Improving the SO2 tolerance of CO2 reduction electrocatalysts using a polymer/catalyst/ionomer heterojunction design

Panagiotis Papangelakis, Rui Kai Miao, Ruihu Lu, Hanqi Liu, Xi Wang, Adnan Ozden, Shijie Liu, Ning Sun, Colin P. O’Brien, Yongfeng Hu, Mohsen Shakouri, Qunfeng Xiao, Mengsha Li, Behrooz Khatir, Jianan Erick Huang, Yakun Wang, Yurou Celine Xiao, Feng Li, Ali Shayesteh Zeraati, Qiang Zhang, Pengyu Liu, Kevin Golovin, Jane Y. Howe, Hongyan Liang, Ziyun Wang (), Jun Li (), Edward H. Sargent and David Sinton ()
Additional contact information
Panagiotis Papangelakis: University of Toronto
Rui Kai Miao: University of Toronto
Ruihu Lu: University of Auckland
Hanqi Liu: Shanghai Jiao Tong University
Xi Wang: Shanghai Jiao Tong University
Adnan Ozden: University of Toronto
Shijie Liu: University of Toronto
Ning Sun: Shanghai Jiao Tong University
Colin P. O’Brien: University of Toronto
Yongfeng Hu: Sinopec Shanghai Research Institute of Petrochemical Technology
Mohsen Shakouri: University of Saskatchewan
Qunfeng Xiao: University of Saskatchewan
Mengsha Li: University of Toronto
Behrooz Khatir: University of Toronto
Jianan Erick Huang: University of Toronto
Yakun Wang: University of Toronto
Yurou Celine Xiao: University of Toronto
Feng Li: University of Toronto
Ali Shayesteh Zeraati: University of Toronto
Qiang Zhang: Shanghai Jiao Tong University
Pengyu Liu: Shanghai Jiao Tong University
Kevin Golovin: University of Toronto
Jane Y. Howe: University of Toronto
Hongyan Liang: Tianjin University
Ziyun Wang: University of Auckland
Jun Li: Shanghai Jiao Tong University
Edward H. Sargent: University of Toronto
David Sinton: University of Toronto

Nature Energy, 2024, vol. 9, issue 8, 1011-1020

Abstract: Abstract The high concentrations of CO2 in industrial flue gases make these point sources attractive candidates for renewably powered electrocatalytic conversion of CO2 to products. However, trace SO2 in common flue gases rapidly and irreversibly poisons catalysts. Here we report that limiting hydrogen adsorption in the vicinity of electrochemically active sites deactivates SO2 to enable efficient CO2 conversion. We realize this approach via a polymer/catalyst/ionomer heterojunction design with combined hydrophobic and highly charged hydrophilic domains that diminish hydrogen adsorption and promote CO2 over SO2 transport. We develop an SO2-tolerant system that maintains ~50% faradaic efficiency towards multi-carbon products for over 150 h (at 100 mA cm–2). Extending this strategy to a high-surface-area composite catalyst, we achieve faradaic efficiencies of 84%, partial current densities of up to 790 mA cm–2 and energy efficiencies of ~25% towards multi-carbon products with a CO2 stream containing 400 ppm SO2, a performance that is competitive with the best reports using pure CO2.

Date: 2024
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DOI: 10.1038/s41560-024-01577-9

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