainly due to energy consumption.
Care should be then taken when comparing the impacts of the PtG
system with the fossil NG production applying the subdivision ap-
proach, since subdivision does not reflect the reduced emissions of
cement production with CO2 capture.
For a more general perspective, the system needs to be ex-
panded to include both PtG system, oxygen, and cement produc-
tions. Applying the system expansion strategy where the CO2 used
by the PtG process is also credited, Table 5 and Fig. 9 present the
environmental impacts of the integrated CO2 conversion process

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Table 5
LCA Characterization results of the integrated CO2 conversion process to SNG compared with the reference system ap-
plying the system expansion approach.
Impact category Unit
Fossil resource scarcity (FS) kg oil eq
Mineral resource scarcity (MS) kg Cu eq
Water use (WU) m³
Terrestrial acidification (TA) kg SO2 eq
Freshwater eutrophication (FE) kg P eq
Climate change (CC) kg CO2 eq
Fig. 9. Comparative LCA environmental impact results in relative% of impact of the integrated CO2 conversion process to SNG and the reference system applying the system
expansion approach.
to SNG compared with the reference system. The impacts on MS,
WU, and TA of the suggested alternative are still higher than the
conventional reference system, even though it should be pointed
out that uncertainty remains high, and the difference could still
mean that PtG and reference system have similar impacts. How-
ever, the impacts on fossil resource scarcity (FS) and freshwater
eutrophication (FE) are drastically reduced by over 70%. Regard-
ing the CC, the impacts reach 19.65 kgCO2 -eq per GJ for the in-
tegrated CO2 -based process in comparison to 82.17 kgCO2 -eq per
GJ for the reference system. The CO2 emissions of the CO2 -based
process are thus decreased by about 76% in comparison to the ref-
erence system, due to high energy recovery and integration from
the exothermic methanation reaction, as well as use of copro-
duced oxygen which leads to an environmental benefit receiving
a credit for the conventional production of oxygen by a cryogenic
ASU (as more detailed in a zoomed-in view of the CC impact in
Fig. 10).
In contrast to negative emission technologies, the use of CO2
captured from cement plants’ flue gas to produce SNG remains a
carbon positive system. However, the LCA results show that a sub-
stantial carbon reduction is achieved compared to the fossil-based
reference system, in which heat integration plays a crucial role. Cli-
mate change impact reduction requires a complex heat manage-
ment system to recover heat from the exothermic Sabatier reac-
tion. Moreover, it is most pronounced with the use of renewable
electricity for the generation of hydrogen. Its contribution to CC is
drastically lower compared with benchmarked NG, as the CC im-
pact is reduced by about 76%. Similarly, the fossil resource scarcity
is drastically reduced by over 80% due to both the heat integra-
tion allowing the use of waste heat from the methanation to sub-
sequent processes, and the substitution of natural gas by the CO2 -
based SNG.
Sustainable Production and Consumption 30 (2022) 301–315
Fossil-based reference system Integrated CO2 - based alternative
33.11 4.88
2.81 4.61
1.08 1.31
0.20 0.24
1.06 10−2 2.74 10−3
82.17 19.65
3.2. Uncertainty and sensitivity analysis
3.2.1. Uncertainty analysis
The different units are then systematically assessed using the
predefined Pedigree matrices (see Table SI.8 to Table SI.11 in the
Supporting Information SI.5.1). The Pedigree scores are then dis-
played in the Supporting Information SI.5.2, from Table SI.12 to Ta-
ble SI.15. The Pedigree matrix for the assessment of uncertainty in
process models and their sub models is presented in Table SI.12.
The assessment shows high scores, except for the SNG upgrading
section. Regarding the technical input data (see Table SI.13), the
input parameters have a high score for both the CO2 capture and
conversion units (methanation section) due to the expertise and
maturity of the processes; the empirical basis indicator demon-
strating the lowest score as they are based on modelled/derived
data and indirect measurements (no experimental work was per-
formed). Low uncertainty in reactions and kinetic models related
to the catalyst is assumed, as a commercial catalyst was used and
has been widely characterized (Chauvy et al., 2020). The SNG up-
grading section demonstrates the lowest scores mainly due to lim-
ited expertise and lower level of maturity of the implemented pro-
cess. The H2 production unit shows a higher level of uncertainty, as
it is only based on data publicly available, taking also into account
that current data are mostly available for stand-alone electrolysers
up to 10 MW. The Pedigree scores related to the economic input
data (capital investment) are presented in Table SI.14. Regarding
the CO2 capture and CO2 conversion units, the scores assigned are
the highest for the proxy, and relatively intermediate for the relia-
bility of the source and the completeness (equipment list), as only
the major units are included in the equipment list. Input economic
data for other parameters are almost complete. The uncertainty re-
lated to the H2 production is the highest, based on open literature
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Fig. 10. Comparison between the Climate Change impact (CC) of the integrated CO2 conversion process to SNG with the fossil-based reference system, applying the system
expansion approach.
Table 6
Data quality indicator scores.
Process model Technical input data
1. CO2 capture unit 3.38 3.13
a
2. CO2 conversion unit 2.56 2.40
3. H2 production 2.50 2.30
a
Including the upgrading section.
data that are not fully documented. Finally, Table SI.15 presents the
scores for the environmental LCI. LCI data result from process mod-
elling while the EcoInvent database is used to provide background
process LCI data. Thus, the CO2 capture and CO2 conversion units
demonstrate high scores. It is worth noting that proxy chemicals
were used to model the catalyst for the methanation process. Also,
infrastructures are modelled only from the EcoInvent database and
open data, which lower the scores. The system representativeness
denotes high scores. Finally, H2 production denotes the largest un-
certainties.
For the three main units constituting the PtG process chain (i.e.,
the CO2 capture unit, CO2 conversion unit, and H2 production),
the intermediate DQI scores are built with respect to the tech-
nical, economic, and environmental data, and the aggregated DQI
scores are then calculated. Results are presented in Table 6. The
aggregated DQI scores for both the CO2 capture unit, CO2 conver-
sion unit are quite high, 2.98 and 2.54, respectively, the DQI scores
ranging hypothetically from 0 to 4. H2 production denotes a lower
DQI (2.13), which is mainly related to the economic input data. In-
creasing in the quality of the economic input data will substan-
tially increase the overall quality of the inventory collection. The
uncertainties, given as percentage, range thus from 26% to 47%, for
the input data related to the CO2 capture unit and the H2 produc-
tion, respectively.
Additionally, when comparing the CO2 -based alternative with
the conventional production of NG (see Fig. 8), it can be noticed
that the difference is significant regarding all the impact cate-
gories when applying the subdivision approach, which indicates
that the environmental performances related to these impact cat-
egories are considered as significant and reliable, according to the
default rules given by Jolliet et al. and discussed in the previous
section (Jolliet et al., 2016). However, as the differences are less sig-
nificant when applying the system expansion approach (see Fig. 9),
especially for the MS, MU, and TA indicators, no strong conclusion
can be drawn regarding these impacts as this could still mean that
the suggested process and the reference system have similar im-
pacts (see Table 7).
Sustainable Production and Consumption 30 (2022) 301–315
Economic input data Environmental input data Aggregated DQI score
2.60 2.80 2.98
2.40 2.80 2.54
1.40 2.30 2.13
3.2.2. Sensitivity analysis
Finally, Fig. 11 shows the effect of modifying key parameters on
the different environmental impacts, in comparison with the base
case values as shown in Fig. 8 to 10. For most impacts, except FS
and FE, the feedstock consumption is the most sensitive parame-
ter with a 10% variance, followed by the energy consumption. A
variance of ± 30% on the capital investment does not lead to ma-
jor changes compared to the base case, except, not surprisingly, on
mineral resource scarcity MS.
3.3. Limitations of the analysis
Since a cradle-to-gate basis was chosen, all life cycle stages af-
ter the production of SNG were neglected, as gate-to-grave emis-
sions for CO2 -based and fossil-based production are identical. The
cradle-to-gate boundary is considered sufficient when comparing
the impact based on the lower heating value of the methane con-
tent. However, (Artz et al., 2018) indicate that if the function of the
produced SNG is to provide an energy carrier, for instance to oper-
ate a combustion process in a propulsion system, a cradle-to-grave
system should be considered and include the impacts related to
the combustion to provide the energy.
The accuracy of this study is limited by the data cut-offs used
as the H2 production is not modelled and only aggregated data are
used. The transportation is not included as all the processes are as-
sumed to be co-located, neglecting for instance necessary pipeline
infrastructure.
The study is also limited by data timeliness, as some of the data
used from database are several years out of date. Indeed, they are
not annually updated since environmental data can vary over time
due to changes in process efficiency and regulations, for example.
Thus, the level of uncertainty might arise since the reference pro-
cesses used today may be slightly more efficient than those used
in the models.
Additionally, some materials, i.e., solvent and catalysts, are
modelled using proxy and aggregated data, leading to additional
uncertainty. The degradation of the amine solvent is not modelled
but considered from aggregated data.
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Table 7
Relative differences between LCA results for both the subdivision and system expansion approaches

Impact Subdivision approach System expansion approach

࢞%a Decision result ࢞%b Decision result

FS 96 Significant difference (as > 10%) 86 Significant difference (as > 10%)
MS -99 -39 Non-significant difference
WU -96 -17 Non-significant difference
TA -66 Significant difference (as > 30%) -19 Non-significant difference (as < 30%)
FE -79 Significant difference (as > 30%) 74 Significant difference (as > 30%)
CC -25 Significant difference (as > 10%) 76 Significant difference (as > 10%)
1
[conv. NG production – CO2 -based alternative]. Positive values mean that the conventional natural gas
production has larger impacts than the CO2 -based synthetic natural gas, and vice versa.
2
[ref. system – integrated CO2 -based alternative]. Positive values mean that the reference system has
larger impacts than the integrated CO2 -based synthetic natural gas, and vice versa.

Fig. 11. Sensitivity analyses for the environmental impacts. Variances: Energy consumption ± 25%; feedstock consumption ± 10%; capital investment ± 30%.

Finally, the EIO-LCA models use as the basis for data only the
ones that are publicly available, which might be incomplete. Fur-
thermore, most data are categorized, and assumptions are required
to allocate these data to the most appropriate sector.
Overall, the uncertainty assessment, carried out based on the
Pedigree analysis, might be seen as subjective but transparent. It is
also complementary to the sensitivity analysis, which assessed the
value range of the parameters.
4. Conclusion
In the future, it is expected that significant expansion of renew-
able SNG capacities will arise, the key bottleneck being the avail-
ability of excess renewable energy. The suggested PtG process uses
surplus renewable power, from wind, for electrolysis to produce re-
newable hydrogen, which is then mixed with captured CO2 and
converted to SNG, before being fed into the existing NG pipeline
system once it meets the network specifications.
PtG systems, integrating thus all energy sectors, electricity, gas,
heat, and CO2 market in one synergic system, denote some envi-
ronmental potential in the context of CO2 mitigation and defos-
silization of the energy system. However, the environmental bene-
fits of CO2 -based SNG production must be proven. Thus, the inte-
grated techno-economic and environmental assessments based on
a hybrid LCA approach carried out in this study show that the PtG

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strategy reduces drastically fossil resource scarcity, compared to
as business-as-usual scenario. As opposed to subdivision approach,
applying system expansion via substitution also shows that the
PtG process with CO2 captured from cement plants’ flue gas re-
duces the overall GHG emissions (76% reduction). Heat integration
is also shown as necessary, otherwise the environmental perfor-
mance would deteriorate significantly.
As demonstrated in this study, the environmental impacts of
such system must be evaluated carefully on a life cycle basis. The
LCA shows that several environmental impacts of the suggested
PtG system are higher than conventional fossil natural gas. Also,
the strength of the knowledge base underlying the parameters
(i.e., input data) was assessed by the Pedigree analysis. It showed
that the uncertainty related to input parameters varied between
26 and 47%. Additionally, it was complemented by a sensitivity
analysis, assessing the value range of the parameters respectively
to the environmental indicators. It is worth noting that a techni-
cal table is provided in the Supporting Information (see SI.5) to
summarize the main information of the assessment, as advised by
Müller et al. (2020), and Zimmermann et al. (2020).
Finally, the evaluation of the environmental consequences of in-
troducing such PtG plants is of interest. A change-based (conse-
quential) modelling approach, estimating how flows to and from
the environment would be affected by different potential decisions,
should be then applied complementary to the present study.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared to
influence the work reported in this paper.
CRediT authorship contribution statement
Remi Chauvy: Conceptualization, Investigation, Methodology,
Writing – original draft, Writing – review & editing, Visualization.
Lionel Dubois: Validation, Writing – original draft, Writing – re-
view & editing. Diane Thomas: Writing – review & editing, Su-
pervision. Guy De Weireld: Validation, Writing – review & editing,
Supervision.
Acknowledgements
The European Cement Research Academy (ECRA) is gratefully
acknowledged by the authors for its technical and financial sup-
port. Remi Chauvy also thanks the support from the “NCKU 90 and
Beyond” Initiative, at the National Cheng Kung University (NCKU),
Taiwan.
Supplementary materials
Supplementary material associated with this article can be
found, in the online version, at doi:10.1016/j.spc.2021.12.004.
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