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CO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers

Hefei Li, Pengfei Wei, Tianfu Liu, Mingrun Li, Chao Wang, Rongtan Li, Jinyu Ye, Zhi-You Zhou, Shi-Gang Sun, Qiang Fu, Dunfeng Gao (), Guoxiong Wang () and Xinhe Bao
Additional contact information
Hefei Li: Chinese Academy of Sciences
Pengfei Wei: Chinese Academy of Sciences
Tianfu Liu: Chinese Academy of Sciences
Mingrun Li: Chinese Academy of Sciences
Chao Wang: Chinese Academy of Sciences
Rongtan Li: Chinese Academy of Sciences
Jinyu Ye: Xiamen University
Zhi-You Zhou: Xiamen University
Shi-Gang Sun: Xiamen University
Qiang Fu: Chinese Academy of Sciences
Dunfeng Gao: Chinese Academy of Sciences
Guoxiong Wang: Chinese Academy of Sciences
Xinhe Bao: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Producing valuable chemicals like ethylene via catalytic carbon monoxide conversion is an important nonpetroleum route. Here we demonstrate an electrochemical route for highly efficient synthesis of multicarbon (C2+) chemicals from CO. We achieve a C2+ partial current density as high as 4.35 ± 0.07 A cm−2 at a low cell voltage of 2.78 ± 0.01 V over a grain boundary-rich Cu nanoparticle catalyst in an alkaline membrane electrode assembly (MEA) electrolyzer, with a C2+ Faradaic efficiency of 87 ± 1% and a CO conversion of 85 ± 3%. Operando Raman spectroscopy and density functional theory calculations reveal that the grain boundaries of Cu nanoparticles facilitate CO adsorption and C − C coupling, thus rationalizing a qualitative trend between C2+ production and grain boundary density. A scale-up demonstration using an electrolyzer stack with five 100 cm2 MEAs achieves high C2+ and ethylene formation rates of 118.9 mmol min−1 and 1.2 L min−1, respectively, at a total current of 400 A (4 A cm−2) with a C2+ Faradaic efficiency of 64%.

Date: 2024
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DOI: 10.1038/s41467-024-49095-2

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