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

Jinqiang Zhang, Yufei Cao, Pengfei Ou, Geonhui Lee, Yufei Zhao, Shijie Liu, Erfan Shirzadi, Roham Dorakhan, Ke Xie, Cong Tian, Yuanjun Chen, Xiaoyan Li, Yurou Celine Xiao, Ali Shayesteh Zeraati, Rui Kai Miao, Sungjin Park, Colin P. O’Brien, Jun Ge, Xin Zhou, David Sinton () and Edward H. Sargent ()
Additional contact information
Jinqiang Zhang: University of Toronto
Yufei Cao: University of Toronto
Pengfei Ou: University of Toronto
Geonhui Lee: University of Toronto
Yufei Zhao: University of Toronto
Shijie Liu: University of Toronto
Erfan Shirzadi: University of Toronto
Roham Dorakhan: University of Toronto
Ke Xie: University of Toronto
Cong Tian: University of Toronto
Yuanjun Chen: University of Toronto
Xiaoyan Li: University of Toronto
Yurou Celine Xiao: University of Toronto
Ali Shayesteh Zeraati: University of Toronto
Rui Kai Miao: University of Toronto
Sungjin Park: University of Toronto
Colin P. O’Brien: University of Toronto
Jun Ge: Tsinghua University
Xin Zhou: South China University of Technology
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-58756-9

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