A redox-active polymeric network facilitates electrified reactive-capture electrosynthesis to multi-carbon products from dilute CO2-containing streams.

Zhang, J; Cao, Y; Ou, P; Lee, G; Zhao, Y; Liu, S; Shirzadi, E; Dorakhan, R; Xie, K; Tian, C; Chen, Y; Li, X; Xiao, YC; Shayesteh Zeraati, A; Miao, RK; Park, S; O'Brien, CP; Ge, J; Zhou, X; Sinton, D; Sargent, EH

A redox-active polymeric network facilitates electrified reactive-capture electrosynthesis to multi-carbon products from dilute CO2-containing streams.

Cao, Y Ou, P Lee, G Zhao, Y Liu, S Shirzadi, E Dorakhan, R Xie, K Tian, C Chen, Y Li, X Xiao, YC Shayesteh Zeraati, A Miao, RK Park, S O'Brien, CP Ge, J Zhou, X Sinton, D Sargent, EH

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Publisher:: NATURE PORTFOLIO
Publication Type:: Journal Article
Citation:: Nat Commun, 2025, 16, (1), pp. 3553
Issue Date:: 2025-04-15

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Field	Value	Language
dc.contributor.author	Zhang, J https://orcid.org/0000-0001-5476-0134
dc.contributor.author	Cao, Y
dc.contributor.author	Ou, P
dc.contributor.author	Lee, G
dc.contributor.author	Zhao, Y
dc.contributor.author	Liu, S
dc.contributor.author	Shirzadi, E
dc.contributor.author	Dorakhan, R
dc.contributor.author	Xie, K
dc.contributor.author	Tian, C
dc.contributor.author	Chen, Y
dc.contributor.author	Li, X
dc.contributor.author	Xiao, YC
dc.contributor.author	Shayesteh Zeraati, A
dc.contributor.author	Miao, RK
dc.contributor.author	Park, S
dc.contributor.author	O'Brien, CP
dc.contributor.author	Ge, J
dc.contributor.author	Zhou, X
dc.contributor.author	Sinton, D
dc.contributor.author	Sargent, EH
dc.date.accessioned	2025-07-15T06:21:50Z
dc.date.available	2025-03-28
dc.date.available	2025-07-15T06:21:50Z
dc.date.issued	2025-04-15
dc.identifier.citation	Nat Commun, 2025, 16, (1), pp. 3553
dc.identifier.issn	2041-1723
dc.identifier.issn	2041-1723
dc.identifier.uri	http://hdl.handle.net/10453/188351
dc.description.abstract	Reactive capture - the integration of CO2 capture with electrochemical upgrade - offers the prospect of improving overall energy efficiency in captured-CO2-to-fuels by eliminating the gas-phase CO2 desorption step, and by further offering a CO2-free gas product stream. Two related challenges limit the potential impact of electrified reactive capture today: its propensity to produce lower-value C1 products (carbon products containing one carbon atom per molecule); and its failure to retain performance when fed dilute streams (e.g. ~1-10% CO2). We posit that these could be addressed using catalysts that locally concentrate and activate in-situ generated CO2: we integrate a redox-active polymeric network whose polymer fragments undergo reversible reduction during the electrochemical conversion process, enabling electron transfer to CO2 molecules generated in-situ from carbonate capture liquid. We report as a result a 55 ± 5% C2+ (carbon products containing two or more carbon atoms per molecule) Faradaic efficiency (FE) at 300 mA/cm2 in an electrochemical reactive capture system in which the electrolysis stage is fed with 1 M K2CO3. We obtain 56 ± 4 wt% C2H4 in the product gas stream. When we use a dilute stream consisting of 1% CO2 in N2 at the KOH capture stage, we retain the C2+ FE to within 85% (relative) of its value achieved in the case of pure CO2.
dc.format	Electronic
dc.language	eng
dc.publisher	NATURE PORTFOLIO
dc.relation.ispartof	Nat Commun
dc.relation.isbasedon	10.1038/s41467-025-58756-9
dc.rights	info:eu-repo/semantics/openAccess
dc.title	A redox-active polymeric network facilitates electrified reactive-capture electrosynthesis to multi-carbon products from dilute CO2-containing streams.
dc.type	Journal Article
utslib.citation.volume	16
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	open_access	*
dc.rights.license	This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License (CC BY-NC-ND 4.0). To view a copy of this license, visit https://creativecommons.org/licenses/by-nc-nd/4.0/
dc.date.updated	2025-07-15T06:21:47Z
pubs.issue	1
pubs.publication-status	Published online
pubs.volume	16
utslib.citation.issue	1

Abstract:

Reactive capture - the integration of CO2 capture with electrochemical upgrade - offers the prospect of improving overall energy efficiency in captured-CO2-to-fuels by eliminating the gas-phase CO2 desorption step, and by further offering a CO2-free gas product stream. Two related challenges limit the potential impact of electrified reactive capture today: its propensity to produce lower-value C1 products (carbon products containing one carbon atom per molecule); and its failure to retain performance when fed dilute streams (e.g. ~1-10% CO2). We posit that these could be addressed using catalysts that locally concentrate and activate in-situ generated CO2: we integrate a redox-active polymeric network whose polymer fragments undergo reversible reduction during the electrochemical conversion process, enabling electron transfer to CO2 molecules generated in-situ from carbonate capture liquid. We report as a result a 55 ± 5% C2+ (carbon products containing two or more carbon atoms per molecule) Faradaic efficiency (FE) at 300 mA/cm2 in an electrochemical reactive capture system in which the electrolysis stage is fed with 1 M K2CO3. We obtain 56 ± 4 wt% C2H4 in the product gas stream. When we use a dilute stream consisting of 1% CO2 in N2 at the KOH capture stage, we retain the C2+ FE to within 85% (relative) of its value achieved in the case of pure CO2.

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http://hdl.handle.net/10453/188351