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Review
Limits to Paris compatibility
of CO2 capture and utilization
Kiane de Kleijne,1,* Steef V. Hanssen,1 Lester van Dinteren,1 Mark A.J. Huijbregts,1 Rosalie van Zelm,1 and Heleen de
Coninck1,2
1Department of Environmental Science, Radboud Institute for Biological and Environmental Sciences, Radboud University, P.O. Box 9010,

6500 GL Nijmegen, the Netherlands

2Technology, Innovation and Society Group, Department of Industrial Engineering and Innovation Sciences, Eindhoven University of

Technology, P.O. Box 513, 5600 MB Eindhoven, the Netherlands

*Correspondence: [email protected]
https://doi.org/10.1016/j.oneear.2022.01.006

SUMMARY

The Paris Agreement’s temperature goals require global CO2 emissions to halve by 2030 and reach net zero
by 2050. CO2 capture and utilization (CCU) technologies are considered promising to achieve the tempera-
ture goals. This paper investigates which CCU technologies—using atmospheric, biogenic, or fossil CO2—
are Paris compatible, based on life cycle emissions and technological maturity criteria. We systematically
gathered and harmonized CCU technology information for both criteria and found that CCU with technology
readiness levels (TRLs) of 6 or higher can be Paris compatible in 2030 for construction materials, enhanced oil
recovery, horticulture industry, and some chemicals. For 2050, considering all TRLs, we showed that only
products storing CO2 permanently or produced from only zero-emissions energy can be Paris compatible.
Our findings imply that research and policy should focus on accelerating development of CCU technologies
that may achieve (close to) zero net emissions, avoiding lock-in by CCU technologies with limited net emis-
sion reductions.

INTRODUCTION the general public because it is seen as part of the circular econ-
omy and a form of sustainable waste processing.15 It also ap-
In the 2015 Paris Agreement, almost all of the world’s nations peals to industry because CCU creates value from waste
committed to collectively hold ‘‘the increase in the global through CO2-based products16,17 while avoiding the storage
average temperature to well below 2
C above pre-industrial costs and concerns of geological storage of captured CO2,
levels and pursuing efforts to limit the temperature increase to known as carbon (dioxide) capture and storage (CCS).18
1.5
C above pre-industrial levels.’’2 This is also known as the However, the relevance of CCU in climate change mitigation is
Paris Agreement’s long-term temperature goal (LTTG). Climate questioned in the literature, based on several concerns: (1) CCU
change mitigation pathways with ‘‘no or low overshoot’’ of products may not always substantially reduce emissions
1.5
C3 are compatible with the Paris Agreement’s LTTG4–7 and compared with their conventional counterparts that do not
characterized by two key numbers: in 2030, global net anthropo- require the energy-intensive CO2 capture and conversion
genic carbon dioxide (CO2) emissions are halved compared with steps;19–22 (2) utilization of captured CO2, rather than permanent
2020 emissions, and in 2050, net CO2 emissions are zero.3 This geological storage, may result in a higher global warming effects
net zero CO2 target implies that no sector can be excluded from because utilized CO2 is typically re-emitted when the CCU prod-
deep emission reductions, that some technologies that still have uct is used or disposed of;16,19 (3) CCU may not be economically
significant emissions need to be phased out, and that a range of feasible because of the high financial costs associated with the
technologies is required to reach these emission reductions. energy-intensive CO2 capture and conversion steps;19,23 and
Carbon (dioxide) capture and utilization (CCU) is among these (4) CCU may form a political distraction from reducing CO2 emis-
options for potential emission reduction and is defined here as a sions, in particular when replacing CCS, because the scale at
process in which CO2 is technologically captured from CO2 point which CO2 could be utilized is limited compared with the scale
sources or ambient air and is subsequently used in or as a prod- at which CO2 could be stored geologically.21
uct. The reason why CCU could contribute to climate change The goal of this review is to provide conceptual clarity on what
mitigation is that it replaces fossil feedstocks, avoids upstream CCU is and what can be expected from different CCU technolog-
emissions, and temporarily keeps CO2 out of the atmosphere un- ical routes, in particular in reaching the Paris Agreement’s LTTG.
til re-emitted in the use phase of the product.8–13 CCU is distin- We first describe the different process steps and varieties of
guished from (permanent) carbon dioxide removal (CDR) of at- CCU technologies. Next, we present a framework to assess
mospheric CO2. The two terms only overlap when CO2 in a ‘‘Paris compatibility’’ in the context of CCU, using criteria based
CCU product has recently been removed from the atmosphere on technological maturity and greenhouse gas emissions reduc-
and is never re-emitted.14 CCU appeals to policymakers and tions. We then show the results of a systematic review of the

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A Sources of CO 2 B Capture of CO 2 C U liza on of CO 2 D CCU categories E Subs tute F CCU life me

CO2
days to years
terrestrial biomass
- direct use direct uses of CO2

atmospheric CO2
CO2 years to centuries

direct air capture enhanced hydrocarbon

recovery

- indirect carbona on months to centuries

- direct carbona on
CO2 - curing of cement mineral carbonates and
CO2 construc on materials

capture from point - thermochemical conversion

sources - electrochemical conversion
- photocataly c conversion
months to decades
- transesterifica on
- hydrothermal liquefac on
fuels and chemicals
biogenic fossil microalgae cul va on

Figure 1. Scope of CCU

This overview of CCU includes sources of CO2 (A), capture of CO2 (B), and examples of utilization processes (C) leading to different CCU products in four
categories (D), each with its substituted product in the conventional economy (E) and lifetime (F). CO2 capture via terrestrial biomass (top process under ‘‘capture
of CO2’’) is not included in the this paper’s CCU definition.

CCU literature following this framework. Last, we discuss our (E) Substitute. A CCU product is assumed to replace a prod-
findings and provide a research and policy outlook for climate uct in the conventional economy with the same chemical
change mitigation through CCU. For an overview of acronyms structure, composition, or characteristics, typically pro-
used, see Note S1. duced from fossil fuels and referred to as the substitute.24
(F) CCU lifetime. CO2 is, depending on the CCU product,
stored permanently or released into the atmosphere after
WHAT IS CCU? a certain period of time, called its lifetime, ranging from
days to centuries. For example, for fuels, the utilized
Scope of CCU CO2 is emitted into the air upon combustion. For the pur-
In line with our definition of CCU, we defined six key character- pose of this paper, we define storage as reaching perma-
istics of CCU (Figure 1): nency when it has a duration consistent with geological
timescales: centuries or longer.
(A) Sources of CO2. CO2 can originate from fossil fuel or
biomass combustion in power plants or industrial plants, Because we consider CCU for climate change mitigation, we
from industrial processes such as the calcination reaction exclude the use of CO2 from natural reservoirs because this
in cement production or biomass fermentation, or from source of CO2 does not reduce atmospheric CO2 concentra-
the atmosphere directly using direct air capture (DAC). tions.25 Our definition of CCU constrains CCU to processes
(B) Capture of CO2. CO2 is captured technologically on an in- that ‘‘technologically capture CO2,’’ including industrial and en-
dustrial scale by separating CO2 from a bulk gas stream gineered biological processes such as CO2 capture from flue
or the atmosphere using a solvent or sorbent, a mem- gases by microalgae, and excluding land-based CO2 sequestra-
brane, cryogenics, or industrially cultivated organisms, tion in biomass (in contrast to, for example, Detz and van der
such as microalgae, to photosynthesize CO2 into Zwaan13 and Hepburn et al.11). Use of biomass for energy and
biomass. materials is therefore also not in the scope of this review.
(C) Utilization of CO2. CO2 is used directly or indirectly by CCU is sometimes connected to CDR. CDR is a necessity to
converting CO2 into a range of products, often requiring limit warming to 1.5
C3 and has been defined as ‘‘anthropogenic
electricity, heat, and/or catalysts. activities removing CO2 from the atmosphere and durably stor-
(D) CCU categories. The resulting CCU products can be ing it in geological, terrestrial, or ocean reservoirs, or in prod-
categorized as direct uses, enhanced hydrocarbon re- ucts.’’14 CDR includes methods like bioenergy with CCS
covery (EHR), mineral carbonates and construction mate- (BECCS) and direct air CCS (DACCS).26 CCU can only be classi-
rials, and fuels and chemicals. fied as CDR, following the criteria formulated by Tanzer and

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Ramı́rez,27 when (1) physical CO2 is removed from atmosphere and condensation.33 CO2 from a point source can also be
by capturing CO2 directly from the air or capturing CO2 from a captured photosynthetically or electrosynthetically into
biogenic source, (2) the CO2 is stored permanently and not biomass by living organisms:15,37 microalgae are cultivated
re-emitted to the atmosphere at a later point, and (3) the net at CO2 concentrations of 5%–20%, making flue gas a suitable
quantity of CO2 stored permanently through CCU is greater source, and have a conversion efficiency of solar energy into
than the quantity of CO2 emitted over the product’s full life cycle, chemical energy higher than that of terrestrial plants (3%–
including use of the product and the emissions associated with 8% instead of 0.5%).38 Co-location of the facility at the site
the energy required for the CO2 capture and conversion pro- of the point source is important to avoid the need for trans-
cesses. When the criteria for CDR are not met but the life cycle porting flue gas.39 Other options for biofixation include micro-
emissions are lower than for the substituted product, CCU is organisms such as acetogenic bacteria40 or anaerobic CO2-
considered a climate change mitigation measure. Avoided emis- sequestering bacteria.38
sions compared with the substituted product may be presented CO2 capture from ambient air
as a negative number but should not be confused with physical DAC of CO2 can be performed using a range of separation pro-
removal of CO2 from the atmosphere.27 cesses. Because atmospheric CO2 concentrations (approxi-
mately 400 ppm) are 100–300 times lower than for point sources,
Capture of CO2 energy requirements, and therefore costs, for DAC are substan-
CO2 capture from a point source tially larger than for point source capture.41,42 Expert elicitation
CO2 is typically captured from a point source, such as flue gas leads to expected cost declines to around 200 US dollars
streams at power plants or industrial plants, or from industrial (USD) per ton of CO2 captured by 2050,43 still higher than the
processes where CO2 is produced as a by-product. Capturing 15–35 USD per ton of CO2 captured for high-purity point sources
CO2 from a bulk gas stream entails separating the CO2 from and 60–120 USD per ton of CO2 captured for lower-purity point
the rest of the stream. Sometimes CO2 separation is already sources; e.g., steel or cement production.17,44 An exception
required in the primary production process; for example, in would be when lower-purity CO2 streams are sufficient, such
ammonia synthesis, natural gas processing, and biogas upgrad- as for microalgae.45 The two main categories of DAC methods
ing to biomethane.28 This leads to a high-purity stream of CO2 are based on (1) amine-functionalized solid sorbents, which
along with the primary product. require regeneration at low temperatures or via moisturizing,46
Depending on the concentration and components present in a and (2) alkaline hydroxide capture solutions, which require
gas stream, one of three main separation processes may be high-temperature solvent regeneration.47 Less energy-intensive
most suitable29: (1) absorption of CO2 in a liquid solvent, (2) regeneration processes are under development, including elec-
adsorption of CO2 onto a solid, and (3) using a membrane to trochemical regeneration48 and bipolar membrane electrodi-
separate CO2 through selective permeability.30 In CO2 absorp- alysis.49
tion processes using amine-based solvents like monoethanol-
amine, CO2 is chemically bound, and then the CO2 is stripped Utilization of CO2
to allow the solvent to absorb CO2 again in the next cycle. This Direct uses of CO2
is called regeneration of the solvent and requires heat. Besides CO2 can be used directly, without conversion, in several sectors.
single-amine absorption, amine blends are in development In horticultural production, elevating CO2 concentrations in
where amines are combined for complementary characteristics. greenhouses increases crop yields by approximately 50%.50
An integrated CCU process has also been proposed to reduce This process is called CO2 enrichment and is traditionally
the overall energy demand, absorbing CO2 from raw natural achieved by combustion of fossil fuels such as diesel50 or natural
gas in methanol, after which conversion takes place.31 Other de- gas,51 which has the dual purpose of greenhouse heating.
velopments include ionic liquids, which are liquids composed Because more CO2 is required to reach the desired CO2 concen-
entirely of ions with a melting point of less than 100
C.32 Physical tration than is produced for heat, captured CO2 can be used.50
adsorption research has focused on improving the adsorbents CO2 can also be used directly as a refrigerant for supermarket
as well as the adsorption processes of regeneration.32 Alterna- applications, replacing hydrofluorocarbons with higher global
tives, like high-temperature solid adsorption of CO2, require warming potentials,52 reducing risks of leakage and associated
less energy input for regeneration compared with low-tempera- global warming effects.53 CO2 can also be used as a carbonating
ture liquid absorption.33–35 Use of membranes for CO2 separa- agent in sugar production and soft drinks, as a solvent for extrac-
tion is based on creating configurations especially for CO2 selec- tion of flavors, in the decaffeination process, as dry ice, in fire ex-
tivity from polymer or ceramic materials.33 tinguishers, and in the pharmaceutical industry as a respiratory
Other emerging CO2 capture technologies are high-temper- stimulant.16,21,54
ature solid looping systems: calcium carbonate looping, EHR
where calcium oxide is used as a sorbent that binds CO2 to Enhanced oil recovery (EOR) is a method where CO2 is injected
form limestone, and chemical looping combustion, where a into the subsurface to recover oil from almost depleted reser-
metal oxide is used to separate CO2 from other components voirs. EOR is a mature technology that has been practiced
in the flue gas, foregoing the need for gas separation, followed commercially for decades, starting in the early 1970s in North
by an exothermic metal oxide regeneration reaction.32,36 America.25 Similarly, CO2 can be used to recover natural gas
Cryogenic systems are based on the differences in the tem- from coalbeds (enhanced coalbed methane [ECBM]), although
perature and pressure at which constituent gases in flue gas there are currently no active ECBM projects.55 Although the
become liquid, removing CO2 from the bulk stream by cooling source of CO2 for EHR is typically natural CO2 reservoirs (not

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part of our definition of CCU), EHR can also be performed with ter-gas shift (rWGS) reaction and mixing it with H2 or via steam
CO2 captured from point sources or DAC.45 methane reforming (SMR) and, finally, using the Fischer-Tropsch
Mineral carbonates and construction materials process to create hydrocarbon chains.82 The stoichiometric ratio
Mineral carbonation is a process where CO2 reacts with magne- of H2 to CO in syngas can be adjusted to the targeted end prod-
sium or calcium oxides, -hydroxides, or -silicates in an ucts, as occurs currently via the WGS reaction in conventional
exothermic reaction, forming stable carbonate products;56 ex- syngas-based processes.83
amples of magnesium- or calcium-rich materials are mined min- In photocatalytic conversion, CO2 is converted to, for
erals57 or industrial residues such as slag from steel produc- example, methane or methanol using sunlight, water, and dye-
tion,58,59 red gypsum,60 fly ash,61,62 or desalination brines.63 sensitized semiconductors.84 Electrochemical reduction, where
These processes can be categorized into direct or indirect CO2 is reduced at atmospheric temperature using electricity,85
carbonation processes.59 In the direct carbonation process, a can be used to produce, for example, ethanol,12 methanol,86,87
gas-solid reaction takes place between CO2 and the ground min- dimethyl carbonate (DMC),20 formate,88 or formic acid.85 When
erals. The produced carbonates can be used in concrete, CO2 is captured by microalgae, the microalgae can be converted
asphalt, and other construction practices.64 In the indirect into fuels or chemicals; e.g., via transesterification or hydrogena-
carbonation process, magnesium or calcium ions are first ex- tion of algal oil89,90 or hydrothermal liquefaction.91 Microalgae
tracted in an alkaline solution, and then they react with CO2 to may also be used as fish food92 or food.93
form precipitated magnesium carbonate (PMC),63 precipitated
calcium carbonate (PCC)59 or nano-calcium carbonate
(NCC).65 These carbonates can be used as a pigment or filler ma- ASSESSING THE PARIS COMPATIBILITY OF CCU
terial in production of paper, plastics, and pharmaceuticals.66 TECHNOLOGIES
CO2 can be used to cure concrete, absorbing CO2 instead of
steam in the hardening process. Steam-cured concrete normally Paris compatibility criteria
re-absorbs roughly 30% of its production’s CO2 emissions dur- In this paper, a CCU technology is classified as Paris compatible
ing its lifetime,67,68 so emissions are not reduced by CO2-accel- when its deployment is expected to be in line with reaching the
erated curing in itself. Instead, the reduction is achieved because Paris Agreement’ LTTG and corresponding 1.5
C mitigation
of the lower steam requirement69 and the improvements in me- pathway. This definition results in two questions to assess Paris
chanical properties, reducing the amount of cement compatibility: (1) is the CCU technology ready on time and (2)
required,70–72 in a similar way as addition of ‘‘cementitious’’ ma- does the CCU technology sufficiently reduce CO2 emissions?
terials like carbonated minerals reduces the need for cement in These questions result in the Paris compatibility criteria for
concrete.61,73 Other options under development include produc- 2030 and 2050 outlined in this section (Figure 2). The following
tion of carbon nanomaterials like graphene,74 nanofibers, or two sections present a review of the literature underlying the
nanotubes from CO2,75 which can be used in construction, criteria and explain how these criteria can be applied to CCU
reducing energy and material demand in the manufacturing technologies.
process.76 Maturity criteria
Fuels and chemicals Technological maturing, the process leading from research and
Fuels and chemicals directly based on fossil fuels or fossil feed- development (R&D) to demonstration trials, early market forma-
stocks are energy-dense products. Therefore, producing these tion, and widespread diffusion, can span several decades and is
chemicals or fuels from CO2 often requires an energy-intensive ridden with financial risks and technological uncertainties.94 We
conversion process at high pressure and/or increased tempera- include technological maturity as a criterion for Paris compati-
ture, supported by catalysts, because CO2 is an inert and ther- bility because for a technology to be able to contribute to emis-
modynamically stable molecule. Conversion processes include sion reductions in 2030 or 2050, it must be developed sufficiently
thermochemical, electrochemical, and photocatalytic con- to be ready for widespread diffusion.
version. The technological readiness level (TRL) of a technology is an
In thermochemical conversion (sometimes referred to as ‘‘hy- indication of the maturity of a technology on a scale that summa-
drogenation’’), CO2 and H2 are prepared separately and subse- rizes detailed information on technological maturity into a single
quently combined.77 The hydrogen supplies part of the energy value.95 The scale has nine levels, spanning from basic concept
needed for the CO2 conversion process. This process allows (TRL 1) to successful, real-life operation (TRL 9). TRL 6 presents
production of chemicals and fuels that would otherwise be of a turning point in technological development by requiring an
fossil origin, like methane or methanol.12 Methanol, in turn, can operational system at a relevant scale. The time it takes to prog-
serve as a feedstock for production of other chemicals and fuels, ress through the TRL scale differs per technology and is context
such as ethylene,78 polyols,79 and dimethyl ether (DME).80 dependent, but for CCU technologies, 10–15 years is typically
Methane production can be a method for long-term storage of assumed to be needed to progress from lab scale to full-scale
renewable energy from intermittent electricity, producing H2 implementation.9,96,97 In line with Chauvy et al.,9 we assume
with water electrolysis, followed by CO2 hydrogenation to that, for a CCU technology to be ready in 2030, it must be in at
methane (Sabatier reaction) and methane combustion for power least TRL 6 in 2020. Given that it is possible to progress from
generation at a later time (power-methane-power).81 Another the R&D phase (TRL 1–3) to real-life operation (TRL 9) in 20–30
key hydrogenation process is synthesis of liquid hydrocarbon years,9,98 the TRL is no impediment for a CCU technology for
fuels, which consists of synthesis gas (syngas) production via 2050. This does not mean that it can be assumed that a technol-
conversion of CO2 to carbon monoxide (CO) in the reverse wa- ogy in the R&D phase in 2020 will be ready in 2050, only that a

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50
Paris-compa ble mi ga on pathway Paris compa bility criteria for CCU
Global anthropogenic CO2 emissions (GtCO2/yr)

40
Technological maturity Emission reduc on

30
2030 ≥6 ≤ 50%

20 Half of 2020 emissions

2050 ≥1 ≤0
10

-10
2010 2020 2030 2040 2050 2060

Figure 2. Paris compatibility criteria for CCU technologies

Paris-compatible mitigation pathway using scenario data from Huppmann et al.1 as the mean of no and low overshoot 1.5
C scenarios from which Paris
compatibility criteria for CCU technologies for 2030 and 2050 were derived. TRL is the 2020 technology readiness level, ECCU are the emissions associated with
the CCU product (in kgCO2-equiv/kg CO2 utilized), and Esubstitute are the emissions associated with the substituted product (in kgCO2-equiv/kg CO2 utilized).

technology cannot be excluded from Paris compatibility in 2050 a certain field; for example, in the chemical industry102 and even
based on its 2020 TRL. for CCU technologies9 (Table 1). Despite the differences between
Emissions criteria descriptions of TRLs, the commonality is that TRL 6 represents a
1.5
C-pathways are characterized by two key numbers: in 2030, break from the foregoing TRLs by requiring an operational system
global net CO2 emissions are halved compared with 2020 emis- at a relevant scale (pilot plant) to have been developed.
sions, and in 2050, net CO2 emissions are zero.3 For CO2 emis- To assess whether a CCU technology fulfills the Paris compat-
sion reductions to be in line with 1.5
C pathways, the CCU tech- ibility maturity criteria, its TRL in 2020 must be determined from
nology must halve CO2 emissions associated with production direct TRL specifications or by applying the milestones as defined
and use of the CCU product by 2030 compared with the emis- by Buchner et al.102 (Table 1) to descriptions of the technology’s
sions associated with the current conventional, substituted state of development. Table 1 includes examples of CCU technol-
product. In 2050, CO2 emissions associated with the CCU prod- ogies for each TRL, and Note S2 provides a comprehensive over-
uct must be zero to be Paris compatible. Although emission data view of TRL ratings of CCU technologies. Some studies report
are often provided for a basket of greenhouse gases (GHGs) ranges instead of a single TRL for a CCU technology. This can
instead of CO2 only, CCU is focused on reducing CO2 emissions, be done for three reasons: (1) the technology is a ‘‘composed’’
which is by far the most prominent contributor to total GHG technology made up of multiple processes, each with its individ-
emissions, directly as well as indirectly.99,100 ual TRL. Hence, the range of these individual TRLs is reported; (2)
more than one technology is in development to produce a CO2-
Maturity of CCU technologies based product, and the full range is reported for this product
The TRL scale has its origin at the American National Aeronautics instead of for each production process separately; or (3) there is
and Space Administration in the 1970s and became more widely uncertainty because of a lack of data. In this paper, we deal
known when the US Department of Defense started using it to with these ranges in TRL in the following way: in the case of a
improve its technology R&D outcomes.101 It was first comprehen- composed technology (reason 1), the lowest TRL is counted as
sively described by Mankins,95 and has since received recogni- the overall TRL because it is the weakest link in the chain in the
tion in policy-making, industry, and academia.102 For example, process to commercialization.102 We specify a TRL for each
in 2010, the European Commission advised projects that received CCU production process rather than only per CCU product
European Union (EU) funding to use TRLs for identification of (reason 2). Uncertainty in the TRL is resolved by comparing re-
technological maturity.103 Its use has also been recommended ported process descriptions (e.g., proof of concept, bench-scale
specifically for CCU techno-economic assessments.24,104 process, pilot plant) with the descriptions of Buchner et al.102 to
The European Commission defines TRLs in a generalized way to find the best match (reason 3), as explained in Note S2.
allow comparability of technologies in different fields, including en-
ergy and climate technologies (Table 1).105A downside of a gener- Emissions of CCU technologies
alized scale is the general description for each level, including To assess the Paris compatibility of CCU technologies, we deter-
criteria that may not be applicable or not specific enough to mined the GHG emission intensity of CCU products (kgCO2-
achieve unambiguous TRL ratings.102,106 Adaptations to the equiv/kg CO2 utilized) and of substituted conventional products
generalized scale were developed to better rate technologies in (assuming 1:1 replacement) based on a literature search of life

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Table 1. Technology readiness levels for CCU technologies

Description by Buchner
Description by European Description by Chauvy et al.9 et al.102 for the chemical
TRL Commission105 for CCU evaluation industry CCU examples
1 basic principles observed published research that idea; ppportunities methanol via photocatalytic
identifies the principles that identified, basic research conversion9,84
underlie the technology translated into possible
applications
2 technology concept publications or other concept; technology ethanol12 and methanol107
formulated references that outline the concept and/or application via electrochemical
application being considered formulated, patent research reduction108
and that provide analysis to conducted
support the concept; the
step up from TRL 1 to TRL 2
moves the ideas from pure to
applied research; amajor
part of the work is analytical
or paper studies;
experimental work is
designed to corroborate the
basic scientific observations
made during TRL 1 work
3 experimental proof of active R&D has been proof of concept; applied ethylene via electrochemical
concept initiated; at TRL 3, the work laboratory research started, reduction,109 DME via
has moved beyond the functional principle/reaction syngas12,110
publication phase to (mechanism) proven,
experimental work predicted reaction observed
(qualitatively)
4 technology validated in lab TRL4–6 represent the bridge preliminary process PCC and PMC63,66,97,111
from scientific research to development; concept
engineering; TRL 4 is the first validated in laboratory
step in determining whether environment, scale-up
the individual components preparation started, shortcut
will work together as a process models found
system
5 technology validated in basic technological detailed process formic acid via
relevant environment components are integrated development; process electrochemical reduction in
so that the system models found, property data an aqueous
configuration is similar to the analyzed, simulation of environment,63,66,97,111
final application in almost all process and pilot plant using sodium bicarbonate using
respects bench scale information flue gas directly63,66,97,111
6 technology demonstrated in represents a major step up in pilot trials; pilot plant Fischer-Tropsch fuels,97,112
relevant environment a technology’s constructed and operated urea from steel gases113,114
demonstrated readiness; with low-rate production,
TRL 6 begins true products approved in final
engineering development of application, detailed process
the technology as an models found
operational system
7 system prototype TRL 7 is a significant step demonstration and full-scale CO and syngas via the
demonstration in an beyond TRL 6, requiring an engineering; parameter and reverse water gas shift
operational environment actual system prototype performance of pilot plant reaction,12,112 methane and
optimized, (optional) demo methanol via hydrogenation
plant constructed and of CO29,115,116
operating, equipment
speciation, including
components that are type
conferrable to full-scale
production
(Continued on next page)

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Table 1. Continued
Description by Buchner
Description by European Description by Chauvy et al.9 et al.102 for the chemical
TRL Commission105 for CCU evaluation industry CCU examples
8 system complete and represents the end of true commissioning; products Polyols,9,117,118 construction
qualified system development; the and processes integrated in materials from carbonated
technology has been proven organizational structure steel slag51,119,120
to work in its final form and (hardware and software), full-
under the expected scale plant constructed
conditions
9 actual system proven in an technology is in its final form production; full-scale plant CO2 enrichment in
operational environment and operates under the full audited (site acceptance agricultural greenhouses,121
range of operating mission test), turn-key plant, CO2 EOR55,122
conditions production operated over full
range of expected conditions
in industrial scale and
environment, performance
guarantee enforceable
Shown are descriptions of technology readiness levels (TRL) and examples of CCU technologies for each TRL. See Note S2 for an overview of TRLs for
all studied CCU technologies.

cycle assessment (LCA) studies on CCU. In this way, 1,041 CCU product and substitute. In our analysis, we determine the
studies were identified (see experimental procedures). After absolute CO2 emissions of a CCU product and the percentual
screening these papers for relevance and excluding reviews CO2 emission reduction of a CCU product relative to its substi-
and meta-analyses without original data, 106 studies remained tute. This requires a wider ‘‘cradle-to-grave’’ approach that in-
(Note S3). We then selected the most recent study with the cludes end-of-life emissions for both products. In practice, how-
most complete life cycle inventory for each available combina- ever, data on transport and use-phase emissions often lack in
tion of CCU technology and type of CO2 source (fossil, biogenic, the reviewed LCA studies, except for re-emission of CO2 upon
or atmospheric). Not all combinations could be found in the liter- combustion or dissolution. So where cradle-to-grave data
ature. This resulted in 30 studies (1 on direct use, 6 on EHR, 8 on were not available, we used cradle-to-factory-gate emissions
mineral carbonates and construction materials, and 15 on fuels and added end-of-life emissions, as proposed by Fernández-
and chemicals), together covering 44 unique CCU technologies Dacosta et al.,23 assuming that use-phase emissions were
and resulting in 74 CCU technology-CO2 source combinations negligible. Combustion and dissolution were then included in
(see Note S3, which also provides an overview of the specific the end-of-life emissions. We did not harmonize production
CO2 sources and CO2 capture processes covered). These infrastructure and transport emissions and follow the choices
studies were harmonized regarding (1) functional unit, (2) system in the respective LCAs because these emissions contribute
boundaries, (3) electricity mix, (4) hydrogen production, (5) negligibly to the total GHG intensity.124–126 For the substituted
dealing with multifunctionality, and (6) accounting of temporary products, emissions were also determined based on a cradle-
carbon storage, as detailed below. For the substituted products, to-grave basis.
we followed the choices made in the original papers, assuming Electricity mix
the CCU product replaces a product with identical molecular To improve inter-comparability of CCU products and take into
structure or, if this does not exist, a product with the same char- account the expected decarbonization of the electricity
acteristics and function.24 sector,127 we harmonized the GHG intensity of electricity used
Functional unit in all foreground processes of the studies considered. This in-
The functional unit of CCU products can be end product-based cludes electricity use in the capture and conversion process
(e.g., kg or MJ product) or input-based (e.g., kg CO2 utilized). and hydrogen production via electrolysis. The harmonized
Most CCU LCA studies use an end product-based functional GHG intensity of electricity was set to be in line with emissions
unit, which allows estimating absolute emission reductions pathways limiting global warming to 1.5
C:3 0.17 kgCO2/kWh
when switching to a CCU product. However, to be able to for 2030 and 0 kgCO2/kWh for 2050. For zero-emissions elec-
compare different CCU technologies, the functional unit should tricity, it is assumed that the (limited) emissions of renewable
be the same and, thus, input based.12,123 We therefore use electricity production are compensated by CDR (e.g., from bio-
1 kg of CO2 utilized as functional unit in this paper. It is possible energy with CCS).
to go from an end product-based functional unit to the functional Hydrogen
unit of 1 kg of CO2 utilized by determining the product’s GHG in- Hydrogen is an important feedstock in the production of fuels
tensity in kgCO2-equiv/kg product and multiplying it by kg prod- and chemicals from CO2 and is produced using fossil fuels
uct/kg CO2 utilized. with or without CCS or water electrolysis. Because we assume
System boundaries hydrogen production to decarbonize in Paris-compatible path-
Most LCA studies quantify ‘‘cradle-to-factory-gate’’ emissions, ways, we harmonize all studies toward electrolysis-based
assuming that emissions beyond the gate are the same for hydrogen following their reported electricity requirements,

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A B

C C

, ,

Figure 3. Determining the GHG intensity of CCU products through the substitution approach
(A and B) In the system expansion via substitution approach, the GHG intensity of the CCU product ECCU is determined by the difference between the emissions of
(A) the multifunctional system and (B) the marginal production system of the primary product.

unless H2 is co-produced in the conversion process. For an elec- than release of utilized CO2 (for example, from fossil feed-
tricity requirement of 52 kWh/kg H2 and using the aforemen- stock added in the conversion process); and
tioned electricity carbon intensities for 2030 and 2050, electrol- Ereleased GHG emissions of utilized CO2 to the atmosphere at
ysis-based hydrogen results in 6.85 kgCO2-equiv/kg H2 in the end of life of the CCU product.
2030 and 0 kgCO2-equiv/kg H2 in 2050. We use the substitution
approach to deal with the co-produced O2 (experimental pro- In most cases, Eutilized and Ereleased cancel each other out.
cedures). However, Ereleased is less than Eutilized when some of the utilized
Multifunctionality CO2 is lost in the conversion process (i.e., included in Econversion )
The CCU production chain is typically inherently multifunctional; or when the CO2 is stored permanently; then Ereleased is zero. A
an industrial facility or power plant produces a primary product negative value for ECCU can occur when CO2 is stored perma-
(e.g., steel or electricity) as well as CO2, which is used as feed- nently and the amount of CO2 utilized is greater than the com-
stock in the secondary CCU process. GHG emissions of this sys- bined emissions of the CCU production, use, and end-of-life
tem must be divided between the primary product and the sec- processes.
ondary CCU product. DAC-based CCU systems are not The interpretation of a negative value for ECCU depends on the
multifunctional because there is no primary product. We apply source of CO2. In the case of CO2 with a fossil origin, a negative
system expansion via a substitution approach to solve this multi- ECCU means that the total GHG emissions of the system with
functionality problem following the LCA standard ISO 14044 and CCU are reduced in comparison with the system without CCU
LCA guidelines for CCU104 (Figure 3). and that this emission reduction can be attributed to CCU. It
System expansion via substitution assumes that a primary does not mean that CCU is CDR because CO2 is not removed
production plant with CCU directly substitutes an identical plant from the atmosphere.27,128 In the case of CO2 that is removed
without CCU to ultimately determine the emissions that can be from the atmosphere, directly (through DAC) or indirectly
associated with CCU itself. It is formalized as shown in Equation (through capture of CO2 with biogenic origin), a negative value
1 (for a full derivation, see experimental procedures): for ECCU does mean that CDR takes place. For biogenic CO2,
CDR would also require sustainable sourcing of the
ECCU =  Eutilized + Ecapture process + Econversion + Eother + Ereleased biomass used.
(Equation 1) The substitution approach is based on the assumption that a
point source without capture is 1:1 substituted by the same
where E stands for GHG emissions (in kgCO2-equiv/kg CO2 uti- plant with capture. In the near future (i.e., 2030), this assump-
lized), specifically tion holds because many plants without capture can still be
substituted. In the long run, however, the reference system is
ECCU GHG emissions of the CCU product; expected to transform toward a zero-emissions economy.
Eutilized CO2 utilized in production of the CCU product; Therefore, in a Paris-compatible 2050 system, we can no
Ecapture process GHG emissions associated with capturing CO2 longer assume that there are unabated fossil point sources to
and separating CO2 from the bulk gas stream; substitute and associated emissions to avoid. Because emis-
Econversion GHG emissions of the conversion process of CO2 sions are no longer unabated, considering CCU as an option
into the end product; to abate fossil CO2 emissions means that the responsibility
Eother other (remaining) GHG emissions associated with the for not emitting shifts to CCU. In terms of calculating the
CCU product, such as GHG emissions at end of life other GHG intensity of CCU for a fossil CO2 source in 2050, this

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Table 2. GWP factors (GWPstorage-100) for temporary storage of CO2 in CCU products using a 100-year time horizon
Lifetime 0–6 months 0.5–1 year 1 year 5 years 10 years 25 years 50 years 100 + years
GWPstorage -100 1 0.99 0.98 0.92 0.85 0.67 0.42 0

means that all emissions from the stack onward are assigned to the following attributes: (1) preventing (high) capture emissions,
the CCU product: (2) preventing (high) conversion emissions, (3) preventing
re-emission of CO2, and (4) replacing an emission-intensive
ECCUðfossil in 2050Þ = Ecapture losses + Ecapture process process.
(Equation 2)
+ Econversion + Eother + Ereleased Paris-compatible CCU technologies in 2030 are CO2 enrich-
ment in the horticulture industry50 with CO2 from a co-located
where E stands for GHG emissions (in kgCO2-equiv/kg CO2 uti- biogas to biomethane upgrading unit, which is considered a
lized), specifically by-product (i.e., is characterized by attribute 1) and can be
used directly (attribute 2). In the carbonation process of steel
ECCUðfossil in 2050Þ GHG emissions of the CCU product (for 2050 slag to produce construction blocks, flue gas is used directly,58
in a Paris-compatible scenario where substitution of un- omitting the capture step (1). CO2 is stored permanently through
abated fossil CO2 point sources cannot be assumed) and an exothermic carbonation reaction134 (2 and 3). In EOR, CO2 is
Ecapture losses CO2 not captured in the capture process, used directly (2) and can be Paris compatible for several gas sep-
assuming a capture rate of 95%.32,81,122 aration methods135–137 as long as no more than 2 barrels of oil
(bbl) are recovered per ton CO2 injected. This allows a favorable
In the results, we report ECCU , but when this applies to fossil
balance of the CO2 released upon combustion of the recovered
CO2 sources in 2050, Equation 2 is used for the calculation.
oil and the CO2 stored permanently (3). Urea production from
For CCU processes based on biogenic or atmospheric CO2 in
basic oxygen furnace gas (BOFG) uses waste heat from the steel
2050, Equation 1 still applies because availability of these sour-
plant for capture and conversion processes (1 and 2) and re-
ces in 2050 is in line with a Paris-compatible scenario.
places electricity production from BOFG.113 Hence, quantifica-
Benefits of temporary storage of CO2
tion of the GHG intensity of urea includes replacement of elec-
The importance of a product’s lifetime for CCU’s contribution to
tricity produced from BOFG by the 1.5
C-compatible electricity
climate change mitigation has been stressed in the litera-
mix (4). Last, close to halving emissions is CO via rWGS with rela-
ture.26,129 Temporary storage of CO2 by lowering atmospheric
tively low conversion emissions (2).12
CO2 concentrations for the duration of the product’s lifetime
Low TRL CCU technologies that only fulfill the emissions crite-
decreases radiative forcing over this period of time.130 We
rion can be characterized by the same four attributes. The so-
calculated the GHG intensity of CCU products without (base
dium bicarbonate process uses flue gas directly, avoiding the
case) and with the benefit of temporary carbon storage (sensi-
capture step (attribute 1).138 Indirect mineral carbonation reac-
tivity analysis) using a time horizon of 100 years. Global warm-
tions producing PMC or PPC may have low emissions for high
ing potentials are used for this calculation, adjusted for tempo-
efficiency of the alkaline absorption process, depending on pro-
rary carbon storage (global warming potential [GWP]storage).
cess development. They store CO2 permanently (3).63 Formic
Global warming potentials describe the contribution to radiative
acid via hydrogenation reduces emissions sufficiently compared
forcing of delayed CO2 emissions compared with direct CO2
with the emission-intensive substitute (4).12 Electrochemical pro-
emissions over 100 years. We derived the GWPstorage-100 fac-
duction of formic acid via supercritical CO2139 and methane and
tors using the method described by Guest et al.,131 which is
methanol via photocatalytic conversion84 have low conversion
based on Clift and Brandao,132 combined with the more recent
emissions (2) because they do not require electricity-intensive
atmospheric CO2 decay curves described by Joos et al.133 The
hydrogen.
factors depend on the lifetime of the CCU product, as shown in
High TRL CCU technologies not fulfilling the emissions crite-
Table 2; see the experimental procedures for an overview of
rion can also be characterized by the aforementioned attributes.
CCU lifetimes. To include the storage effect, Ereleased in Equa-
However, here, these are the reasons for not fulfilling the emis-
tions 1 and 2 is multiplied by GWPstorage-100. In this way,
sions criterion. CO2 curing of concrete72,140 does not sufficiently
only captured CO2 is affected by this temporary storage
reduce emissions because of the emissions associated with
benefit, not fossil carbon added in some CCU routes as addi-
cement production (2). Fuels and chemicals based on thermo-
tional feedstock.
chemical conversion typically have high conversion emissions
because of electricity-intensive hydrogen production (2). Finally,
FULFILMENT OF PARIS COMPATIBILITY CRITERIA EOR with a recovery ratio over 2 bbl per ton of CO2 injected does
not store a sufficient volume of CO2 compared with combustion
Paris compatibility in 2030 emissions141,142 (3).
Figure 4 shows the relative GHG intensity of CCU technologies Benefits of temporary CO2 storage
in 2030 plotted against their 2020 TRL. As explained above, a Some products store CO2 for several decades; e.g., polyeth-
negative GHG intensity ratio means that an emissions reduction ylene and polypropylene. Adding the temporary storage benefit
takes place for fossil CO2 and CDR when the source of CO2 is based on a lifetime of 50 years leads to a reduced GHG intensity
biogenic or atmospheric. CCU technologies fulfilling the 2030 of roughly 25%. This, however, is not enough to lead to a differ-
emissions criterion can be characterized by one or more of ence in Paris compatibility. For long-lived polyols, the reduction

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Figure 4. Paris compatibility of CCU
technologies in 2030
Technological maturity of CCU technologies in
terms of their 2020 technology readiness level and
GHG emission intensity ratio of the CCU product in
2030 compared with its substitute. The four shapes
represent the four CCU categories, and the colors
are used to differentiate between the different types
of CO2 sources. For a CCU technology to be Paris
compatible in 2030, it must currently have a TRL of 6
or higher and reduce emissions by at least 50%
compared with its substitute. Technologies in the
lower right gray area fulfill these Paris compatibility
criteria. The full dataset, including outliers not
shown in this figure, and source data for this figure
are provided in Data S1.

are fulfilled). In addition, steel slag carbon-

ation using fossil flue gas directly to pro-
duce cementitious material58 achieves
close to zero emissions because no cap-
ture process is required, the carbonation
process is exothermic, and the CO2 is
stored permanently (fulfilling criteria 1
and 2).
Because CO2 is not stored permanently
in fuels or chemicals, these products can
only be strictly Paris compatible when the
CO2 is of biogenic or atmospheric origin
and zero emissions are associated with
the capture and conversion processes (ful-
filling criteria 2 and 3). This situation is ap-
proached when heat integration is applied,
electric heat is used, or simply only elec-
tricity is required. Processes approaching
zero emissions are methane production
from H2 and biogenic CO2;143 DMM via
condensation with formaldehyde or via
direct synthesis, both for a biogenic
source;144 and Fischer-Tropsch fuels
from atmospheric CO2, based on a fully
electric process for capture and conver-
is only a few percent because a large share of the embodied car- sion.145 The assumption of zero-emission electricity is crucial
bon is from fossil feedstock, to which the storage factor does not because the GHG intensity of these options using the 2030 elec-
apply. The lifetime of the other chemicals and fuels is assumed to tricity mix is between 1.21 and 1.39 kgCO2-equiv/kg CO2 utilized
be 6 months, where the GWPstorage-100 factor of 0.99 does not (see Figure S1 for the absolute GHG intensity of CCU products
affect Paris compatibility. For EHR, construction materials, and in 2030).
most mineral carbonates, permanent storage was already Benefits of temporary CO2 storage
assumed in the base case. Inclusion of the benefit of temporary storage of 6 months is
Paris compatibility in 2050 enough to obtain a negative absolute GHG intensity for DMM
Figure 5 shows the GHG intensity of CCU products in 2050 via condensation with formaldehyde or via direct synthesis,
(ECCU , in kgCO2-equiv/kg CO2 utilized) (Equations 1 and 2). In both for a biogenic source.144
2050, low low-TRL technologies may be Paris compatible. The
characteristics of CCU technologies fulfilling the 2050 emissions DISCUSSION AND RESEARCH OUTLOOK
criterion are simplified to (1) preventing re-emission of CO2, (2)
only using zero-emissions energy, and (3) utilizing CO2 recently Maturity
removed from the atmosphere (biogenic/atmospheric). We considered technological maturity in terms of TRLs of indi-
Construction blocks from carbonation of steel slag using a pu- vidual technologies because data are available for individual
rified stream of biogenic CO2134 are Paris compatible, resulting in technologies. Others have suggested ‘‘system readiness
CDR because the CO2 is stored permanently (i.e., criteria 1 and 3 levels’’146,147 to reflect the technology’s need to embed in a

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Figure 5. Paris compatibility of CCU
technologies in 2050
GHG intensity of CCU products in 2050 (kgCO2-
equiv/kg CO2 utilized). The four shapes represent
the four CCU categories, and the colors are used to
differentiate between the different types of CO2
sources. The TRL is not indicated because 2020
technological maturity does not preclude technol-
ogies from fulfilling the Paris compatibility criteria by
2050. Technologies in the lower gray area fulfill
these Paris compatibility criteria. The full dataset,
including outliers not shown in this figure, and
source data for this figure are provided in Data S1.

mental effect of technologies is expected

to decrease as they mature because of
energy efficiency improvements and/or
development of catalysts for more effi-
ethylene, ER cient conversion;139,127 (3) some CCU
ethylene, MTO precipitated magnesium carbonate
processes could be adapted so that
precipitated calcium carbonate
FT-fuel carbonated slag cementitious material more CO2 is utilized per product pro-
dimethoxymethane, direct duced (for example, for EOR);150 and (4)
CH4 dimethoxymethane, with formaldehyde
if product lifetimes could be extended,
then they could, based on the temporary
storage benefit, decrease their contribu-
tion to climate change. Future LCA
studies could focus on CCU technolo-
gies that are developing quickly and for
carbonated slag construction block which no LCAs are available or for which
only LCAs based on low-TRL data are
available or on how CCU processes
can be adapted to reduce overall
emissions.
Even when the emissions criteria are
not fulfilled, it is possible that there are
no future alternative technological routes
that provide the same product at a lower
GHG intensity. Although a CCU technol-
ogy is not strictly Paris compatible in
such cases, CCU could still play a role
in the overall energy system transition.
In addition, if other environmental effects
certain system. Because of this embedding, assessment of besides climate are included in the equation, then CCU op-
technological readiness at a systemic level could lead to lower tions may, in certain cases, be viewed more positively than re-
levels of maturity. This means that Paris compatibility of CCU maining alternatives to our fossil fuel-based production sys-
could be overestimated. On the other hand, concerted, trans- tem. For instance, CCU products do not have the land-use
disciplinary action on innovation could speed up technological effects of crop-based biomaterials (including biodiversity).151
maturing of promising technologies. For example, this could Further research could include alternative routes for the
apply to sodium bicarbonate, which fulfills the emission reduc- assessment and define emission reduction criteria per prod-
tion criterion but is in TRL 5. As a next step, ‘‘technological uct group. The assessment of emission reduction could be
innovation system’’ analyses148,149 can be performed to pro- extended beyond the technology level to the sector or even
vide information on what actors can do to advance such tech- the system level. Determining the global climate change
nologies. mitigation potential of CCU at scale requires that interac-
tions with other mitigation options as well as broader changes
Emissions in the economy are considered, which may be achieved
Our harmonization allowed a comparison of CCU technolo- using integrated assessment models. Further research could
gies, but some uncertainty in future emissions remains focus on including CCU in these models and determining
because (1) LCAs of low-TRL technologies may be based on how much each CCU technology could contribute at scale
idealized modeling data, underestimating the environmental to CO2 emission reductions within and across different
effects because of an information bias;108 (2) the environ- sectors.

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Multifunctionality 2050 emissions criterion. A lock-in in these CCU processes

The multifunctionality problem is one that needs to be solved could be prevented by implementing an exit strategy for indus-
carefully and transparently. Otherwise, it is possible to end up tries relying on CCU processes that are only 2030 compatible.
with statements that cannot be simultaneously true, such as CCU technologies that are currently used or considered and
the following: CCU can make traditionally CO2-emitting indus- that are not 2030 compatible could lead to a lock-in within years.
tries (e.g., fossil fuel electricity generation, chemicals, cement) We recommend that these are critically evaluated regarding their
carbon-neutral10,75 while producing carbon-neutral CCU potential for a short-term exit strategy.
products.78,152 The reality is that the eventual emission of
CO2 must be accounted for by one of the processes. And, Sources of CO2 and capture processes
as shown above, when moving to a future without unabated We found that energy requirements for CO2 capture and their
fossil emissions, this emission has to be allocated to CCU. associated emissions differ between specific CO2 sources and
The right year of this allocation shift is unclear and may capture processes, in line with Mu €ller et al.128 and von der Assen
depend on the GHG reduction targets of a specific country, et al.159 Whether a CCU process is Paris compatible can thus
sector, or company. Although we consider the year 2050, depend on the capture process itself (e.g., a DAC process based
based on Paris-compatible emission pathways at a global on natural gas143 rather than renewable electricity145 may render
level, other countries or firms may have reasons to select a the entire CCU product non-Paris compatible). Our research has
different point in time where fossil points sources can no focused on available CO2 source-CCU technology combinations
longer go unabated. in the LCA literature, and further research could harmonize CO2
sources and capture processes to provide additional insights
Decarbonization of electricity into remaining CO2 source-CCU technology combinations.
The carbon intensity of electricity of 0.17 kgCO2/kWh that we This would allow including more innovative CO2 capture routes
used for 2030 is higher than the carbon intensity in many of and identifying more environmentally optimal combinations of
the CCU LCA studies; for example, when based on only renew- capture processes and conversion processes for different CO2
ables. This means that, in these cases, we found a higher 2030 sources.
GHG intensity of CCU products compared with the original
studies. Still, our 2030 carbon intensity of electricity may be CCU versus CCS
an underestimation because it was based on emission path- Cuéllar-Franca and Azapagic16 showed that, per ton of CO2
ways that only include use-phase emissions, not upstream captured, CCS results in lower emissions than CCU. Although
emissions. Our 2030 results, however, are not sensitive to capture emissions are the same, emissions for compression
this increase in carbon intensity; doubling the carbon intensity and injection of CO2 in geological formations are lower than
(0.34 kgCO2/kWh) did not affect Paris compatibility of technol- most CCU technologies’ emissions from conversion and ulti-
ogies in 2030. However, storing renewable electricity in a fuel or mate release of CO2. Based on this, only CCU technologies
chemical results in a loss of primary energy153 and has a low with low conversion emissions and permanent storage could
energy return on energy invested.21 Hence, use of low-carbon compete with CCS. Although the avoided emissions of the prod-
electricity for mitigation options other than CCU has been uct that CCU replaces are not taken into account,16 including
shown to achieve higher emission reductions per kWh; e.g., these could still lead to the same conclusion, as shown for meth-
for e-mobility and heat pumps10 or DACCS.154 Alternatively, anol.19 To deal with residual flows containing CO2 from essential
CCU technologies have been proposed to use excess renew- industries as long as they exist, further research could focus on
able electricity and aid the energy transition by balancing the systematic comparison of CCS and CCU technologies in light of
peaks of renewable power production.155,156 This suggestion their product-specific substitutes123 and TRLs.
is sobered by its limited economic attractiveness as a result
of the low-capacity factors,81 but further research on the sys- CONCLUSIONS AND POLICY RECOMMENDATIONS
temic effects of electrification of the CCU process would be
of value. By combining the literature on technological maturity of CCU
with the global emission reduction requirements consistent
Lock-in with the Paris Agreement, we conclude that only very few CCU
The only CCU technologies that are 2030 and 2050 Paris options would be Paris compatible. Moreover, some CCU op-
compatible are construction materials based on carbonation of tions only meet the criteria in the short run and could lead to a
steel slag, either using fossil flue gas directly or using CO2 lock-in toward 2050. We find that, for a CCU technology to be
captured from a biogenic source. Arguably, implementing CCU Paris compatible in 2030, it has to have low GHG emissions
options that only reduce emissions sufficiently for 2030 but not from CO2 capture and conversion, replace a GHG-intensive sub-
for 2050 could lead to a carbon lock-in, which would occur stitute, and (in most cases) lead to permanent storage. For 2050,
when large investments are made in 2030, complicating the criteria become more stringent, and Paris compatibility typi-
phase-out and discouraging necessary transitions later cally depends on a combination of no capture and conversion
on.157,158 Hence, assuming that a CCU production plant built emissions (e.g., by using zero-emission electricity or waste
in 2030 is still operational in 2050 would mean that the 2050 heat), permanent storage, and use of biogenic or atmospheric
emissions criterion should be added to assess 2030 Paris CO2 sources. Achieving CDR via CCU technologies is only
compatibility. In that case, with the exception of some construc- possible when biogenic or atmospheric CO2 is used and stored
tion materials, none of the 2030-compatible options fulfill the permanently.

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Although our conclusions are robust as a result of the harmo- Selection of LCA studies to determine the GHG intensity of CCU
products
nization approach we adopted, we also showed that determining
To assess Paris compatibility of CCU technologies, we determined the GHG
the CO2 emission reduction associated with a CCU technology emission intensity of CCU products (kgCO2-equiv/kg CO2 utilized) and of
depends on a range of assumptions. When designing policies substituted conventional products (assuming 1:1 replacement) based on a
for implementation of CCU technologies, clear guidelines for literature search of life cycle assessment studies on CCU. The Web of Science
search string used was as follows:
these assumptions must be in place. We recommend using a TOPIC = CCU* OR "carbon capture and utili$ation" OR "carbon capture
future electricity mix and considering the full life cycle, including utili$ation" OR "carbon capture and use" OR "carbon capture and re-use"
possible re-emission of CO2. To clarify the emission reduction OR "carbon dioxide capture and utili$ation" OR "carbon dioxide capture utili$-
ation" OR "carbon dioxide capture and use" OR "carbon dioxide capture and
potential of CCU, it should also be made very clear against
re-use" OR ‘‘carbon dioxide utili$ation’’ OR ‘‘carbon dioxide use’’ OR "CO2
what CCU is compared. We distinguish three benchmarks: (1) use" OR ‘‘CO2 utili$ation’’ OR ‘‘CO2 re-use’’ OR ‘‘CO2-enhanced’’ OR
emission reduction of CCU compared with emitting CO2 at the ‘‘CO2-based’’ OR ‘‘CO2-activated’’ OR ‘‘CO2 capture and utili$ation’’ OR
point source, (2) emission reduction of CCU compared with the ‘‘CO2 capture and use’’ OR ‘‘CO2 capture and re-use’’ OR ‘‘produc* from
CO2’’ OR ‘‘produc* from carbon dioxide’’ OR ‘‘carbonat* curing’’ OR ‘‘CO2
substituted original product, and (3) emission reduction of CCU curing’’ OR ‘‘carbonat* aggregate*’’OR (CO2 calcium carbonat*) OR (‘‘carbon
compared with other alternative technological routes replacing dioxide’’ ‘‘calcium carbonat*’’) OR (CO2 micro-alga*) OR (CO2 micro-alga*)
the original product. This study’s assessment of the Paris OR (‘‘carbon dioxide’’ micro-alga*) OR (‘‘carbon dioxide’’ micro-alga*) OR
(CO2 carbon nanotube*) OR (‘‘carbon dioxide’’ carbon nanotube*) OR (CO2
compatibility of CCU was based on the first two benchmarks, carbon nanofib*) OR (‘‘carbon dioxide’’ carbon nanofib*) OR (CO2 enhanced
but the third could shed light on the potential trade-offs between oil recovery) OR (‘‘carbon dioxide’’ enhanced oil recovery) OR (CO2 Fischer-
CCU and other options for replacing fossil-based production, Tropsch synthesis) OR (‘‘carbon dioxide’’ Fischer-Tropsch synthesis)
AND TOPIC = LCA OR life cycle OR life cycle OR "carbon footprint*"
which may change the verdict on CO2 source-CCU options close
OR "climate footprint*’’ OR "environment* impact*" OR "climat* impact*" OR
to the Paris compatibility emission frontier. "GHG balance" OR "greenhouse gas balance" OR "carbon balance" OR
Our findings have implications for climate and innovation pol- "global warming potential" OR "global warming impact*" OR ‘‘global warming
icy. Research funding may currently be allocated to CCU options footprint*’’ OR ‘‘carbon-negative’’ OR ‘‘below zero’’.
On November 30, 2020, this search string led to 1,041 results. After
that are unlikely to be mature in time for the Paris temperature screening these papers for relevance (1) fulfilling our definition of CCU, (2)
limits or that are not able to sufficiently reduce emissions. To determining the GWP and not only LCA endpoints, and (3) including emissions
be in line with the objectives of the Paris Agreement, such fund- from energy use and excluding conference proceedings and reviews and
meta-analyses without original data, 106 studies remained (Note S3). Microal-
ing would have to be redirected to mitigation options consistent
gae biofuel studies were excluded based on the agreement in the most recent
with the Paris Agreement and unlikely to result in carbon lock-in. reviews, meta-analyses, and harmonized LCA studies that emissions were not
CCU encompasses a wide range of technologies with different reduced consistently compared with fossil fuels160–162 or, on average, even
conversion processes, product lifetimes, and substituted prod- doubled.163 For each individual combination of CCU technology and type of
CO2 source (fossil, biogenic, or atmospheric), the most recent study with the
ucts. Therefore, we recommend that decision-makers recognize most complete life cycle inventory was selected. This resulted in 30 studies
this diversity in CCU, base their decisions on the share of emis- (1 on direct use, 15 on fuels and chemicals, 8 on mineral carbonates and con-
sions an individual CCU technology can reduce, and whether struction materials, and 6 on EHR), together covering 44 unique CCU technol-
ogies and resulting in 74 combinations based on multiple CO2 sources. If the
(close to) zero emissions or CDR can be achieved rather than same CCU process was presented with small changes in setup or composi-
treating CCU as a homogeneous technology. In addition, the tion, then the process with the lowest overall GHG emissions was used in
technology’s current level of maturity and when it is expected this study. If several CO2 sources of the same ‘‘type’’ (fossil, biogenic, or atmo-
spheric) were given in the LCA, the source most likely to be deploying CO2
to be ready for diffusion should be considered. Such a focus
capture in a 1.5
C pathway and to still exist in 2030 and 2050 was preferred
could facilitate creation of strategies that accelerate develop- (i.e., an industrial facility over a fossil fuel-based power plant and a natural
ment of technologies with low TRLs that may lead to (close to) gas power plant over a coal-fired power plant). For processes for which a
zero emissions or CDR. pure biogenic source was not available but a source representing a mix of
biogenic and fossil sources was available, the mix was included in addition
to the fossil and atmospheric sources. When the emissions for the substitute
EXPERIMENTAL PROCEDURES were not included in the study, the emissions reported in another LCA for
the same product were used and are referred to in Note S4.
Resource availability
Lead contact Derivation of GHG emissions of CCU products in 2030
For questions related to this article, please contact the lead contact, Kiane de We apply a system expansion via substitution approach to solve the multifunc-
Kleijne ([email protected]). tionality problem following the LCA standard ISO 14044 and LCA guidelines for
Materials availability CCU.104 This method assumes that a primary production plant with CCU
Not applicable to this study. directly substitutes an identical plant without CCU to ultimately determine
Data and code availability the emissions that can be associated with CCU itself. The GHG emissions of
For identification of a Paris-compatible mitigation pathway, we used data these two systems can be determined as shown in Equations 3 and 4:
available from the Integrated Assessment Modeling Consortium (IAMC)
1.5
C Scenario Explorer and Data.1 The full dataset (Data S1) with harmonized Eplant w=o CCU = Eupstream + Eprimary; direct + Eprimary; other (Equation 3)
emissions of CCU technologies for 2030 and 2050 and source data for Figures
4, 5, and S1 have been deposited at Data Archiving and Networked Services Eplant with CCU = Eupstream + Eprimary; other + Ecapture losses + Ecapture process
(DANS) under https://doi.org/10.17026/dans-28h-n6zj. + Econversion + Eother + Ereleased
(Equation 4)
Identification of a Paris-compatible mitigation pathway
We use all ‘‘no-overshoot’’ and ‘‘low-overshoot’’ 1.5
C pathways as defined in where E stands for GHG emissions (in kgCO2-equiv/kg CO2 utilized). All emis-
the IAMC 1.5
C Scenario Explorer and Data1 (version 1.1). We take the mean of sions are scaled to the functional unit of 1 kg of CO2 utilized. We specifically
the global annual emissions in these pathways from 2010–2060 to arrive at the distinguish the following GHG emissions:
Paris-compatible mitigation pathway in Figure 2. ‘‘Half of 2020 emissions’’ in
Figure 2 is found by multiplying the mean 2020 emissions in these pathways Eupstream Upstream GHG emissions associated with extraction of re-
by 0.5. sources or production of the carbon feedstock feeding into the primary

180 One Earth 5, February 18, 2022

 ll
Review
production process (as feedstock and/or fuel), including handling and Assumptions to arrive at harmonized GHG emissions of CCU product
transport to the plant and substitute
Eprimary; direct Direct CO2 emissions emitted at the point source in the pri- To complement the ‘‘Emissions of CCU technologies’’ section and Note S4,
mary production process which includes detailed assumptions according to the LCA study, this section
Eprimary; other Other (remaining) GHG emissions associated with the primary provides details regarding overarching assumptions in harmonization of GHG
production plant emissions of CCU products.
Ecapture losses Emissions of CO2 that are not captured in the capture process For some CCU products, not all carbon in the end product has its origin in
(capture is not 100% efficient) captured CO2. Instead, some processes use fossil methane or methanol as
Ecapture process GHG emissions associated with capturing CO2 and sepa- additional feedstock; for example, in dry reforming of methane, where
rating the CO2 from the bulk gas stream (e.g., from additional elec- (captured) CO2 and methane are used to produce CO and H2.164 This results
tricity use) in emission of additional CO2 besides the Ereleased of 1 kgCO2/kg CO2 utilized
Econversion GHG emissions of the conversion process of the CO2 into the upon combustion of the chemical/fuel; these additional emissions are included
end product in Eother . Conversely, in CO2 EOR, the CO2 utilized to produce the hydrocarbon
Ereleased Emissions of utilized CO2 into the atmosphere at the end of life of does not end up in the product itself but stays behind in the depleted oil field.
the CCU product The CO2 is cycled and used several times in the process; the amount of CO2
Eother Other (remaining) GHG emissions associated with the CCU product, utilized per barrel of oil is taken to be the total amount of CO2 injected in a
such as GHG emissions at end of life other than release of utilized CO2 well over the years of CO2 EOR operation and divided by the total number of
barrels of oil produced. Given that the CO2 utilized is defined as the CO2 stored
The amount of CO2 that is utilized in CCU can be determined as shown in in the well, Ereleased is zero. The combustion of the produced hydrocarbon is
Equation 5: included in Eother .
Several processes produce co-products with the CCU product or with the
Eutilized = Eprimary; direct  Ecapture losses (Equation 5) feedstock, leading to a multifunctionality problem. In ethylene production, pro-
pylene, butene, and hydrogen are co-produced;78 in the electrochemical
reduction process, O2 and H2 are co-produced;107 and for hydrogen produc-
The GHG emissions that can be attributed to the CCU product via substitution
tion via electrolysis, 7.94 kg O2/kg H2 is co-produced. We follow the LCA stan-
can thus be determined via Equations 6a, 6b, 6c:
dard ISO 14044 guidelines and apply the system expansion via substitution
ECCU = Eplant with CCU  Eplant w=o CCU (Equation 6a) approach. In particular, we assume that the production of 1 kg of H2 via elec-
trolysis avoids the production of 7.94 kg of O2 via cryogenic air separation. We
used the production process of O2 using air separation in EcoInvent v.3.6 and
ECCU = Eupstream + Eprimary; other + Ecapture losses + Ecapture process adapted this process to ensure harmonization of the electricity used in
+ Econversion + Eother + Ereleased  Eupstream  Eprimary; direct  Eprimary; other electrolysis and the substituted oxygen production process; we replaced the
(Equation 6b) electricity source for the required 1.42 kWh/kg O2 in the EcoInvent process
by the 2030 and 2050 electricity mix used in the harmonization. In 2030, this
results in an emission reduction factor of 22% for H2 production because of
Solving and filling in Equation 5 then results in Equation 6c: substitution; we multiply the emissions for H2 with a factor of 0.78; in 2050,
with electricity assumed to be emission-free, H2 production has (close to)
ECCU =  Eutilized + Ecapture process + Econversion + Eother + Ereleased (Equation 6c) zero emissions.
For cement-based substitutes and CCU construction materials, we include
the CO2 uptake during the use phase and end-of-life phase, which is not
In the case of DAC, there is no multifunctionality problem, but Equation 6c can included in the analyzed LCAs. Xi et al.67 show that, from 1930 to 2013,
still be used to determine ECCU because Eutilized is simply the amount of CO2 43% of the limestone calcination emissions in cement production were offset
captured from the air. When the CO2 must already be separated in the primary because of atmospheric CO2 absorption in a natural cement carbonation pro-
process, CO2 is a by-product, and the capture emissions (Ecapture process ) cess. Cao et al.68 project that, from 2015 to 2100, 30% of cement production
are zero. emissions are absorbed by cement carbonation, largely in line with Xi et al.,67
Equation 6c is used in the main text as Equation 1. considering that calcination of limestone currently accounts for 58.4% of the
CO2 emissions of cement production.68 To take this uptake of CO2 into ac-
count, we multiply the emissions of cement production by a factor 0.7 to
Derivation of GHG emissions of CCU products in 2050 find the full life cycle emissions, including uptake.
The substitution approach is based on the assumption that a point source In our analysis, we assume that industrial waste as feedstock is impact free.
without capture is 1:1 substituted by the same plant with capture. In the Several processes in the mineral carbonates and construction materials cate-
near future (i.e., 2030) this assumption holds because many plants without gory require input of industrial waste; e.g., steel slag, fly ash, or desalination
capture can still be substituted. In the long run, however, the reference system brines. Although some studies assume that CCU avoids landfilling or process-
is expected to transform toward a zero-emissions economy. Therefore, in a ing of these waste streams, assigning avoided emissions to the CCU product,
Paris-compatible 2050 system, we can no longer assume that there are un- there is no consensus on how much these are (i.e., a factor 4 difference be-
abated fossil point sources to substitute and associated emissions to avoid. tween avoided emissions from slag landfilling of 0.04 kgCO2-equiv/kg
Because emissions are no longer unabated, considering CCU as an option CaCO366 and 0.16 kgCO2-equiv/kg CaCO365). We follow the most regularly
to abate fossil CO2 emissions means that the responsibility for not emitting used and most conservative approach of assuming impact-free waste streams.
shifts to CCU. In terms of calculating the GHG intensity of CCU for a fossil
CO2 source in 2050, this means that all emissions from the stack onward are Lifetimes of CCU products
assigned to the CCU product (Equation 7): We calculated the GHG intensity of CCU products without (base case) and with
the benefit of temporary carbon storage (sensitivity analysis), using a time hori-
ECCUðfossil in 2050Þ = Ecapture losses + Ecapture process + Econversion + Eother + Ereleased zon of 100 years. To include the storage effect, Ereleased in Equations 1 and 2 is
(Equation 7) multiplied by GWPstorage-100, whose value depends on the product-specific
lifetime (Table 2). For direct use of CO2 in an agricultural greenhouse, a lifetime
of less than 6 months is assumed, based on Mazotti et al.129 For EHR, perma-
Equation 7 is used in the main text as Equation 2. nent storage129 or at least millennia11 is assumed. For mineral carbonates and
To calculate Ecapture losses in 2050, a high capture rate of 95% is assumed construction materials, a lifetime of centuries to permanent is assumed, based
based on the finding that such high capture rates would be needed32 and on Hepburn et al.,11 Pan et al.,58 and Sanna et al.,56 except for sodium bicarbon-
are expected to become dominant after 2040122 under stringent decarboniza- ate, which may release CO2 upon use, assuming a lifetime of 6 months. In
tion targets. Furthermore, in achieving a net-zero CO2 system, Wevers et al.81 the fuels and chemicals category, for more stable chemicals (polyethylene, poly-
found that going beyond a 95% capture rate would be energetically unfavor- propylene, and polyols), a lifetime of 50 years is assumed, based on the lifetime
able for deploying DAC for the remaining 5%. of months to decades for polymers11 or decades to centuries for polyure-
In the results, we report ECCU , but when this applies to fossil CO2 sources in thanes.129 For the remainder of fuels and chemicals, a lifetime of 6 months is
2050, Equation 7 is used for the calculation. For CCU processes based on assumed, based on the lifetime of 6 months indicated for methanol and urea
biogenic or atmospheric CO2 in 2050, Equation 6c still applies because the by Mazotti et al.,129 and for methane, Fischer-Tropsch fuels, and DME by Hep-
availability of these sources in 2050 is in line with a Paris-compatible scenario. burn et al.11

One Earth 5, February 18, 2022 181

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