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 Swamirao Kale; Prashant Bhatt; Alexander H. Ip; Mohamed Eddaoudi; E. 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 Swamirao Kale, Prashant Bhatt, Alexander H. Ip, Mohamed Eddaoudi, E. Sargent, David Sinton

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

79 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)
Journal	Nature Energy
DOIs	https://doi.org/10.1038/s41560-022-01188-2
State	Published - Jan 12 2023

Bibliographical note

KAUST Repository Item: Exported on 2023-01-17
Acknowledgements: 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).

UN SDGs

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

Access to Document

10.1038/s41560-022-01188-2

Cite this

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

@article{bdeaaf1ee21d46a892c1419c27eb6f2b,

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 Xiao-yan Li and Shijie Liu and Osama Shekhah and Pengfei Ou and {Zou Finfrock}, Y. and Ya-Kun Wang and Tartela Alkayyali and {Garc{\'i}a de Arquer}, {F Pelayo} and Kale, {Vinayak Swamirao} and Prashant Bhatt and Ip, {Alexander H.} and Mohamed Eddaoudi and E. Sargent and David Sinton",

note = "KAUST Repository Item: Exported on 2023-01-17 Acknowledgements: 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).",

year = "2023",

month = jan,

day = "12",

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

language = "English (US)",

journal = "Nature Energy",

issn = "2058-7546",

publisher = "Springer Nature",

}

Ozden, A, Li, J, Kandambeth, S, Li, X, Liu, S, Shekhah, O, Ou, P, Zou Finfrock, Y, Wang, Y-K, Alkayyali, T, García de Arquer, FP, Kale, VS , Bhatt, P, Ip, AH, Eddaoudi, M, Sargent, E & Sinton, D 2023, 'Energy- and carbon-efficient CO2/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption', Nature Energy. 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 - García de Arquer, F Pelayo

AU - Kale, Vinayak Swamirao

AU - Bhatt, Prashant

AU - Ip, Alexander H.

AU - Eddaoudi, Mohamed

AU - Sargent, E.

AU - Sinton, David

N1 - KAUST Repository Item: Exported on 2023-01-17 Acknowledgements: 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).

PY - 2023/1/12

Y1 - 2023/1/12

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.

UR - http://hdl.handle.net/10754/687121

UR - https://www.nature.com/articles/s41560-022-01188-2

U2 - 10.1038/s41560-022-01188-2

DO - 10.1038/s41560-022-01188-2

M3 - Article

SN - 2058-7546

JO - Nature Energy

JF - Nature Energy

ER -

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

Abstract

Bibliographical note

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this