developing thin and strong SPEs that
Promises High-Energy-Density Lithium-Sulfur
are compatible for both anode and
cathode with low interfacial resistance,
more advanced high-energy-density
energy storage and conversion devices
can be expected for applications.
1. Manthiram, A., Fu, Y., Chung, S.H., Zu, C., and
Su, Y.S. (2014). Rechargeable lithium-sulfur
batteries. Chem. Rev. 114, 11751–11787.
2. Zhang, H., Oteo, U., Judez, X., Eshetu, G.G.,
Martinez-Ibañez, M., Carrasco, J., Li, C., and
Armand, M. (2019). Designer Anion Enabling
Solid-State Lithium-Sulfur Batteries. Joule 3,
this issue, 1689–1702.
3. Pang, Q., Kwok, C.Y., Kundu, D., Liang, X.,
and Nazar, L.F. (2019). Lightweight Metallic
Preview
Pricing CO2 Direct Air Capture
Brandon R. Sutherland1,*
Negative emissions technologies such as direct air capture systems are an
important tool to impede climate change. Recently in Applied Energy, Azara-
badi and Lackner reported a generalized cost model for direct air capture of
CO2. Their findings emphasize the importance of sorbent cycle duration and sta-
bility in minimizing total system cost.
The human-caused component of car-
bon dioxide emissions has grown expo-
nentially starting from the early 1800s,
doubling roughly every 30 years.1 This
has resulted in an anthropogenic-driven
climate change that has increased global
average temperatures greater than 1 C
beyond the pre-industrial level. To curtail
adverse effects associated with a warmer
Earth, the Paris Climate Change Agree-
ment has set a target of reducing the
temperature increase this century to
well below 2 C of this level.2 Realizing
this requires reducing all greenhouse
gas (GHG) emissions to zero by mid-
21st century.
The world’s ingrained dependence on
fossil fuels to produce electricity, to
control heating and cooling, and as
a transportation fuel make a carbon-
MgB2 Mediates Polysulfide Redox and
Int. Ed. Engl. 55, 2521–2525.
Batteries. Joule 3, 136–148.
4. Degott, P. (1986). Polymere Carbone-Soufre
Synthese et Proprietes Electrochimiques.
PhD thesis (l’Institut National Polytechnique
de Grenoble).
5. https://www.bluecar.fr/sites/bluecar/files/
medias/PDF/2_bluecar_20_p.pdf.
6. Zhao, Q., Chen, P., Li, S., Liu, X., and Archer,
L.A. (2019). Solid-state polymer electrolytes
stabilized by task-specific salt additives.
J. Mater. Chem. A Mater. Energy Sustain. 7,
7823–7830.
7. Ma, Q., Zhang, H., Zhou, C., Zheng, L.,
Cheng, P., Nie, J., Feng, W., Hu, Y.S., Li, H.,
Huang, X., et al. (2016). Single Lithium-Ion
Conducting Polymer Electrolytes Based on a
free transition immensely challenging—
especially considering the rapid time-
scales needed to meet climate targets.
The energy infrastructure needs to shift
toward renewable power sources and
on-site capture, storage, and utilization
of GHG exhaust streams. A lack of
competitive economics for such tech-
nology to displace traditional fossil fuels
has greatly impeded progress on this
front.
Still, society does have the tools to fight
climate change through technology,
government intervention, and public ed-
ucation. It is a complex problem shackled
by economic influence that will require
an open mind for new proposed solu-
tions and long-term risk management.
Beyond simply stopping the emission of
GHGs, an idea that is only growing in
Joule 3, 1569–1577, July 17, 2019 ª 2019 Published by Elsevier Inc. 1571
Super-Delocalized Polyanion. Angew. Chem.
8. Zhao, Q., Liu, X., Stalin, S., Khan, K., and
Archer, L.A. (2019). Solid-state polymer
electrolytes with in-built fast interfacial
transport for secondary lithium batteries.
Nat. Energy 4, 365–373.
9. Zhao, Q., Zheng, J., and Archer, L. (2018).
Interphases in Lithium–Sulfur Batteries:
Toward Deployable Devices with
Competitive Energy Density and Stability.
ACS Energy Lett. 3, 2104–2113.
10. Wan, J., Xie, J., Kong, X., Liu, Z., Liu, K., Shi,
F., Pei, A., Chen, H., Chen, W., Chen, J.,
et al. (2019). Ultrathin, flexible, solid polymer
composite electrolyte enabled with aligned
nanoporous host for lithium batteries. Nat.
Nanotechnol. Published online May 27,
2019. https://doi.org/10.1038/s41565-019-
0465-3.
importance is taking CO2 out of the
biosphere and putting it back in the geo-
sphere using negative emissions technol-
ogies (NETs). While it is more cost-effec-
tive to reduce GHG emissions toward
the zero limit, the further off track the
world is from meeting climate goals the
more NETs become necessary. Indeed,
the Intergovernmental Panel on Climate
Change predicts that a slow carbon-
neutral transition alone is insufficient
and NETs are needed curb global
average temperature rises.3
One category of NETs consists of CO2-
absorbing biomass. More trees can be
planted (afforestation) or biomass can
be farmed, combusted, or broken down
through other means and then re-
planted. The carbon emissions from this
process can be captured and seques-
tered or used. This is termed bioenergy
with carbon capture and storage,
BECCS. An alternative approach is to
take atmospheric CO2 directly from the
air and store it underground.4 A consis-
tent problem with each of these methods
1Joule,
Cell Press, 50 Hampshire Street, 5th Floor,
Cambridge, MA 02139, USA
*Correspondence: bsutherland@cell.com
https://doi.org/10.1016/j.joule.2019.06.025

Figure 1. A Direct Air Capture System with Sorbent Regeneration
is that the costs are high, often 1–2 orders
of magnitude greater than the trading
price of CO2.
Direct air capture (DAC) is an emerging
NET with recent pilot-scale cost esti-
mates of $94 to $232 per ton CO2,5 pre-
dicted to drop below $60 by 2040.6
DAC uses water and energy as inputs
and produces a pure, compressed
stream of CO2 as an output. CO2 is
captured directly from the air, where it
flows through a separation element,
often a liquid or solid sorbent. An
example sorbent-based DAC process
is shown in Figure 1. Ambient air is
forced through a sorbent functionalized
to bind CO2 either chemically or physi-
cally. Air with reduced CO2 partial pres-
sures is returned to the atmosphere.
Through heat, pressure, or humidity,
the sorbent can be regenerated,
releasing a pure CO2 stream and
enabling re-use.
The output pure CO2 stream in DAC
systems can be stored underground,
used to synthesize commodity chemi-
cals, or re-synthesized into low-carbon
fuels. Compared to approaches that
utilize CO2-absorbing biomass, DAC
1572 Joule 3, 1569–1577, July 17, 2019
plants use 100–50,000+ times less
land.7 Since CO2 is distributed homo-
genously throughout the atmosphere,
DAC plants can be placed anywhere
that is most economic, such as near a
carbon sequestration site to minimize
transport costs.
Reducing the cost of DAC will be crit-
ical to expand its chance at having an
impact, and there is a need for better,
generalized models to estimate cost
bounds. Recently in Applied Energy,
Azarabadi and Lackner have devel-
oped a cost model for direct air cap-
ture systems that factors in market
CO2 price as well as sorbent cycle
time, loading capacity, degradation
rate, and regeneration method.8 The
model provides a value equation for
DAC cost independent from system
design, enabling easy comparison
and unification of the multitude of sor-
bents and processes reported in
literature.
It was found that minimum costs consid-
ering sorbents under various conditions
ranged from $29 to $91 per ton CO2.
These estimates are part of a growing
body of evidence for the falling costs of
DAC. The sorbent cycle life and stability
were determined to be critical parame-
ters that influence cost, something often
neglected in design and testing at the
research scale. This work sheds light on
a common problem in materials
research—neglecting that performance
is coupled to cost, manufacturing
complexity, and stability in real-world
applications. Generalized cost models
that factor in each of these components
are therefore essential not only for com-
panies looking to design DAC plants but
for researchers working on the sorbent
components in the lab.
At current rates of adoption for renew-
able power generation, humans will be
unable to sufficiently limit global tem-
perature rises. Even with a 100% renew-
able grid transition this century,
younger generations will still have the
burden of living in a post-climate-
change world. It is human psychology
to prioritize fixing an immediate prob-
lem over preventing future ones. How-
ever, new technology is rarely some-
thing that can immediately be applied
at scale. Technology takes times to
progress down the learning curve and
reduce its cost. Without continued de-
velopments in NETs today, there will
be one less weapon to combat climate
change as its urgency accelerates in
the future.
1. Hofmann, D.J., Butler, J.H., and Tans, P.P.
(2009). A new look at atmospheric carbon
dioxide. Atmos. Environ. 43, 2084–2086.
2. United Nations Framework Convention on
Climate Change (2015). Adoption of the Paris
Agreement. Proposal by the President. https://
unfccc.int/resource/docs/2015/cop21/eng/
l09.pdf.
3. V. Masson-Delmotte, P. Zhai, H.O. Pörtner, D.
Roberts, J. Skea, P.R. Shukla, A. Pirani, W.
Moufouma-Okia, C. Péan, and R. Pidcock,
et al., eds. (2018). Global warming of 1.5 C. An
IPCC Special Report on the impacts of global
warming of 1.5 C above pre-industrial levels
and related global greenhouse gas emission
pathways, in the context of strengthening the
global response to the threat of climate
change, sustainable development, and efforts
to eradicate poverty (World Meteorological
Organization).
4. Sanz-Pérez, E.S., Murdock, C.R., Didas, S.A.,
and Jones, C.W. (2016). Direct Capture of
 CO2 from Ambient Air. Chem. Rev. 116,
11840–11876.
5. Keith, D.W., Holmes, G., St. Angelo, D., and
Heidel, K. (2018). A Process for Capturing
CO2 from the Atmosphere. Joule 2, 1573–
1594.
Preview
True or False
in Electrochemical
Nitrogen Reduction
Cheng Tang1 and Shi-Zhang Qiao1,*
Electrochemical nitrogen reduction to ammonia has recently gathered enor-
mous interest as an attractive carbon-neutral alternative to the Haber-Bosch
process. However, this novel process severely suffers from poor reproducibility
and reliability. As reported recently in Nature, Chorkendorff and colleagues im-
plemented a systematic benchmarking protocol to eliminate the false and retain
the true in nitrogen electroreduction research.
Ammonia, the second highest pro-
duced chemical in the world (170 Mt
year–1), is the vital ingredient in most
fertilizers used to sustain the ever-
growing global population and is also
being considered for use in renewable
energy storage as an energy-dense
carbon-neutral liquid fuel. Today, the
preeminent Haber-Bosch process con-
tributes 90% of annual ammonia pro-
duction. However, this century-old pro-
cess requires massive energy input and
capital cost and creates significant CO2
emissions.1 Recently, the electrochemi-
cal nitrogen reduction reaction (NRR)
using renewable electricity under
ambient conditions was proposed in
principle as a perfect alternative to the
Haber-Bosch process.2 Ideally, this
would make ammonia production less
dependent on fossil fuels and decen-
tralized for on-site and on-demand
production.2,3
To date, various electrocatalysts and
strategies to enhance electrochemical
6. Fasihi, M., Efimova, O., and Breyer, C. (2019).
Techno-economic assessment of CO2 direct
air capture plants. J. Clean. Prod. 224,
957–980.
7. Fajardy, M., and Mac Dowell, N. (2017). Can
BECCS deliver sustainable and resource
NRR activity and selectivity have been
reported. However, significant doubt
and discussion has arisen as to whether
these results should be ascribed to
actual N2 electroreduction or false pos-
itives.4 Although many artifact sources
have been recognized and a series of
control experiments have been estab-
lished since 2018,5–8 the reliability, ac-
curacy, and reproducibility of recent
literature still requires improvement.
Therefore, a benchmarking protocol
for electrochemical NRR research
regarding contamination elimination,
control experiments, and data report-
ing is urgently needed.
In a landmark study recently published
in Nature, Chorkendorff and col-
leagues highlighted this ‘‘true or false’’
issue in the electrochemical NRR
research community.9 They put for-
ward a rigorous protocol to correctly
quantify N2 electroreduction activity
and re-evaluated several catalysts and
processes, revealing both the feasi-
Joule 3, 1569–1577, July 17, 2019 ª 2019 Elsevier Inc. 1573
efficient negative emissions? Energy Environ.
Sci. 10, 1389–1426.
8. Azarabadi, H., and Lackner, K.S. (2019). A
sorbent-focused techno-economic analysis
of direct air capture. Appl. Energy 250,
959–975.
bility and challenges of electrochemi-
cal NRR.
Thorough identification and efficient
elimination of all potential contaminant
sources is the prerequisite to design
and conduct meaningful NRR experi-
ments. In addition to some gradually
recognized contaminant sources, the
authors especially emphasize artifacts
originating from ion-conducting mem-
branes and feed gas streams. Nafion
membranes have been shown to allow
significant accumulation, release, and
crossover of ammonia, resulting in false
negatives or positives. Alternatively, a
microporous polypropylene mem-
brane, Celgard 3401, was recommen-
ded for all aqueous experiments
without the requirement of a cleaning
procedure. However, commercial Cel-
gard membranes are highly hydropho-
bic and designed for lithium batteries
and thus require specific hydrophilic
treatment while maintaining mechani-
cal flexibility for aqueous NRR. High-
purity N2 gas or even isotope-labeled
15
N2 gas usually contains a tiny amount
of impurities in the form of NH3 or NOx.
The former contamination can be ratio-
nally excluded using control experi-
ments with N2 at open-circuit potential
(OCP), while the latter cannot be inde-
pendently probed because NOx can
readily be reduced electrochemically
to NH3. The feed gas was thus
1Center for Materials in Energy and Catalysis,
School of Chemical Engineering and Advanced
Materials, The University of Adelaide, Adelaide,
SA 5005, Australia
*Correspondence: s.qiao@adelaide.edu.au
https://doi.org/10.1016/j.joule.2019.06.020