pubs.acs.

org/est Perspective

Deep CCS: Moving Beyond 90% Carbon Dioxide Capture

Matthew N. Dods, Eugene J. Kim, Jeffrey R. Long,* and Simon C. Weston*
Cite This: Environ. Sci. Technol. 2021, 55, 8524−8534 Read Online

ACCESS Metrics & More Article Recommendations *

sı Supporting Information

ABSTRACT: The large-scale deployment of carbon capture

technologies is expected to play a crucial role in efforts to meet
See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

stringent climate targets set forth by the Paris Agreement, but

current models rely heavily upon carbon dioxide removal (CDR)
strategies for which viability at the gigatonne scale is uncertain.
Downloaded via UNIV OF GLASGOW on August 11, 2021 at 16:13:35 (UTC).

While most 1.5 and 2 °C scenarios project rapid decarbonization

of the energy sector facilitated by carbon capture and sequestration
(CCS), they generally assume that CCS units can only capture
∼90% of the CO2 in coal and natural gas combustion flues because
this was previously considered the optimal condition for aqueous
amine scrubbers. In this Perspective, we discuss a small but
growing body of literature that examines the prospect of moving significantly beyond 90% capturea concept we term deep CCS
in light of recent developments in materials and process design. The low incremental costs associated with performing varying
degrees of deep CCS suggest that this approach is not only feasible but may also alleviate burdens placed upon CDR techniques
facing significant barriers to large-scale deployment. We estimate that rapid deployment of deep CCS in deep decarbonization
pathways could avoid more than 1 gigatonne of CO2 globally each year. The principles of deep CCS could also be applied directly to
the CDR strategy of employing bioenergy with CCS, which could lead to a significant alleviation of the land and freshwater burden
associated with this technology.
KEYWORDS: deep decarbonization, capture rate, carbon dioxide removal

1. INTRODUCTION commercially mature technology for capturing CO2 from point

Global anthropogenic CO2 emissions now exceed 40 Gt/yr,1 sources involves absorbing the CO2 into aqueous amine
∼75% of which derive from the combustion of fossil fuels.2 In solutions.20 In many cases, existing coal- and natural gas-fired
power stations can be retrofitted with carbon capture units,
order to keep average surface temperatures well below 2 °C of
and thus it would not be necessary to overhaul or replace all
preindustrial values, as set forth by the Paris Agreement,
existing fossil-fuel burning plants to reap the benefits of CCS.
integrated assessment model (IAM) scenarios (see Supporting
Plants that are retrofitted with carbon capture units may also
Information (SI) Table S1 for a glossary of commonly used
be operated flexibly in response to changes in electrical
terms) have underscored the need for rapid decarbonization of
demand.18,21−24 While 1.5 and 2 °C IAM scenarios have
the power generation sector.3,4 Variable renewable energy
frequently projected that CCS will be instrumental in
technologies are prevalent in these scenarios, although their
minimizing the cost of climate change mitigation,25 commer-
penetration into the global energy portfolio is still limited by
cial deployment of CCS has not yet reached the scale projected
technoeconomic and sociopolitical hurdles.5−12 Principal
by these scenarios. This disparity is due in part to cost overruns
among these obstacles are the costs associated with the
and technical obstacles faced by first-of-a-kind CCS facilities as
construction of infrastructure for renewable electrical gen- well as past limited public and private support. Until now,
eration and the need to balance inflexible supply with time- these factors have restricted the deployment of CCS to <50
varying demand.13−18 Although many 1.5 and 2 °C IAM MtCO2/yr globally, with a large portion of these plants
scenarios project rapid scale-up of variable renewables by performing enhanced oil recovery with the captured CO2.26−32
midcentury,3,19 the growing need to curb anthropogenic CO2 However, the near tripling of large-scale CCS capacity in
emissions has motivated the deployment of alternative low-
carbon technologies in the near-term.
Carbon capture and sequestration (CCS) is one leading Received: November 3, 2020
strategy that has been proposed as a means to substantially Published: June 23, 2021
mitigate CO2 emissions20 and refers to a set of technologies
that capture CO2 directly from the flue exhaust of point
sources (such as fossil-fueled power plants) and store it
underground in geological formations. Currently, the most

© 2021 American Chemical Society https://doi.org/10.1021/acs.est.0c07390

8524 Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

development between 2017 and 2020 suggests that this this purpose.55 Given these biogeophysical and socioeconomic
technology is now entering a new period where large-scale constraints and the uncertain practical potential of afforesta-
commercial deployment will soon be feasible.32 tion/reforestation and BECCS, substantial investigation into
Although CCS can in principle decarbonize a substantial alternatives, such as DACS, is underway in order to satisfy the
portion of the power generation sector, it is unable to mitigate global CDR requirement.37,56 DACS offers some alleviation of
emissions from disperse sources, such as those derived from the land/water burden because it does not require arable land
the transportation and residential sectors. By contrast, or nearly as much water as afforestation/reforestation or
techniques capable of actively removing CO2 from the air BECCS. However, commercial DACS operations are currently
can ameliorate these disperse emissions, and are widely hampered by substantial costs, primarily arising from to the
deployed in deep decarbonization pathways.33−35 These need to regenerate CO2 from strongly binding capture
techniques, collectively referred to as carbon dioxide removal media.50,57−59 The direct air capture company Carbon
(CDR), describe an array of natural and artificial strategies for Engineering recently published a conceptual analysis of its
removing CO2 from ambient air. Currently, the most pilot plant that estimates an overall levelized cost for DACS in
commonly explored CDR strategies for large-scale deployment the range $113−232 per tonne of CO2 captured, with the
include afforestation/reforestation, bioenergy with CCS lower end of this estimate corresponding to designs for which
(BECCS), and direct air capture with sequestration (DACS), low-carbon electricity is available at low cost.60 Although this is
among others.36−41 Briefly, afforestation describes the process a significant improvement upon previous cost estimates for
of planting trees on land where there was not recently forestry, DACS (e.g., $600/tonne of CO2),52,61 it is still more expensive
whereas reforestation describes the planting of trees on than the majority of estimates for conventional point-source
recently deforested land.42−45 BECCS describes the capture CCS technologies (e.g., $36−53/tonneCO2 for coal CCS and
and storage of CO2 produced from the conversion of biomass $48−111/tonneCO2 for natural gas combined cycle CCS).62
or biomass-derived fuels into energy,46−49 and DACS While there are circumstances under which DACS could
encompasses the direct removal and storage of CO2 from become cost-competitive with other decarbonization measures
ambient air via engineered processes.50−53 Although these in the near-term,63,64 most 1.5 and 2 °C IAM scenarios project
techniques are commonly expected to remove >100 Gt of CO2 that fossil CCS will hold a central role in decarbonizing the
cumulatively by the end of the century (Figure 1),4,38,54 their power generation sector in the next few decades.
feasibility for large-scale deployment remains highly uncertain. In these scenarios, decarbonization of the power generation
For BECCS and afforestation/reforestation, this uncertainty is sector is typically only partially achieved with CCS. One
primarily due to concerns over land and freshwater availability fundamental reason is that the capture fractions considered in
at the levels needed for large-scale CDR and the ecological and most designs and IAMs are well below the values of ∼99% and
ethical risks that arise from the dedication of fertile land for ∼99.7% for natural gas combined cycle (NGCC) and
pulverized coal combustion, respectively, that would be needed
to achieve outlet CO2 compositions equal to the ∼410 ppm in
ambient air (commonly referred to as “carbon-zero” or “carbon
neutral” capture fractions). Thus, residual CO2 emissions still
escape fossil fuel-fired units, despite the presence of carbon
capture. Although ∼90% capture is commonly assumed in
designs and models irrespective of plant size or the
composition of the flue gas, it is not necessarily the most
cost-effective capture fraction for these circumstances (Figure
2a).69−72 Recent studies72−75 have demonstrated that pursuing
capture significantly beyond 90% in point-source CCS,
hereafter referred to as deep CCS, may be associated with
only marginal increases in plant capital and operating expense.
In this Perspective, we assess the pursuit of such deeper
capture targets in light of the global carbon budget and
propose that the residual emissions avoided may dramatically
alleviate burdens placed upon CDR techniques. We note that
our discussion hinges upon the assumption that deep CCS
would be implemented only after the successful deployment of
conventional CCS. Our hope is that this article will broadly
motivate scientists and engineers to consider >90% capture in
their investigations of carbon capture materials and process
configurations, and that it will encourage the modeling
community to move beyond the artificial assumption of 90%
in their representations of CCS.

2. TECHNOECONOMIC BENEFITS OF DEEP CCS

Figure 1. Cumulative carbon dioxide removal for 1.5 °C (upper) and Deep CCS may offer an inexpensive route toward deep
2 °C (lower) scenarios. Data are from the Grantham Institute TIMES decarbonization of the fossil-fueled energy sector because it
Integrated Assessment Model in ref 54. Until recently, integrated requires only minor adjustments to conventional (∼90%
assessment modeling of technological CDR other than BECCS has capture) designs. Although the operating expense per tonne of
been uncommon.63−68 CO2 avoided in deep CCS will be larger than in conventional
8525 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

These incremental efficiency losses can indeed be kept small

in aqueous amine scrubbers, for which the operating expense is
dominated by the reboiler duty for solvent regeneration.
Higher capture fractions can be achieved by increasing the
interfacial area of the absorber and by modulating the column
hydrodynamics with increased liquid:gas ratios, although
absorber intercooling can reduce the liquid flow rates needed.
Provided that mass transfer limitations are not prohibitive, the
rich loading is unlikely to vary substantially with capture
fraction, and the reboiler duty will scale with the increased
solvent flow.21,23,78 Rochelle and colleagues recently demon-
strated that 99.1% capture from coal combustion flue can be
accomplished with only a 20% increase in solvent flow rate and
less than 5% increase in the reboiler duty with the advanced
flash stripper design, both relative to 90% capture.74 A recent
modeling study from Jiang et al.73 further demonstrated that
the advanced flash stripper design can enable 99.7% capture
from coal combustion flue gas with an increase in the cost of
CO2 avoided by only $2.6/tonne and an increase in the
levelized cost of electricity by only $8.1/MWh (both relative to
90% capture). Even without extensive thermal integration of
the scrubbing system, capture fractions exceeding 99% can be
achieved with minimal added cost, but thermal degradation of
the amine solutions in the high-temperature stripper remains a
critical concern.79−81
Many of the amine solvents that have shown promise for
fossil CCS are thermodynamically capable of capturing CO2 at
compositions well below 410 ppm. However, mass transfer
limitations arising from these ultradilute CO2 compositions
mandate large absorption interfacial areas with associated
capital expense, imposing a practical upper limit on the capture
Figure 2. (a) In conventional CCS, typically only ∼90% of the CO2 fraction. In the same study referenced above from Jiang et al.,73
from the power plant exhaust is captured. (b) The outlet CO2 the authors found that approximately half of the absorber
composition resulting from DACS must necessarily be less than the column is needed to achieve just 3.2% of the overall CO2
inlet composition (∼410 ppm of CO2). (c) With deep CCS, it is capture. In scrubbers treating NGCC flue gas, which is more
possible to achieve an outlet composition of <410 ppm of CO2. dilute in CO2 than coal flue gas, the interfacial areas needed to
However, note that there may be circumstances where it is more achieve a 410 ppm outlet may become unfeasibly large and
feasible to pursue outlet compositions ≥410 ppm in deep CCS. may dominate the incremental capital expense. Considering
Because deep CCS generally describes capture significantly beyond that many 1.5 and 2 °C IAM scenarios project that NGCC
90%, it can yield carbon positive, carbon negative, or net carbon zero/
with CCS will occupy a substantial portion of the global energy
carbon neutral outlets.
portfolio in 2100,19 efforts should be directed toward the
development and testing of materials capable of performing
CCS due to the need to overcome incremental kinetic and low-cost deep CCS from NGCC flues.82
thermodynamic limitations, the increase in minimum separa- The superior diffusional kinetics and high volumetric
tion work per mole of CO2 captured upon moving from 90% capacities of porous adsorbents make them excellent
to ∼100% capture is relatively small, namely ∼0.48 and ∼0.57 candidates in this context, as the overall land footprint of
kJ/molCO2 for pulverized coal combustion and NGCC, deep CCS units utilizing these materials can be kept fairly
respectively (all calculations are performed at a temperature small.20 Modular designs may also be possible, wherein
of 25 °C; for more details, see SI Section 2). The energetic conventional (i.e., ∼ 90% capture) contactors can be appended
palatability of deep CCS arises from the logarithmic depend- with deeper capture units in a multistage configuration that
ence of the minimum separation work on the composition of alleviates some of the financial risk in adopting deep CCS.
the inlet stream (SI Figure S2), which is ∼11−15% CO2 for Indeed, these deeper capture units could be financed by
coal and ∼4−6% for NGCC flues. By contrast, the energy incentives and regulatory frameworks aimed at residual
needed to compress the additional ∼10% of CO2 scales linearly emissions reductions at a later time. Such an approach might
with the amount of CO2 captured (provided that the purity of enable a reduction in incremental capital and operating
the desorbed stream is unchanged upon moving from 90% to expenses, given that smaller contactors could be used for the
∼100% capture), and is only ∼12 kJ/molCO2. Although higher concentration separation upstream and thermodynamic
entropic irreversibilities prohibit practical attainment of these tuning of the stages could be optimized to minimize heat
thermodynamic minima for separation and compression,76,77 transfer inefficiencies. The immense diversity of amine-
this simple calculation demonstrates that the operating expense functionalized adsorbents renders them particularly well suited
for deep CCS may closely approach that for conventional CCS for this application, because the capture material (and hence
if incremental efficiency losses can be minimized upon the Gibbs energy of adsorption) can be varied at different
exceeding ∼90% capture. stages to achieve the desired capture fraction, assuming kinetic
8526 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

limitations are not governing.83−85 In particular, amine- capture, and thus while it is commonly thought that fossil CCS
appended metal−organic frameworks exhibiting cooperative is at best carbon neutral (∼410 ppm outlet), there is no
adsorption could enable precise control over the adsorption fundamental reason why a deep CCS exhaust cannot be carbon
enthalpies in each stage, which may lead to considerable negative with respect to the inlet air supply (Figure 2c).
energy savings for the overall unit, especially if direct-contact However, even for a ∼ 0 ppm of CO2 deep CCS outlet, the
steam stripping is used for regeneration.86−90 Research into negative emissions achieved inside the plant boundaries (which
these adsorbents is only now emerging, and will benefit from we define as starting at the point of fuel combustion and
the development of new models and technoeconomic analyses ending at the exhaust of the CO2 capture unit) will be small
to establish realistic cost and energy considerations that will compared to the current and anticipated lifecycle emission
guide their development for deep CCS. For additional rates for the coal and natural gas supply chains in the United
discussion of potential sorbent materials and process States (SI Section 7). As such, deep CCS should not be viewed
configurations for deep CCS, see SI Section 3. as a CDR technique, but the pursuit of sub-410 ppm outlet
Given that deep CCS will produce outlet streams with CO2 compositions can still offset a portion of the upstream
concentrations similar to that in ambient air, the deployment emissions and is warranted if the incremental cost can be
of materials and process configurations in deep CCS may kept low. Because the proportion of CO2 in NGCC flue
synergistically inform cost reductions for DACS through streams is smaller than that in coal flue gas, it may be more
technological learning.27,91,92 We anticipate that for suitable suitable to target these sub-410 ppm levels in NGCC
coal and NGCC units, the cost of implementing deep CCS will combustors (SI Section 6). With regards to process design,
be lower than that for DACS for a number of reasons. For the weak mass-transfer driving forces associated with capturing
example, unless wind currents can be harnessed effectively,93 CO2 from sub-410 ppm streams will likely require use of
DACS requires pressurization of the inlet air with the aid of capture media with rapid diffusional kinetics (e.g., certain
large fans operating with low-carbon electricity (Figure 2b). In porous adsorbents).72
the ∼1 MtCO2/yr design from Carbon Engineering, 61 kWh/ BECCS is one proposed strategy where lifecycle negative
tonne CO2 of electricity is needed to support an air velocity of
emissions can theoretically be achieved, and which may
1.4 m/s in a fan with inlet area of 45 000 m2.60 In contrast,
additionally benefit from the pursuit of deeper capture targets.
deep CCS does not require sizable fans, because it draws
The extent of negative emissions achievable in BECCS is
directly from a pressurized flue. Another requirement for direct
intertwined with direct/indirect land use changes and the
air capture plants is that they operate at ambient temperature,
given the impracticality of heating large quantities of ambient carbon footprint of the biomass.99−106 Achieving deeper
air. Therefore, for a temperature-swing process, large amounts capture targets in the BECCS unit could synergistically reduce
of sensible heat would be required to regenerate the sorbents, the amount of biomass that must be processed upstream to
which typically have large heat capacities and/or low thermal achieve a fixed negative emission rate, albeit at some reduction
conductivities. On the other hand, the temperature of a deep in energy efficiency due to the need to overcome the increased
CCS inlet can be controlled with direct contact coolers that are parasitic load.48,107 Consider the direct firing of European
already employed commercially. The above-ambient sorption Miscanthus as a representative energy-dedicated crop. In order
temperatures that could be utilized in deep CCS would require to remove 1 MtCO2 equivalents per year (MtCO2e/yr) on a
less sensible heat relative to DACS and may also enable a stark lifecycle basis, we estimate that achieving a 99.5% capture
reduction in water coadsorption in solids, due to the fraction with deep BECCS requires 3900 fewer hectares of
exponential dependence of relative humidity on temper- arable land relative to 90% capture (a savings of ∼10%),
ature.94,95 without taking into account land use changes that could further
We note that DACS also offers advantages that are otherwise magnify these reductions (see SI Section 4). Additionally, since
inaccessible with deep CCS. For example, direct air capture the freshwater demand for BECCS is expected to be
can ameliorate legacy emissions from unmitigated fossil fuel dominated by losses due to evapotranspiration during biomass
combustion. Additionally, DACS operations are inherently cultivation, the transition from 90% to 99.5% capture could
more flexible in their geographical placement than CCS save more than 15 MtH2O/yr, or ∼10% of the freshwater
technologies, and as such the cost of transporting and storing needed for 90% capture. Although the additional parasitic load
CO2 may be lower for DACS than for CCS operations. incurred in achieving this deeper capture target would decrease
Additionally, direct air capture does not require pretreatment electrical production, this inefficiency is ameliorated in part by
of the incoming air to protect the capture media from toxic the embodied energy saved in consuming less biomass. The
gases (e.g., SOx and NOx), which can be particularly incremental parasitic load associated with deep BECCS is
problematic for coal capture units.96,97 Although these expected to decrease over time with the development of new
economic benefits are unlikely to surmount the intrinsic cost technology, bringing the lifecycle energy efficiency of deep
differential between DACS and deep CCS, there are scenarios BECCS closer to that for conventional BECCS. Co-generation
where the large-scale deployment of DACS may be justified in of bioenergy with a low-carbon fuel, such as natural gas, may
the near-term.63,64,98 An improved understanding of all factors close this efficiency gap without substantially reducing the
influencing deployment of DACS relative to deep CCS is direly lifecycle carbon negativity.108,109 Ultimately, the calculations
needed in conjunction with research into materials and process described here are order-of-magnitude estimates obtained
configurations devoted to each approach. using the average multiplicative factors detailed in SI Section 4,
and are intended to motivate further research into deep
3. THE PROSPECT OF NEGATIVE EMISSIONS BECCS. Detailed investigations of the technoeconomics and
Conservation of mass requires that the CO2 composition of a food−energy−water implications of deep BECCS are needed
DACS outlet be less than the inlet air composition. DACS and in order to more accurately assess the practical potential of this
deep CCS both obey the same thermodynamic limit of 100% concept.
8527 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

4. THE POTENTIAL FOR DEEP IMPACT considerations and improved parametrizations of CCS
technoeconomic models to account for deep capture
All of the IAM scenarios featured in the 27th Energy Modeling
targets.22,129
Forum required cumulative sequestration of at least 600
As discussed above, although deep CCS can achieve negative
GtCO2 by 2100 to meet 2 °C warming targets, but to the best
emissions inside the plant boundaries, these removals are likely
of our knowledge, none of these scenarios considered capture
to be outweighed by supply chain emissions upstream that are
fractions significantly beyond 90% during peak deployment, or
bounded by extraction, transportation, and processing of the
the period of time during which the maximum number of
fuel. These supply chain emissions include fugitive (uninten-
plants are outfitted with fossil CCS.20,110−118 Indeed, while tional) and vented (intentional) emissions from coal mines,
90% capture is not a strict limit in IAMs, it is frequently natural gas reservoirs, pipelines, railcars, ships, and process
informed by technoeconomic assessments developed for first- equipment.130−135 However, the increment between 90 and
generation CCS designs.70,71 Given the stringent carbon ∼100% capture can be carbon negative if supply chain
budgets of 1.5 °C scenarios, the residual emissions from emissions can be kept small. Even if this increment is not
conventional fossil CCS units could necessitate an accelerated carbon negative, it could still alleviate dependences on some of
transition to renewables or other technologies with lower the least viable CDR strategies projected by current 90%
lifecycle emissions.19,25,119,120 Alternatively, the rapid develop- model scenarios, so long as the residual emissions captured
ment and commercialization of deep CCS may provide a exceed the supply chain emissions (Figure 3). Working with
smoother transition toward renewables and, by minimizing
residual emissions from the fossil-fueled power generation
sector, may obviate a substantial amount of CDR over the
century.35,121
Working with published results from the IAM MESSAGE
GLOBIOM,122 we estimate that replacing existing fossil CCS
units with deep CCS units worldwide could avoid an additional
∼1.8 GtCO2/yr in the 2 °C scenario at peak deployment. In
the 1.5 °C scenario, which projects lower overall deployment
of CCS, the CO2 avoided is reduced to only ∼770 Mt/yr (SI
Section 5). However, if cost reductions over the next ∼40 years
can enable the implementation of deep CCS in existing coal
and NGCC units for which conventional CCS is currently
considered uneconomical, the impact of deep CCS in the 1.5
°C scenario can be significantly augmented. Indeed, if deep
CCS is ultimately recognized as a technique for reducing the
need for CDR, the number of coal and NGCC plants deemed
suitable for CCS may exceed current projections. We
emphasize that deep CCS should not be regarded as a
replacement for CDR, because there are circumstances where
CDR can provide economic, social, and/or environmental
benefits that are otherwise inaccessible with deep
CCS.36,53,123−125 However, in some cases, deep CCS has the
potential to serve as a viable and cost-effective alternative to
replace certain CDR strategies that currently face significant Figure 3. We estimate that deep CCS can avoid ∼1 GtCO2/yr of
technical or economic hurdles. Note that the above analysis residual emissions globally, which translates to 80 Mha of forest (with
represents at best an order-of-magnitude estimate of the a mean carbon uptake of 3.4 tCeq/ha/yr), 2.7 Mha of land for
terrestrial enhanced weathering (assuming a potential of 0.1 GtCeq/
impact of deep CCS in these particular scenarios, and
yr/Mha), 32 Mha of cropland for BECCS with an energy-dedicated
ultimately, the detailed incorporation of deep CCS into IAM crop (assuming a mean carbon uptake of 8.6 t Ceq/ha/yr), or 1000
frameworks will be needed in order to determine the DACS plants (assuming a net CDR rate of 1 MtCO2/yr per
circumstances under which CDR can truly be avoided by plant).56,60,140
deep CCS.126
In an initial evaluation of potential emissions avoided from lower bound emission factors of 12.4 kgCO2e/MWh (derived
retrofitting coal and NGCC fleets with deep CCS, we focused in SI Section 7) and 3.6 gCO2e/MJ for the coal136 and natural
on plants in the United States, which in 2017 generated 14.5% gas137 supply chains, respectively, we find that the incremental
of global combustion CO2 emissions.2 Working with 2018 data carbon intensity for a 100 ppm deep CCS outlet is −1.3
from the Energy Information Administration,127,128 we MtCO2e/yr (coal) and −2.3 MtCO2e/yr (NGCC) for the
identified plants potentially suitable for deep CCS retrofit by plants considered for retrofit in the United States. In
categorizing operational coal and NGCC units by electrical comparison, one of the DACS designs from Carbon Engineer-
production and age. Assuming conservative fuel-based parasitic ing requires 8.81 GJ of natural gas per tonne of CO2
loads of 13% for NGCC and 21% for coal,62 we estimate that a captured,60 and our calculations show that the associated
combined total of 128 MtCO 2 /yr of emissions can supply chain emissions reduce the effective CDR rate from 966
theoretically be avoided. Due to the assumptions made in to 931 ktCO2/yr, again assuming the emission factor of 3.6
this analysis (see SI Section 6), this calculation should be gCO2e/MJ from ref 137.137 Given that the net carbon
regarded as an order-of-magnitude estimate of impact. More intensities of deep CCS and DACS are expected to be highly
accurate assessments can be achieved with plant-specific sensitive to upstream emissions, it will be imperative to reduce
8528 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

these emissions to maximize the overall impact of both Author Contributions

technologies.71,138,139 All authors have given approval to the final version of the
manuscript.
5. OUTLOOK
Notes
Targeting CO2 capture fractions significantly beyond 90% is
The authors declare the following competing financial
technoeconomically feasible and could reduce the need for
interest(s): J.R.L. has a financial interest in and serves on the
large amounts of costly or unfeasible CDR if implemented at
scale in the near term. The technological learning gained from board of directors of Mosaic Materials, a start-up company
commercializing deep CCS could synergistically inform working to commercialize metal-organic frameworks for gas
designs for DACS and deep BECCS, alleviating some of the separations.
uncertainty in accessing large-scale technological CDR. We Biographies
note that the principles of deep CCS can be extended in some
cases (e.g., iron and steel manufacturing) to the industrial
sector, which in 2017 was responsible for 24% of global
combustion CO2 emissions.2,141−146 Additionally, we highly
encourage reparametrization of IAMs to more thoroughly
investigate the potential of deep CCS/deep BECCS for various
socioeconomic and technological assumptions, particularly
given that the artificial assumption of ∼90% capture may
necessitate a shift to suboptimal power generation mixes in
deep decarbonization pathways.25,98 Although materials
capable of performing deep CCS already exist, continued
improvements in process efficiency are warranted to bring the
intrinsic costs of deep CCS even closer to those of
conventional CCS, especially as natural gas continues to
occupy a larger portion of the global energy portfolio.82,147
Although the incremental costs associated with performing Jeffrey R. Long is a Professor of Chemistry and Chemical &
deep CCS can be kept low relative to the base cost of Biomolecular Engineering at the University of California, Berkeley
conventional CCS, widespread deployment of deep CCS will and a Faculty Senior Scientist in the Materials Sciences Division at
be predicated on the successful implementation of conven- Lawrence Berkeley National Laboratory. His research involves the
tional CCS.

■
synthesis and physical characterization of new materials with potential
applications in sustainable energy and environmental remediation,
ASSOCIATED CONTENT and his 360 publications have received more than 76 000 citations. He
*
sı Supporting Information
cofounded and directs the start-up company Mosaic Materials, which
The Supporting Information is available free of charge at is developing metal−organic frameworks for low-energy carbon
https://pubs.acs.org/doi/10.1021/acs.est.0c07390. dioxide separations, with particular focus on its direct removal from
Computational details and additional information air.
(PDF)

■ AUTHOR INFORMATION
Corresponding Authors
Jeffrey R. Long − Department of Chemical and Biomolecular
Engineering and Department of Chemistry, University of
California, Berkeley, California 94720, United States;
Materials Sciences Division, Lawrence Berkeley National
Laboratory, Berkeley, California 94720, United States;
orcid.org/0000-0002-5324-1321; Email: jrlong@
berkeley.edu
Simon C. Weston − Corporate Strategic Research,
ExxonMobil Research and Engineering Company,
Annandale, New Jersey 08801, United States; orcid.org/
0000-0002-7439-5055; Email: simon.c.weston@
Simon Weston is a Senior Research Associate at the Corporate
exxonmobil.com
Strategic Research Laboratories of ExxonMobil Research and
Authors Engineering and dedicated to creating new materials for application
Matthew N. Dods − Department of Chemical and in molecular separations, storage and catalysis. Although originally
Biomolecular Engineering, University of California, Berkeley, trained as an organic chemist, he has a multidisciplinary background
California 94720, United States in coordination chemistry, inorganic chemistry, high throughput
Eugene J. Kim − Department of Chemistry, University of experimentation, informatics, and CO2 capture research. He has led
California, Berkeley, California 94720, United States several research teams bridging industrial and academic work with a
Complete contact information is available at: focus on how scientific fundamentals can lead us to better materials
https://pubs.acs.org/10.1021/acs.est.0c07390 for a given application.

8529 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology

■
pubs.acs.org/est Perspective

ACKNOWLEDGMENTS Informed by Weather Regimes. Nat. Clim. Change 2017, 7 (8), 557−
562.
We acknowledge ExxonMobil Research and Engineering (16) Pfenninger, S.; Gauché, P.; Lilliestam, J.; Damerau, K.; Wagner,
Company for financial support of this work. We gratefully F.; Patt, A. Potential for Concentrating Solar Power to Provide
acknowledge George Walchuk, Dr. Haroon Kheshgi, and Dr. Baseload and Dispatchable Power. Nat. Clim. Change 2014, 4 (8),
Bryan Mignone of ExxonMobil Research and Engineering 689−692.
Company for helpful discussions, and Dr. Katie Meihaus for (17) Rodríguez, R. A.; Becker, S.; Andresen, G. B.; Heide, D.;
editorial assistance. Greiner, M. Transmission Needs across a Fully Renewable European

■
Power System. Renewable Energy 2014, 63, 467−476.
(18) Van Den Broek, M.; Berghout, N.; Rubin, E. S. The Potential of
REFERENCES Renewables versus Natural Gas with CO2 Capture and Storage for
(1) Friedlingstein, P.; Jones, M. W.; O’Sullivan, M.; Andrew, R. M.; Power Generation under CO2 Constraints. Renewable Sustainable
Hauck, J.; Peters, G. P.; Peters, W.; Pongratz, J.; Sitch, S.; Le Quéré, Energy Rev. 2015, 49, 1296−1322.
C.; Bakker, D. C. E.; Canadell, J. G.; Ciais, P.; Jackson, R. B.; Anthoni, (19) Rogelj, J.; Popp, A.; Calvin, K. V.; Luderer, G.; Emmerling, J.;
P.; Barbero, L.; Bastos, A.; Bastrikov, V.; Becker, M.; Bopp, L.; Gernaat, D.; Fujimori, S.; Strefler, J.; Hasegawa, T.; Marangoni, G.;
Buitenhuis, E.; Chandra, N.; Chevallier, F.; Chini, L. P.; Currie, K. I.; Krey, V.; Kriegler, E.; Riahi, K.; Van Vuuren, D. P.; Doelman, J.;
Feely, R. A.; Gehlen, M.; Gilfillan, D.; Gkritzalis, T.; Goll, D. S.; Drouet, L.; Edmonds, J.; Fricko, O.; Harmsen, M.; Havlík, P.;
Gruber, N.; Gutekunst, S.; Harris, I.; Haverd, V.; Houghton, R. A.; Humpenöder, F.; Stehfest, E.; Tavoni, M. Scenarios towards Limiting
Hurtt, G.; Ilyina, T.; Jain, A. K.; Joetzjer, E.; Kaplan, J. O.; Kato, E.; Global Mean Temperature Increase below 1.5 °C. Nat. Clim. Change
Goldewijk, K. K.; Korsbakken, J. I.; Landschützer, P.; Lauvset, S. K.; 2018, 8 (4), 325−332.
Lefèvre, N.; Lenton, A.; Lienert, S.; Lombardozzi, D.; Marland, G.; (20) Bui, M.; Adjiman, C. S.; Bardow, A.; Anthony, E. J.; Boston, A.;
McGuire, P. C.; Melton, J. R.; Metzl, N.; Munro, D. R.; Nabel, J. E. Brown, S.; Fennell, P. S.; Fuss, S.; Galindo, A.; Hackett, L. A.; Hallett,
M. S.; Nakaoka, S. I.; Neill, C.; Omar, A. M.; Ono, T.; Peregon, A.; J. P.; Herzog, H. J.; Jackson, G.; Kemper, J.; Krevor, S.; Maitland, G.
Pierrot, D.; Poulter, B.; Rehder, G.; Resplandy, L.; Robertson, E.; C.; Matuszewski, M.; Metcalfe, I. S.; Petit, C.; Puxty, G.; Reimer, J.;
Rödenbeck, C.; Séférian, R.; Schwinger, J.; Smith, N.; Tans, P. P.; Reiner, D. M.; Rubin, E. S.; Scott, S. A.; Shah, N.; Smit, B.; Trusler, J.
Tian, H.; Tilbrook, B.; Tubiello, F. N.; Van Der Werf, G. R.; P. M.; Webley, P.; Wilcox, J.; Mac Dowell, N. Carbon Capture and
Wiltshire, A. J.; Zaehle, S. Global Carbon Budget 2019. Earth Syst. Sci. Storage (CCS): The Way Forward. Energy Environ. Sci. 2018, 11 (5),
Data 2019, 11 (4), 1783−1838. 1062−1176.
(2) International Energy Agency. CO2 Emissions from Fuel (21) Bui, M.; Tait, P.; Lucquiaud, M.; Mac Dowell, N. Dynamic
Combustion 2011; 1−92. DOI: 10.1670/96-03N. Operation and Modelling of Amine-Based CO2 Capture at Pilot Scale.
(3) Intergovernmental Panel on Climate Change. Fifth Assessment Int. J. Greenhouse Gas Control 2018, 79 (August), 134−153.
Report, 2014; DOI: 10.1017/cbo9781107415416. (22) Zhai, H.; Ou, Y.; Rubin, E. S. Opportunities for Decarbonizing
(4) Intergovernmental Panel on Climate Change. Special Report: Existing U.S. Coal-Fired Power Plants via CO2 Capture, Utilization
Global Warming of 1.5 °C, 2018. and Storage. Environ. Sci. Technol. 2015, 49 (13), 7571−7579.
(5) Clack, C. T. M.; Qvist, S. A.; Apt, J.; Bazilian, M.; Brandt, A. R.; (23) Flø, N. E.; Kvamsdal, H. M.; Hillestad, M. Dynamic Simulation
Caldeira, K.; Davis, S. J.; Diakov, V.; Handschy, M. A.; Hines, P. D. of Post-Combustion CO2 Capture for Flexible Operation of the
H.; Jaramillo, P.; Kammen, D. M.; Long, J. C. S.; Morgan, M. G.; Brindisi Pilot Plant. Int. J. Greenhouse Gas Control 2016, 48, 204−215.
Reed, A.; Sivaram, V.; Sweeney, J.; Tynan, G. R.; Victor, D. G.; (24) Rua, J.; Bui, M.; Nord, L. O.; Mac Dowell, N. Does CCS
Weyant, J. P.; Whitacre, J. F. Evaluation of a Proposal for Reliable Reduce Power Generation Flexibility? A Dynamic Study of Combined
Low-Cost Grid Power with 100% Wind, Water, and Solar. Proc. Natl. Cycles with Post-Combustion CO2 Capture. Int. J. Greenhouse Gas
Acad. Sci. U. S. A. 2017, 114 (26), 6722−6727. Control 2020, 95, 102984.
(6) Narayanan, A.; Mets, K.; Strobbe, M.; Develder, C. Feasibility of (25) Budinis, S.; Krevor, S.; Mac Dowell, N.; Brandon, N.; Hawkes,
100% Renewable Energy-Based Electricity Production for Cities with A. An Assessment of CCS Costs, Barriers and Potential. Energy
Storage and Flexibility. Renewable Energy 2019, 134, 698−709. Strateg. Rev. 2018, 22 (January), 61−81.
(7) Hansen, K.; Breyer, C.; Lund, H. Status and Perspectives on (26) Mantripragada, H. C.; Zhai, H.; Rubin, E. S. Boundary Dam or
100% Renewable Energy Systems. Energy 2019, 175, 471−480. Petra Nova - Which Is a Better Model for CCS Energy Supply? Int. J.
(8) Esteban, M.; Portugal-Pereira, J.; Mclellan, B. C.; Bricker, J.; Greenhouse Gas Control 2019, 82, 59−68.
Farzaneh, H.; Djalilova, N.; Ishihara, K. N.; Takagi, H.; Roeber, V. (27) Reiner, D. M. Learning through a Portfolio of Carbon Capture
100% Renewable Energy System in Japan: Smoothening and Ancillary and Storage Demonstration Projects. Nat. Energy 2016, 1 (1), 1−7.
Services. Appl. Energy 2018, 224 (April), 698−707. (28) Kapetaki, Z.; Scowcroft, J. Overview of Carbon Capture and
(9) Djørup, S.; Thellufsen, J. Z.; Sorknæs, P. The Electricity Market Storage (CCS) Demonstration Project Business Models: Risks and
in a Renewable Energy System. Energy 2018, 162, 148−157. Enablers on the Two Sides of the Atlantic. Energy Procedia 2017, 114
(10) Sgouridis, S.; Csala, D.; Bardi, U. The Sower’s Way: (November 2016), 6623−6630.
Quantifying the Narrowing Net-Energy Pathways to a Global Energy (29) Peck, W. D.; Ayash, S. C.; Klapperich, R. J.; Gorecki, C. D. The
Transition. Environ. Res. Lett. 2016, 11 (9). 094009. North Dakota Integrated Carbon Storage Complex Feasibility Study.
(11) Edenhofer, O.; Hirth, L.; Knopf, B.; Pahle, M.; Schlömer, S.; Int. J. Greenhouse Gas Control 2019, 84, 47−53.
Schmid, E.; Ueckerdt, F. On the Economics of Renewable Energy (30) Dai, Z.; Middleton, R.; Viswanathan, H.; Fessenden-Rahn, J.;
Sources. Energy Econ. 2013, 40, S12−S23. Bauman, J.; Pawar, R.; Lee, S. Y.; McPherson, B. An Integrated
(12) Larsson, S.; Fantazzini, D.; Davidsson, S.; Kullander, S.; Höök, Framework for Optimizing CO2 Sequestration and Enhanced Oil
M. Reviewing Electricity Production Cost Assessments. Renewable Recovery. Environ. Sci. Technol. Lett. 2014, 1 (1), 49−54.
Sustainable Energy Rev. 2014, 30, 170−183. (31) ExxonMobil 2021 Energy & Carbon Summary, 2021.
(13) Heuberger, C. F.; Mac Dowell, N. Real-World Challenges with (32) Global Status of CCS 2020. Global CCS Institute 2020.
a Rapid Transition to 100% Renewable Power Systems. Joule 2018, 2 (33) Gasser, T.; Guivarch, C.; Tachiiri, K.; Jones, C. D.; Ciais, P.
(3), 367−370. Negative Emissions Physically Needed to Keep Global Warming
(14) Bistline, J. E. Economic and Technical Challenges of Flexible below 2°C. Nat. Commun. 2015, 6. DOI: 10.1038/ncomms8958.
Operations under Large-Scale Variable Renewable Deployment. (34) Hilaire, J.; Minx, J. C.; Callaghan, M. W.; Edmonds, J.; Luderer,
Energy Econ. 2017, 64, 363−372. G.; Nemet, G. F.; Rogelj, J.; del Mar Zamora, M. Negative Emissions
(15) Grams, C. M.; Beerli, R.; Pfenninger, S.; Staffell, I.; Wernli, H. and International Climate GoalsLearning from and about
Balancing Europe’s Wind-Power Output through Spatial Deployment Mitigation Scenarios. Clim. Change 2019, 157 (2), 189−219.

8530 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

(35) Rogelj, J.; Luderer, G.; Pietzcker, R. C.; Kriegler, E.; Schaeffer, (53) Wilcox, J.; Psarras, P. C.; Liguori, S. Assessment of Reasonable
M.; Krey, V.; Riahi, K. Energy System Transformations for Limiting Opportunities for Direct Air Capture. Environ. Res. Lett. 2017, 12 (6).
End-of-Century Warming to below 1.5 °C. Nat. Clim. Change 2015, 5 065001.
(6), 519−527. (54) Realmonte, G.; Drouet, L.; Gambhir, A.; Glynn, J.; Köberle, A.
(36) Beerling, D. J.; Kantzas, E. P.; Lomas, M. R.; Wade, P.; Eufrasio, C.; Tavoni, M.; Hawkes, A. An Inter-Model Assessment of the Role of
R. M.; Renforth, P.; Sarkar, B.; Andrews, M. G.; James, R. H.; Pearce, Direct Air Capture in Deep Mitigation Pathways. Nat. Commun. 2019,
C. R.; Mercure, J. F.; Pollitt, H.; Holden, P. B.; Edwards, N. R.; 10 (No. 2019), 1−12.
Khanna, M.; Koh, L.; Quegan, S.; Pidgeon, N. F.; Janssens, I. A.; (55) Heck, V.; Gerten, D.; Lucht, W.; Popp, A. Biomass-Based
Hansen, J.; Banwart, S. A. Potential for Large-Scale CO2 Removal via Negative Emissions Difficult to Reconcile with Planetary Boundaries.
Enhanced Rock Weathering with Croplands. Nature 2020, 583 Nat. Clim. Change 2018, 8 (2), 151−155.
(7815), 242−248. (56) Smith, P.; Davis, S. J.; Creutzig, F.; Fuss, S.; Minx, J.; Gabrielle,
(37) Fuss, S.; Lamb, W. F.; Callaghan, M. W.; Hilaire, J.; Creutzig, B.; Kato, E.; Jackson, R. B.; Cowie, A.; Kriegler, E.; Van Vuuren, D. P.;
F.; Amann, T.; Beringer, T.; De Oliveira Garcia, W.; Hartmann, J.; Rogelj, J.; Ciais, P.; Milne, J.; Canadell, J. G.; McCollum, D.; Peters,
G.; Andrew, R.; Krey, V.; Shrestha, G.; Friedlingstein, P.; Gasser, T.;
Khanna, T.; Luderer, G.; Nemet, G. F.; Rogelj, J.; Smith, P.; Vicente,
Grübler, A.; Heidug, W. K.; Jonas, M.; Jones, C. D.; Kraxner, F.;
J. V.; Wilcox, J.; Del Mar Zamora Dominguez, M.; Minx, J. C.
Littleton, E.; Lowe, J.; Moreira, J. R.; Nakicenovic, N.; Obersteiner,
Negative Emissions - Part 2: Costs, Potentials and Side Effects.
M.; Patwardhan, A.; Rogner, M.; Rubin, E.; Sharifi, A.; Torvanger, A.;
Environ. Res. Lett. 2018, 13 (6). 063002. Yamagata, Y.; Edmonds, J.; Yongsung, C. Biophysical and Economic
(38) Dowling, D. A.; Venki, R. Greenhouse Gas Removal. Report by Limits to Negative CO2 Emissions. Nat. Clim. Change 2016, 6 (1),
the UK Royal Society and Royal Academy of Engineering, 2018. 42−50.
(39) Woolf, D.; Lehmann, J.; Lee, D. R. Optimal Bioenergy Power (57) Shi, X.; Xiao, H.; Azarabadi, H.; Song, J.; Wu, X.; Chen, X.;
Generation for Climate Change Mitigation with or without Carbon Lackner, K. S. Sorbents for the Direct Capture of CO2 from Ambient
Sequestration. Nat. Commun. 2016, 7, 1−11. Air. Angew. Chem., Int. Ed. 2020, 59 (18), 6984−7006.
(40) Smith, P. Soil Carbon Sequestration and Biochar as Negative (58) Creutzig, F.; Breyer, C.; Hilaire, J.; Minx, J.; Peters, G. P.;
Emission Technologies. Glob. Chang. Biol. 2016, 22 (3), 1315−1324. Socolow, R. The Mutual Dependence of Negative Emission
(41) Negative Emissions Technologies and Reliable Sequestration; The Technologies and Energy Systems. Energy Environ. Sci. 2019, 12
National Academies Press, 2019; DOI: 10.17226/25259. (6), 1805−1817.
(42) Busch, J.; Engelmann, J.; Cook-Patton, S. C.; Griscom, B. W.; (59) Babacan, O.; De Causmaecker, S.; Gambhir, A.; Fajardy, M.;
Kroeger, T.; Possingham, H.; Shyamsundar, P. Potential for Low-Cost Rutherford, A. W.; Fantuzzi, A.; Nelson, J. Assessing the Feasibility of
Carbon Dioxide Removal through Tropical Reforestation. Nat. Clim. Carbon Dioxide Mitigation Options in Terms of Energy Usage. Nat.
Change 2019, 9 (6), 463−466. Energy 2020. 5720.
(43) Nave, L. E.; Walters, B. F.; Hofmeister, K. L.; Perry, C. H.; (60) Keith, D. W.; Holmes, G.; St. Angelo, D.; Heidel, K. A Process
Mishra, U.; Domke, G. M.; Swanston, C. W. The Role of for Capturing CO2 from the Atmosphere. Joule 2018, 2, 1573−1594.
Reforestation in Carbon Sequestration. New For. 2019, 50 (1), (61) House, K. Z.; Baclig, A. C.; Ranjan, M.; Van Nierop, E. A.;
115−137. Wilcox, J.; Herzog, H. J. Economic and Energetic Analysis of
(44) Alkama, R.; Cescatti, A. Climate Change: Biophysical Climate Capturing CO2 from Ambient Air. Proc. Natl. Acad. Sci. U. S. A. 2011,
Impacts of Recent Changes in Global Forest Cover. Science 2016, 351 108 (51), 20428−20433.
(6273), 600−604. (62) Rubin, E. S.; Davison, J. E.; Herzog, H. J. The Cost of CO2
(45) Doelman, J. C.; Stehfest, E.; van Vuuren, D. P.; Tabeau, A.; Capture and Storage. Int. J. Greenhouse Gas Control 2015, 40, 378−
Hof, A. F.; Braakhekke, M. C.; Gernaat, D. E. H. J.; van den Berg, M.; 400.
van Zeist, W. J.; Daioglou, V.; van Meijl, H.; Lucas, P. L. Afforestation (63) Fuhrman, J.; Mcjeon, H.; Patel, P.; Doney, S. C.; Shobe, W. M.;
for Climate Change Mitigation: Potentials, Risks and Trade-Offs. Clarens, A. F. Food−Energy−Water Implications of Negative
Glob. Chang. Biol. 2020, 26 (3), 1576−1591. Emissions Technologies in a + 1.5 °C Future. Nat. Clim. Change
(46) Muratori, M.; Bauer, N.; Rose, S. K.; Wise, M.; Daioglou, V.; 2020, 10, 1−8.
Cui, Y.; Kato, E.; Gidden, M.; Strefler, J.; Fujimori, S.; Sands, R. D.; (64) Hanna, R.; Abdulla, A.; Xu, Y.; Victor, D. G. Emergency
van Vuuren, D. P.; Weyant, J. EMF-33 Insights on Bioenergy with Deployment of Direct Air Capture as a Response to the Climate
Carbon Capture and Storage (BECCS). Clim. Change 2020, 163, Crisis. Nat. Commun. 2021, 12, 1−13.
1621−1637. (65) Chen, C.; Tavoni, M. Direct Air Capture of CO2 and Climate
(47) Fridahl, M.; Lehtveer, M. Bioenergy with Carbon Capture and Stabilization: A Model Based Assessment. Clim. Change 2013, 118
(1), 59−72.
Storage (BECCS): Global Potential, Investment Preferences, and
(66) Marcucci, A.; Kypreos, S.; Panos, E. The Road to Achieving the
Deployment Barriers. Energy Res. Soc. Sci. 2018, 42 (October 2017),
Long-Term Paris Targets: Energy Transition and the Role of Direct
155−165.
Air Capture. Clim. Change 2017, 144 (2), 181−193.
(48) Mac Dowell, N.; Fajardy, M. Inefficient Power Generation as an
(67) Strefler, J.; Bauer, N.; Kriegler, E.; Popp, A.; Giannousakis, A.;
Optimal Route to Negative Emissions via BECCS? Environ. Res. Lett. Edenhofer, O. Between Scylla and Charybdis: Delayed Mitigation
2017, 12 (4). 045004. Narrows the Passage between Large-Scale CDR and High Costs.
(49) Muri, H. The Role of Large - Scale BECCS in the Pursuit of the Environ. Res. Lett. 2018, 13 (4). 044015.
1.5 °C Target: An Earth System Model Perspective. Environ. Res. Lett. (68) Fuss, S.; Reuter, W. H.; Szolgayová, J.; Obersteiner, M. Optimal
2018, 13 (4). 044010. Mitigation Strategies with Negative Emission Technologies and
(50) Sanz-Pérez, E. S.; Murdock, C. R.; Didas, S. A.; Jones, C. W. Carbon Sinks under Uncertainty. Clim. Change 2013, 118 (1), 73−87.
Direct Capture of CO2 from Ambient Air. Chem. Rev. 2016, 116 (19), (69) Rao, A. B.; Rubin, E. S. Identifying Cost-Effective CO2 Control
11840−11876. Levels for Amine-Based CO2 Capture Systems. Ind. Eng. Chem. Res.
(51) Santori, G.; Charalambous, C.; Ferrari, M. C.; Brandani, S. 2006, 45 (8), 2421−2429.
Adsorption Artificial Tree for Atmospheric Carbon Dioxide Capture, (70) IEAGHG. CCS in Energy and Climate Scenarios, 2019.
Purification and Compression. Energy 2018, 162, 1158−1168. (71) IEAGHG. Towards Zero Emissions CCS in Power Plants
(52) Socolow, R.; Desmond, M.; Aines, R.; Blackstock, J.; Bolland, Using Higher Capture Rates or Biomass. 2019, No. Marc 1−128.
O.; Kaarsberg, T.; Lewis, N.; Mazzotti, M.; Pfeffer, A.; Sawyer, K.; (72) Brandl, P.; Bui, M.; Hallett, J. P.; Mac Dowell, N. Beyond 90%
Siirola, J.; Smit, B.; Wilcox, J. Direct Air Capture of CO2 with Chemicals Capture: Possible, but at What Cost? Int. J. Greenhouse Gas Control
Panel on Public Affairs; American Physical Society, 2011; p 100. 2021, 105 (January), 103239.

8531 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

(73) Jiang, K.; Feron, P.; Cousins, A.; Zhai, R.; Li, K. Achieving (90) Siegelman, R. L.; Milner, P. J.; Forse, A. C.; Lee, J. H.; Colwell,
Zero/Negative-Emissions Coal-Fired Power Plants Using Amine- K. A.; Neaton, J. B.; Reimer, J. A.; Weston, S. C.; Long, J. R. Water
Based Postcombustion CO2 Capture Technology and Biomass Enables Efficient CO2 Capture from Natural Gas Flue Emissions in an
Cocombustion. Environ. Sci. Technol. 2020, 54 (4), 2429−2438. Oxidation-Resistant Diamine-Appended Metal-Organic Framework. J.
(74) Gao, T.; Selinger, J. L.; Rochelle, G. T. Demonstration of 99% Am. Chem. Soc. 2019, 141 (33), 13171−13186.
CO2 Removal from Coal Flue Gas by Amine Scrubbing. Int. J. (91) Azarabadi, H.; Lackner, K. S. Postcombustion Capture or
Greenhouse Gas Control 2019, 83 (February), 236−244. Direct Air Capture in Decarbonizing US Natural Gas Power? Environ.
(75) Feron, P.; Cousins, A.; Jiang, K.; Zhai, R.; Shwe Hla, S.; Sci. Technol. 2020, 54 (8), 5102−5111.
Thiruvenkatachari, R.; Burnard, K. Towards Zero Emissions from (92) McQueen, N.; Psarras, P.; Pilorgé, H.; Liguori, S.; He, J.; Yuan,
Fossil Fuel Power Stations. Int. J. Greenhouse Gas Control 2019, 87 M.; Woodall, C. M.; Kian, K.; Pierpoint, L.; Jurewicz, J.; Lucas, J. M.;
(April), 188−202. Jacobson, R.; Deich, N.; Wilcox, J. Cost Analysis of Direct Air
(76) Caram, H. S.; Gupta, R.; Thomann, H.; Ni, F.; Weston, S. C.; Capture and Sequestration Coupled to Low-Carbon Thermal Energy
Afeworki, M. A Simple Thermodynamic Tool for Assessing Energy in the United States. Environ. Sci. Technol. 2020, 54 (12), 7542−7551.
Requirements for Carbon Capture Using Solid or Liquid Sorbents. (93) Lackner, K. S.; Brennan, S.; Matter, J. M.; Park, A. H. A.;
Int. J. Greenhouse Gas Control 2020, 97 (October 2019), 102986. Wright, A.; Van Der Zwaan, B. The Urgency of the Development of
(77) House, K. Z.; Harvey, C. F.; Aziz, M. J.; Schrag, D. P. The CO2 Capture from Ambient Air. Proc. Natl. Acad. Sci. U. S. A. 2012,
Energy Penalty of Post-Combustion CO2 Capture & Storage and Its 109 (33), 13156−13162.
Implications for Retrofitting the U.S. Installed Base. Energy Environ. (94) Dijkstra, J. W.; Walspurger, S.; Elzinga, G. D.; Pieterse, J. A. Z.;
Sci. 2009, 2 (2), 193−205. Boon, J.; Haije, W. G. Evaluation of Postcombustion CO2 Capture by
(78) Hirata, T.; Tsujiuchi, T.; Kamijo, T.; Kishimoto, S.; Inui, M.; a Solid Sorbent with Process Modeling Using Experimental CO2 and
Kawasaki, S.; Lin, Y. J.; Nakagami, Y.; Nojo, T. Near-Zero Emission H2O Adsorption Characteristics. Ind. Eng. Chem. Res. 2018, 57 (4),
Coal-Fired Power Plant Using Advanced KM CDR Process. Int. J. 1245−1261.
Greenhouse Gas Control 2020, 92 (October 2018), 102847. (95) Zhang, W.; Liu, H.; Sun, Y.; Cakstins, J.; Sun, C.; Snape, C. E.
(79) DOE/NETL. Cost and Performance of PC and IGCC Plants for a Parametric Study on the Regeneration Heat Requirement of an
Range of Carbon Dioxide Capture; 2011; pp 1−500. Amine-Based Solid Adsorbent Process for Post-Combustion Carbon
(80) Lin, Y. J.; Madan, T.; Rochelle, G. T. Regeneration with Rich Capture. Appl. Energy 2016, 168, 394−405.
Bypass of Aqueous Piperazine and Monoethanolamine for CO2 (96) Kim, K.; Yang, S.; Lee, J. B.; Eom, T. H.; Ryu, C. K.; Jo, S. H.;
Capture. Ind. Eng. Chem. Res. 2014, 53 (10), 4067−4074. Park, Y. C.; Yi, C. K. Analysis of K2CO3/Al2O3 CO2 Sorbent Tested
(81) Abu-Zahra, M. R. M.; Niederer, J. P. M.; Feron, P. H. M.;
with Coal-Fired Power Plant Flue Gas: Effect of SOX. Int. J.
Versteeg, G. F. CO2 Capture from Power Plants. Part II. A Parametric
Greenhouse Gas Control 2012, 9, 347−354.
Study of the Economical Performance Based on Mono-Ethanolamine. (97) Saeed, I. M.; Alaba, P.; Mazari, S. A.; Basirun, W. J.; Lee, V. S.;
Int. J. Greenhouse Gas Control 2007, 1 (2), 135−142.
Sabzoi, N. Opportunities and Challenges in the Development of
(82) Siegelman, R. L.; Milner, P. J.; Kim, E. J.; Weston, S. C.; Long,
Monoethanolamine and Its Blends for Post-Combustion CO2
J. R. Challenges and Opportunities for Adsorption-Based CO2
Capture. Int. J. Greenhouse Gas Control 2018, 79 (November),
Capture from Natural Gas Combined Cycle Emissions. Energy
212−233.
Environ. Sci. 2019, 12 (7), 2161−2173.
(98) Luderer, G.; Vrontisi, Z.; Bertram, C.; Edelenbosch, O. Y.;
(83) Siegelman, R. L.; McDonald, T. M.; Gonzalez, M. I.; Martell, J.
Pietzcker, R. C.; Rogelj, J.; De Boer, H. S.; Drouet, L.; Emmerling, J.;
D.; Milner, P. J.; Mason, J. A.; Berger, A. H.; Bhown, A. S.; Long, J. R.
Fricko, O.; Fujimori, S.; Havlík, P.; Iyer, G.; Keramidas, K.; Kitous, A.;
Controlling Cooperative CO2 Adsorption in Diamine-Appended
Mg2(dobpdc) Metal-Organic Frameworks. J. Am. Chem. Soc. 2017, Pehl, M.; Krey, V.; Riahi, K.; Saveyn, B.; Tavoni, M.; Van Vuuren, D.
139, 10526−10538. P.; Kriegler, E. Residual Fossil CO2 Emissions in 1.5−2 °C Pathways.
(84) Furukawa, H.; Cordova, K. E.; O’Keeffe, M.; Yaghi, O. M. The Nat. Clim. Change 2018, 8 (7), 626−633.
Chemistry and Applications of Metal-Organic Frameworks. Science, (99) Harper, A. B.; Powell, T.; Cox, P. M.; House, J.; Huntingford,
2013, 341 (6149). 1230444. C.; Lenton, T. M.; Sitch, S.; Burke, E.; Chadburn, S. E.; Collins, W. J.;
(85) Sumida, K.; Rogow, D. L.; Mason, J. A.; McDonald, T. M.; Comyn-Platt, E.; Daioglou, V.; Doelman, J. C.; Hayman, G.;
Bloch, E. D.; Herm, Z. R.; Bae, T. H.; Long, J. R. Carbon Dioxide Robertson, E.; van Vuuren, D.; Wiltshire, A.; Webber, C. P.; Bastos,
Capture in Metal-Organic Frameworks. Chem. Rev. 2012, 112 (2), A.; Boysen, L.; Ciais, P.; Devaraju, N.; Jain, A. K.; Krause, A.; Poulter,
724−781. B.; Shu, S. Land-Use Emissions Play a Critical Role in Land-Based
(86) McDonald, T. M.; Mason, J. A.; Kong, X.; Bloch, E. D.; Gygi, Mitigation for Paris Climate Targets. Nat. Commun. 2018, 9 (1).
D.; Dani, A.; Crocellà, V.; Giordanino, F.; Odoh, S. O.; Drisdell, W. DOI: 10.1038/s41467-018-05340-z.
S.; Vlaisavljevich, B.; Dzubak, A. L.; Poloni, R.; Schnell, S. K.; Planas, (100) Plevin, R. J.; O’Hare, M.; Jones, A. D.; Torn, M. S.; Gibbs, H.
N.; Lee, K.; Pascal, T.; Wan, L. F.; Prendergast, D.; Neaton, J. B.; K. Greenhouse Gas Emissions from Biofuels’ Indirect Land Use
Smit, B.; Kortright, J. B.; Gagliardi, L.; Bordiga, S.; Reimer, J. A.; Change Are Uncertain but May Be Much Greater than Previously
Long, J. R. Cooperative Insertion of CO2 in Diamine-Appended Estimated. Environ. Sci. Technol. 2010, 44 (21), 8015−8021.
Metal-Organic Frameworks. Nature 2015, 519 (7543), 303−308. (101) Roe, S.; Streck, C.; Obersteiner, M.; Frank, S.; Griscom, B.;
(87) Kim, E. J.; Siegelman, R. L.; Jiang, H. Z. H.; Forse, A. C.; Lee, Drouet, L.; Fricko, O.; Gusti, M.; Harris, N.; Hasegawa, T.;
J.-H.; Martell, J. D.; Milner, P. J.; Falkowski, J. M.; Neaton, J. B.; Hausfather, Z.; Havlík, P.; House, J.; Nabuurs, G. J.; Popp, A.;
Reimer, J. A.; Weston, S. C.; Long, J. R. Cooperative Carbon Capture Sánchez, M. J. S.; Sanderman, J.; Smith, P.; Stehfest, E.; Lawrence, D.
and Steam Regeneration with Tetraamine-Appended Metal-Organic Contribution of the Land Sector to a 1.5 °C World. Nat. Clim. Change
Frameworks. Science 2020, 369 (6502), 392−396. 2019, 9 (11), 817−828.
(88) Leperi, K. T.; Snurr, R. Q.; You, F. Optimization of Two-Stage (102) Pehl, M.; Arvesen, A.; Humpenöder, F.; Popp, A.; Hertwich,
Pressure/Vacuum Swing Adsorption with Variable Dehydration Level E. G.; Luderer, G. Understanding Future Emissions from Low-Carbon
for Postcombustion Carbon Capture. Ind. Eng. Chem. Res. 2016, 55 Power Systems by Integration of Life-Cycle Assessment and
(12), 3338−3350. Integrated Energy Modelling. Nat. Energy 2017, 2 (12), 939−945.
(89) Nikolaidis, G. N.; Kikkinides, E. S.; Georgiadis, M. C. Model- (103) Field, J. L.; Richard, T. L.; Smithwick, E. A. H.; Cai, H.; Laser,
Based Approach for the Evaluation of Materials and Processes for M. S.; Lebauer, D. S. Robust Paths to Net Greenhouse Gas Mitigation
Post-Combustion Carbon Dioxide Capture from Flue Gas by PSA/ and Negative Emissions via Advanced Biofuels. Proc. Natl. Acad. Sci.
VSA Processes. Ind. Eng. Chem. Res. 2016, 55 (3), 635−646. U. S. A. 2020, 117 (No. 12), 1−10.

8532 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

(104) Khanna, M.; Wang, W.; Hudiburg, T. W.; Delucia, E. H. The Shared Socioeconomic Pathway 2: A Middle-of-the-Road Scenario for
Social Inefficiency of Regulating Indirect Land Use Change Due to the 21st Century. Glob. Environ. Chang. 2017, 42, 251−267.
Biofuels. Nat. Commun. 2017, 8 (May 2016), 1−9. (123) Smith, P.; Adams, J.; Beerling, D. J.; Beringer, T.; Calvin, K.
(105) Sanchez, D. L.; Nelson, J. H.; Johnston, J.; Mileva, A.; V.; Fuss, S.; Griscom, B.; Hagemann, N.; Kammann, C.; Kraxner, F.;
Kammen, D. M. Biomass Enables the Transition to a Carbon- Minx, J. C.; Popp, A.; Renforth, P.; Vicente Vicente, J. L.; Keesstra, S.
Negative Power System across Western North America. Nat. Clim. Land-Management Options for Greenhouse Gas Removal and Their
Change 2015, 5 (3), 230−234. Impacts on Ecosystem Services and the Sustainable Development
(106) Malins, C.; Plevin, R.; Edwards, R. How Robust Are Goals. Annu. Rev. Environ. Resour. 2019, 44, 255−286.
Reductions in Modeled Estimates from GTAP-BIO of the Indirect (124) Bach, L. T.; Gill, S. J.; Rickaby, R. E. M.; Gore, S.; Renforth, P.
Land Use Change Induced by Conventional Biofuels? J. Cleaner Prod. CO2 Removal With Enhanced Weathering and Ocean Alkalinity
2020, 258, 120716. Enhancement: Potential Risks and Co-Benefits for Marine Pelagic
(107) Fajardy, M.; Mac Dowell, N. Can BECCS Deliver Sustainable Ecosystems. Front. Clim. 2019, 1 (October). DOI: 10.3389/
and Resource Efficient Negative Emissions? Energy Environ. Sci. 2017, fclim.2019.00007.
10 (6), 1389−1426. (125) Pozo, C.; Galán-Martín, Á .; Reiner, D. M.; Mac Dowell, N.;
(108) Cumicheo, C.; Mac Dowell, N.; Shah, N. Natural Gas and Guillén-Gosálbez, G. Equity in Allocating Carbon Dioxide Removal
BECCS: A Comparative Analysis of Alternative Configurations for Quotas. Nat. Clim. Change 2020, 10 (7), 640−646.
Negative Emissions Power Generation. Int. J. Greenhouse Gas Control (126) Fuhrman, J.; McJeon, H.; Doney, S. C.; Shobe, W.; Clarens, A.
2019, 90 (February). 102798. F. From Zero to Hero?: Why Integrated Assessment Modeling of
(109) Khorshidi, Z.; Florin, N. H.; Ho, M. T.; Wiley, D. E. Techno- Negative Emissions Technologies Is Hard and How We Can Do
Economic Evaluation of Co-Firing Biomass Gas with Natural Gas in Better. Front. Clim. 2019, 1 (December). DOI: 10.3389/
Existing NGCC Plants with and without CO2 Capture. Int. J. fclim.2019.00011.
Greenhouse Gas Control 2016, 49, 343−363. (127) U.S. Energy Information Administration. Emissions by plant
(110) Koelbl, B. S.; van den Broek, M. A.; Faaij, A. P. C.; van and by region https://www.eia.gov/electricity/data/emissions/.
Vuuren, D. P. Uncertainty in Carbon Capture and Storage (CCS) (128) U.S. Energy Information Administration. Form EIA-860
Deployment Projections: A Cross-Model Comparison Exercise. Clim. detailed data with previous form data (EIA-860A/860B).
Change 2014, 123 (3−4), 461−476. (129) Zhai, H.; Rubin, E. S. A Techno-Economic Assessment of
(111) International Institute for Applied Systems Analysis. Emission Hybrid Cooling Systems for Coal- and Natural-Gas-Fired Power
from energy (MESSAGE) https://docs.messageix.org/projects/ Plants with and without Carbon Capture and Storage. Environ. Sci.
global/en/latest/emissions/message/index.html. Technol. 2016, 50 (7), 4127−4134.
(112) Luderer, G.; Leimbach, M.; Bauer, N.; Kriegler, E.; Baumstark, (130) Kholod, N.; Evans, M.; Pilcher, R. C.; Roshchanka, V.; Ruiz,
L.; Bertram, C.; Giannousakis, A.; Hilaire, J.; Klein, D.; Levesque, A.; F.; Coté, M.; Collings, R. Global Methane Emissions from Coal
Mouratiadou, I.; Pehl, M.; Pietzcker, R.; Piontek, F.; Roming, N.; Mining to Continue Growing Even with Declining Coal Production. J.
Schultes, A.; Schwanitz, V. J.; Strefler, J. Description of the REMIND Cleaner Prod. 2020, 256. 120489.
Model (Version 1.6); 2015. DOI: 10.2139/ssrn.2697070. (131) Schwietzke, S.; Sherwood, O. A.; Bruhwiler, L. M. P.; Miller, J.
(113) Krey, V.; Luderer, G.; Clarke, L.; Kriegler, E. Getting from B.; Etiope, G.; Dlugokencky, E. J.; Michel, S. E.; Arling, V. A.; Vaughn,
Here to There - Energy Technology Transformation Pathways in the B. H.; White, J. W. C.; Tans, P. P. Upward Revision of Global Fossil
EMF27 Scenarios. Clim. Change 2014, 123 (3−4), 369−382. Fuel Methane Emissions Based on Isotope Database. Nature 2016,
(114) Fondazione Eni Enrico Mattei. WITCH Documentation; 2017. 538 (7623), 88−91.
(115) Keppo, I.; van der Zwaan, B. The Impact of Uncertainty in (132) Karacan, C. O.; Ruiz, F. A.; Cote, M.; Phipps, S. Coal Mine
Climate Targets and CO2 Storage Availability on Long-Term Methane: A Review of Capture and Utilization Practices with Benefits
Emissions Abatement. Environ. Model. Assess. 2012, 17 (1−2), 177− to Mining Safety and to Greenhouse Gas Reduction. Int. J. Coal Geol.
191. 2011, 86, 121−156.
(116) Luderer, G.; Bosetti, V.; Steckel, J.; Waisman, H. Economics of (133) Duda, A.; Krzemień, A. Forecast of Methane Emission from
Decarbonization - RECIPE. Appendix A: Model Description IMACLIM- Closed Underground Coal Mines Exploited by Longwall Mining − A
R 2009. Case Study of Anna Coal Mine. J. Sustain. Min. 2018, 17 (4), 184−
(117) Muratori, M.; Kheshgi, H.; Mignone, B.; McJeon, H.; Clarke, 194.
L. The Future Role of CCS in Electricity and Liquid Fuel Supply. (134) Schwietzke, S.; Griffin, W. M.; Matthews, H. S.; Bruhwiler, L.
Energy Procedia 2017, 114 (November 2016), 7606−7614. M. P. Natural Gas Fugitive Emissions Rates Constrained by Global
(118) Muratori, M.; Kheshgi, H.; Mignone, B.; Clarke, L.; McJeon, Atmospheric Methane and Ethane. Environ. Sci. Technol. 2014, 48
H.; Edmonds, J. Carbon Capture and Storage across Fuels and Sectors (14), 7714−7722.
in Energy System Transformation Pathways. Int. J. Greenhouse Gas (135) Zimmerle, D. J.; Williams, L. L.; Vaughn, T. L.; Quinn, C.;
Control 2017, 57, 34−41. Subramanian, R.; Duggan, G. P.; Willson, B.; Opsomer, J. D.;
(119) Tong, D.; Zhang, Q.; Zheng, Y.; Caldeira, K.; Shearer, C.; Marchese, A. J.; Martinez, D. M.; Robinson, A. L. Methane Emissions
Hong, C.; Qin, Y.; Davis, S. J. Committed Emissions from Existing from the Natural Gas Transmission and Storage System in the United
Energy Infrastructure Jeopardize 1.5 °C Climate Target. Nature 2019, States. Environ. Sci. Technol. 2015, 49 (15), 9374−9383.
572 (7769), 373−377. (136) Roman-white, S.; Rai, S.; Littlefield, J.; Cooney, G.; Skone, T.
(120) Kriegler, E.; Luderer, G.; Bauer, N.; Baumstark, L.; Fujimori, J. Life Cycle Greenhouse Gas Perspective on Exporting Liquefied Natural
S.; Popp, A.; Rogelj, J.; Strefer, J.; Van Vuuren, D. P. Pathways Gas from the United States; National Energy Technology Laboratory,
Limiting Warming to 1.5°C: A Tale of Turning around in No Time? 2014; Vol. 79 (107), pp 32260−32261.
Philos. Trans. R. Soc., A 2018, 376 (2119). 20160457. (137) Balcombe, P.; Anderson, K.; Speirs, J.; Brandon, N.; Hawkes,
(121) Sgouridis, S.; Carbajales-Dale, M.; Csala, D.; Chiesa, M.; A. The Natural Gas Supply Chain: The Importance of Methane and
Bardi, U. Comparative Net Energy Analysis of Renewable Electricity Carbon Dioxide Emissions. ACS Sustainable Chem. Eng. 2017, 5 (1),
and Carbon Capture and Storage. Nat. Energy 2019, 4 (6), 456−465. 3−20.
(122) Fricko, O.; Havlik, P.; Rogelj, J.; Klimont, Z.; Gusti, M.; (138) Skone, T.; Littlefield, J.; Marriott, J.; Cooney, G.; Demetrion,
Johnson, N.; Kolp, P.; Strubegger, M.; Valin, H.; Amann, M.; L.; Jamieson, M.; Jones, C.; Mutchek, M.; Yan Shih, C.; Schivley, G.;
Ermolieva, T.; Forsell, N.; Herrero, M.; Heyes, C.; Kindermann, G.; Krynock, M.; Hamilton, B. A. Life Cycle Analysis of Natural Gas
Krey, V.; McCollum, D. L.; Obersteiner, M.; Pachauri, S.; Rao, S.; Extraction and Power Generation. National Energy Technology
Schmid, E.; Schoepp, W.; Riahi, K. The Marker Quantification of the Laboratory 2014, 1−200.

8533 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534
Environmental Science & Technology pubs.acs.org/est Perspective

(139) Alvarez, R. A.; Zavala-Araiza, D.; Lyon, D. R.; Allen, D. T.;

Barkley, Z. R.; Brandt, A. R.; Davis, K. J.; Herndon, S. C.; Jacob, D. J.;
Karion, A.; Kort, E. A.; Lamb, B. K.; Lauvaux, T.; Maasakkers, J. D.;
Marchese, A. J.; Omara, M.; Pacala, S. W.; Peischl, J.; Robinson, A. L.;
Shepson, P. B.; Sweeney, C.; Townsend-Small, A.; Wofsy, S. C.;
Hamburg, S. P. Assessment of Methane Emissions from the U.S. Oil
and Gas Supply Chain. Science 2018, 361 (6398), 186−188.
(140) Schuiling, R. D.; Krijgsman, P. Enhanced Weathering: An
Effective and Cheap Tool to Sequester CO2. Clim. Change 2006, 74
(1−3), 349−354.
(141) Pilorgé, H.; McQueen, N.; Maynard, D.; Psarras, P.; He, J.;
Rufael, T.; Wilcox, J. Cost Analysis of Carbon Capture and
Sequestration of Process Emissions from the U.S. Industrial Sector.
Environ. Sci. Technol. 2020, 54 (12), 7524−7532.
(142) Tanzer, S. E.; Blok, K.; Ramírez, A. Can Bioenergy with
Carbon Capture and Storage Result in Carbon Negative Steel? Int. J.
Greenhouse Gas Control 2020, 100 (December 2019), 103104.
(143) Tian, S.; Jiang, J.; Zhang, Z.; Manovic, V. Inherent Potential of
Steelmaking to Contribute to Decarbonisation Targets via Industrial
Carbon Capture and Storage. Nat. Commun. 2018, 9 (1), 1−8.
(144) Leeson, D.; Mac Dowell, N.; Shah, N.; Petit, C.; Fennell, P. S.
A Techno-Economic Analysis and Systematic Review of Carbon
Capture and Storage (CCS) Applied to the Iron and Steel, Cement,
Oil Refining and Pulp and Paper Industries, as Well as Other High
Purity Sources. Int. J. Greenhouse Gas Control 2017, 61, 71−84.
(145) Davis, S. J.; Lewis, N. S.; Shaner, M.; Aggarwal, S.; Arent, D.;
Azevedo, I. L.; Benson, S. M.; Bradley, T.; Brouwer, J.; Chiang, Y. M.;
Clack, C. T. M.; Cohen, A.; Doig, S.; Edmonds, J.; Fennell, P.; Field,
C. B.; Hannegan, B.; Hodge, B. M.; Hoffert, M. I.; Ingersoll, E.;
Jaramillo, P.; Lackner, K. S.; Mach, K. J.; Mastrandrea, M.; Ogden, J.;
Peterson, P. F.; Sanchez, D. L.; Sperling, D.; Stagner, J.; Trancik, J. E.;
Yang, C. J.; Caldeira, K. Net-Zero Emissions Energy Systems. Science
2018, 360 (6396). eaas9793.
(146) Biermann, M.; Ali, H.; Sundqvist, M.; Larsson, M.; Normann,
F.; Johnsson, F. Excess Heat-Driven Carbon Capture at an Integrated
Steel Mill − Considerations for Capture Cost Optimization. Int. J.
Greenhouse Gas Control 2019, 91, 102833.
(147) Wilson, I. A. G.; Staffell, I. Rapid Fuel Switching from Coal to
Natural Gas through Effective Carbon Pricing. Nat. Energy 2018, 3
(5), 365−372.

8534 https://doi.org/10.1021/acs.est.0c07390
Environ. Sci. Technol. 2021, 55, 8524−8534