Efficient multicarbon formation in acidic CO2 reduction via tandem electrocatalysis.

Chen, Y; Li, X-Y; Chen, Z; Ozden, A; Huang, JE; Ou, P; Dong, J; Zhang, J; Tian, C; Lee, B-H; Wang, X; Liu, S; Qu, Q; Wang, S; Xu, Y; Miao, RK; Zhao, Y; Liu, Y; Qiu, C; Abed, J; Liu, H; Shin, H; Wang, D; Li, Y; Sinton, D; Sargent, EH

Efficient multicarbon formation in acidic CO2 reduction via tandem electrocatalysis.

Chen, Y Li, X-Y Chen, Z Ozden, A Huang, JE Ou, P Dong, J Zhang, J

Tian, C Lee, B-H Wang, X Liu, S Qu, Q Wang, S Xu, Y Miao, RK Zhao, Y Liu, Y Qiu, C Abed, J Liu, H Shin, H Wang, D Li, Y Sinton, D Sargent, EH

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Publisher:: Nature Research
Publication Type:: Journal Article
Citation:: Nature Nanotechnology, 2024, 19, (3), pp. 311-318
Issue Date:: 2024-11-23

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Field	Value	Language
dc.contributor.author	Chen, Y
dc.contributor.author	Li, X-Y
dc.contributor.author	Chen, Z
dc.contributor.author	Ozden, A
dc.contributor.author	Huang, JE
dc.contributor.author	Ou, P
dc.contributor.author	Dong, J
dc.contributor.author	Zhang, J https://orcid.org/0000-0001-5476-0134
dc.contributor.author	Tian, C
dc.contributor.author	Lee, B-H
dc.contributor.author	Wang, X
dc.contributor.author	Liu, S
dc.contributor.author	Qu, Q
dc.contributor.author	Wang, S
dc.contributor.author	Xu, Y
dc.contributor.author	Miao, RK
dc.contributor.author	Zhao, Y
dc.contributor.author	Liu, Y
dc.contributor.author	Qiu, C
dc.contributor.author	Abed, J
dc.contributor.author	Liu, H
dc.contributor.author	Shin, H
dc.contributor.author	Wang, D
dc.contributor.author	Li, Y
dc.contributor.author	Sinton, D
dc.contributor.author	Sargent, EH
dc.date.accessioned	2024-11-18T01:08:35Z
dc.date.available	2023-10-12
dc.date.available	2024-11-18T01:08:35Z
dc.date.issued	2024-11-23
dc.identifier.citation	Nature Nanotechnology, 2024, 19, (3), pp. 311-318
dc.identifier.issn	1748-3387
dc.identifier.issn	1748-3395
dc.identifier.uri	http://hdl.handle.net/10453/181941
dc.description.abstract	The electrochemical reduction of CO2 in acidic conditions enables high single-pass carbon efficiency. However, the competing hydrogen evolution reaction reduces selectivity in the electrochemical reduction of CO2, a reaction in which the formation of CO, and its ensuing coupling, are each essential to achieving multicarbon (C2+) product formation. These two reactions rely on distinct catalyst properties that are difficult to achieve in a single catalyst. Here we report decoupling the CO2-to-C2+ reaction into two steps, CO2-to-CO and CO-to-C2+, by deploying two distinct catalyst layers operating in tandem to achieve the desired transformation. The first catalyst, atomically dispersed cobalt phthalocyanine, reduces CO2 to CO with high selectivity. This process increases local CO availability to enhance the C-C coupling step implemented on the second catalyst layer, which is a Cu nanocatalyst with a Cu-ionomer interface. The optimized tandem electrodes achieve 61% C2H4 Faradaic efficiency and 82% C2+ Faradaic efficiency at 800 mA cm-2 at 25 °C. When optimized for single-pass utilization, the system reaches a single-pass carbon efficiency of 90 ± 3%, simultaneous with 55 ± 3% C2H4 Faradaic efficiency and a total C2+ Faradaic efficiency of 76 ± 2%, at 800 mA cm-2 with a CO2 flow rate of 2 ml min-1.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	Nature Research
dc.relation.ispartof	Nature Nanotechnology
dc.relation.isbasedon	10.1038/s41565-023-01543-8
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject.classification	Nanoscience & Nanotechnology
dc.title	Efficient multicarbon formation in acidic CO2 reduction via tandem electrocatalysis.
dc.type	Journal Article
utslib.citation.volume	19
utslib.location.activity	England
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
utslib.copyright.status	closed_access	*
pubs.consider-herdc	false
dc.date.updated	2024-11-18T01:08:34Z
pubs.issue	3
pubs.publication-status	Published online
pubs.volume	19
utslib.citation.issue	3

Abstract:

The electrochemical reduction of CO2 in acidic conditions enables high single-pass carbon efficiency. However, the competing hydrogen evolution reaction reduces selectivity in the electrochemical reduction of CO2, a reaction in which the formation of CO, and its ensuing coupling, are each essential to achieving multicarbon (C2+) product formation. These two reactions rely on distinct catalyst properties that are difficult to achieve in a single catalyst. Here we report decoupling the CO2-to-C2+ reaction into two steps, CO2-to-CO and CO-to-C2+, by deploying two distinct catalyst layers operating in tandem to achieve the desired transformation. The first catalyst, atomically dispersed cobalt phthalocyanine, reduces CO2 to CO with high selectivity. This process increases local CO availability to enhance the C-C coupling step implemented on the second catalyst layer, which is a Cu nanocatalyst with a Cu-ionomer interface. The optimized tandem electrodes achieve 61% C2H4 Faradaic efficiency and 82% C2+ Faradaic efficiency at 800 mA cm-2 at 25 °C. When optimized for single-pass utilization, the system reaches a single-pass carbon efficiency of 90 ± 3%, simultaneous with 55 ± 3% C2H4 Faradaic efficiency and a total C2+ Faradaic efficiency of 76 ± 2%, at 800 mA cm-2 with a CO2 flow rate of 2 ml min-1.

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http://hdl.handle.net/10453/181941