Energy- and carbon-efficient CO2/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption

Adnan Ozden; Jun Li; Sharath Kandambeth; Xiao Yan Li; Shijie Liu; Osama Shekhah; Pengfei Ou; Y. Zou Finfrock; Ya Kun Wang; Tartela Alkayyali; F. Pelayo García de Arquer; Vinayak S. Kale; Prashant M. Bhatt; Alexander H. Ip; Mohamed Eddaoudi; Edward H. Sargent; David Sinton

doi:10.1038/s41560-022-01188-2

Energy- and carbon-efficient CO₂/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption

Adnan Ozden, Jun Li^*, Sharath Kandambeth, Xiao Yan Li, Shijie Liu, Osama Shekhah, Pengfei Ou, Y. Zou Finfrock, Ya Kun Wang, Tartela Alkayyali, F. Pelayo García de Arquer, Vinayak S. Kale, Prashant M. Bhatt, Alexander H. Ip, Mohamed Eddaoudi^*, Edward H. Sargent^*, David Sinton^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

Carbon dioxide/monoxide (CO₂/CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface—a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The π-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation–π interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. As a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm⁻².

Original language	English (US)
Pages (from-to)	179-190
Number of pages	12
Journal	Nature Energy
Volume	8
Issue number	2
DOIs	https://doi.org/10.1038/s41560-022-01188-2
State	Published - Feb 2023

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1038/s41560-022-01188-2

Cite this

Ozden, A., Li, J., Kandambeth, S., Li, X. Y., Liu, S., Shekhah, O., Ou, P., Zou Finfrock, Y., Wang, Y. K., Alkayyali, T., Pelayo García de Arquer, F., Kale, V. S., Bhatt, P. M., Ip, A. H., Eddaoudi, M., Sargent, E. H., & Sinton, D. (2023). Energy- and carbon-efficient CO₂/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption. Nature Energy, 8(2), 179-190. https://doi.org/10.1038/s41560-022-01188-2

@article{ff1e99e3d91940d5bc66d89a776c98ee,

title = "Energy- and carbon-efficient CO2/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption",

abstract = "Carbon dioxide/monoxide (CO2/CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface—a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The π-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation–π interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. As a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm−2.",

author = "Adnan Ozden and Jun Li and Sharath Kandambeth and Li, {Xiao Yan} and Shijie Liu and Osama Shekhah and Pengfei Ou and {Zou Finfrock}, Y. and Wang, {Ya Kun} and Tartela Alkayyali and {Pelayo Garc{\'i}a de Arquer}, F. and Kale, {Vinayak S.} and Bhatt, {Prashant M.} and Ip, {Alexander H.} and Mohamed Eddaoudi and Sargent, {Edward H.} and David Sinton",

note = "Funding Information: This work was financially supported by the Ontario Research Fund – Research Excellence programme, the Natural Sciences and Engineering Research Council (NSERC) of Canada and Natural Resources Canada{\textquoteright}s Clean Growth Program. This research used synchrotron resources of the Advanced Photon Source (an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory) and was supported by the US DOE under contract number DE-AC02-06CH11357, as well as the Canadian Light Source and its funding partners. Support from the Canada Research Chairs Program is gratefully acknowledged, as is support from an NSERC E.W.R. Steacie Fellowship to D.S. J.L. thanks the National Natural Science Foundation of China (grant number BE3250011), the National Key Research and Development Program of China (grant number 2022YFA1505100), and Shanghai Jiao Tong University (grant number WH220432516) for support. F.P.G.d.A. acknowledges funding from CEX2019-000910-S (MCIN/AEI/10.13039/501100011033), Fundaci{\'o}n Cellex, Fundaci{\'o} Mir-Puig, Generalitat de Catalunya through CERCA and the La Caixa Foundation (100010434; EU Horizon 2020 Marie Sk{\l}odowska-Curie grant agreement 847648). Publisher Copyright: {\textcopyright} 2023, The Author(s), under exclusive licence to Springer Nature Limited.",

year = "2023",

month = feb,

doi = "10.1038/s41560-022-01188-2",

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Ozden, A, Li, J, Kandambeth, S, Li, XY, Liu, S, Shekhah, O, Ou, P, Zou Finfrock, Y, Wang, YK, Alkayyali, T, Pelayo García de Arquer, F, Kale, VS, Bhatt, PM, Ip, AH, Eddaoudi, M, Sargent, EH & Sinton, D 2023, 'Energy- and carbon-efficient CO₂/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption', Nature Energy, vol. 8, no. 2, pp. 179-190. https://doi.org/10.1038/s41560-022-01188-2

TY - JOUR

T1 - Energy- and carbon-efficient CO2/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption

AU - Ozden, Adnan

AU - Li, Jun

AU - Kandambeth, Sharath

AU - Li, Xiao Yan

AU - Liu, Shijie

AU - Shekhah, Osama

AU - Ou, Pengfei

AU - Zou Finfrock, Y.

AU - Wang, Ya Kun

AU - Alkayyali, Tartela

AU - Pelayo García de Arquer, F.

AU - Kale, Vinayak S.

AU - Bhatt, Prashant M.

AU - Ip, Alexander H.

AU - Eddaoudi, Mohamed

AU - Sargent, Edward H.

AU - Sinton, David

N1 - Funding Information: This work was financially supported by the Ontario Research Fund – Research Excellence programme, the Natural Sciences and Engineering Research Council (NSERC) of Canada and Natural Resources Canada’s Clean Growth Program. This research used synchrotron resources of the Advanced Photon Source (an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory) and was supported by the US DOE under contract number DE-AC02-06CH11357, as well as the Canadian Light Source and its funding partners. Support from the Canada Research Chairs Program is gratefully acknowledged, as is support from an NSERC E.W.R. Steacie Fellowship to D.S. J.L. thanks the National Natural Science Foundation of China (grant number BE3250011), the National Key Research and Development Program of China (grant number 2022YFA1505100), and Shanghai Jiao Tong University (grant number WH220432516) for support. F.P.G.d.A. acknowledges funding from CEX2019-000910-S (MCIN/AEI/10.13039/501100011033), Fundación Cellex, Fundació Mir-Puig, Generalitat de Catalunya through CERCA and the La Caixa Foundation (100010434; EU Horizon 2020 Marie Skłodowska-Curie grant agreement 847648). Publisher Copyright: © 2023, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2023/2

Y1 - 2023/2

N2 - Carbon dioxide/monoxide (CO2/CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface—a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The π-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation–π interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. As a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm−2.

AB - Carbon dioxide/monoxide (CO2/CO) electrolysis provides a means to convert emissions into multicarbon products. However, impractical energy and carbon efficiencies limit current systems. Here we show that these inefficiencies originate from uncontrolled gas/ion distributions in the local reaction environment. Understanding of the flows of cations and anions motivated us to seek a route to block cation migration to the catalyst surface—a strategy we instantiate using a covalent organic framework (COF) in bulk heterojunction with a catalyst. The π-conjugated hydrophobic COFs constrain cation (potassium) diffusion via cation–π interactions, while promoting anion (hydroxide) and gaseous feedstock adsorption on the catalyst surface. As a result, a COF-mediated catalyst enables electrosynthesis of multicarbon products from CO for 200 h at a single-pass carbon efficiency of 95%, an energy efficiency of 40% and a current density of 240 mA cm−2.

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DO - 10.1038/s41560-022-01188-2

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