Selective and stable CO2 electroreduction at high rates via control of local H2O/CO2 ratio

Junmei Chen, Haoran Qiu, Yilin Zhao, Haozhou Yang, Lei Fan, Zhihe Liu, ShiBo Xi, Guangtai Zheng, Jiayi Chen, Lei Chen, Ya Liu, Liejin Guo and Lei Wang ()
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Junmei Chen: National University of Singapore
Haoran Qiu: National University of Singapore
Yilin Zhao: National University of Singapore
Haozhou Yang: National University of Singapore
Lei Fan: National University of Singapore
Zhihe Liu: National University of Singapore
ShiBo Xi: Energy & Environment, A*STAR
Guangtai Zheng: National University of Singapore
Jiayi Chen: National University of Singapore
Lei Chen: National University of Singapore
Ya Liu: Xi’an Jiaotong University
Liejin Guo: Xi’an Jiaotong University
Lei Wang: National University of Singapore

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

Abstract: Abstract Controlling the concentrations of H2O and CO2 at the reaction interface is crucial for achieving efficient electrochemical CO2 reduction. However, precise control of these variables during catalysis remains challenging, and the underlying mechanisms are not fully understood. Herein, guided by a multi-physics model, we demonstrate that tuning the local H2O/CO2 concentrations is achievable by thin polymer coatings on the catalyst surface. Beyond the often-explored hydrophobicity, polymer properties of gas permeability and water-uptake ability are even more critical for this purpose. With these insights, we achieve CO2 reduction on copper with Faradaic efficiency exceeding 87% towards multi-carbon products at a high current density of −2 A cm−2. Encouraging cathodic energy efficiency (>50%) is also observed at this high current density due to the substantially reduced cathodic potential. Additionally, we demonstrate stable CO2 reduction for over 150 h at practically relevant current densities owning to the robust reaction interface. Moreover, this strategy has been extended to membrane electrode assemblies and other catalysts for CO2 reduction. Our findings underscore the significance of fine-tuning the local H2O/CO2 balance for future CO2 reduction applications.

Date: 2024
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DOI: 10.1038/s41467-024-50269-1

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