Stabilized Cuδ+-OH species on in situ reconstructed Cu nanoparticles for CO2-to-C2H4 conversion in neutral media

Lei Wang, Zhiwen Chen, Yi Xiao, Linke Huang, Xiyang Wang, Holly Fruehwald, Dmitry Akhmetzyanov, Mathew Hanson, Zuolong Chen, Ning Chen, Brant Billinghurst, Rodney D. L. Smith, Chandra Veer Singh (), Zhongchao Tan () and Yimin A. Wu ()
Additional contact information
Lei Wang: University of Waterloo
Zhiwen Chen: University of Toronto
Yi Xiao: University of Waterloo
Linke Huang: University of Toronto
Xiyang Wang: University of Waterloo
Holly Fruehwald: University of Waterloo
Dmitry Akhmetzyanov: University of Waterloo
Mathew Hanson: University of Waterloo
Zuolong Chen: University of Waterloo
Ning Chen: Canadian Light Source
Brant Billinghurst: Canadian Light Source
Rodney D. L. Smith: University of Waterloo
Chandra Veer Singh: University of Toronto
Zhongchao Tan: University of Waterloo
Yimin A. Wu: University of Waterloo

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

Abstract: Abstract Achieving large-scale electrochemical CO2 reduction to multicarbon products with high selectivity using membrane electrode assembly (MEA) electrolyzers in neutral electrolyte is promising for carbon neutrality. However, the unsatisfactory multicarbon products selectivity and unclear reaction mechanisms in an MEA have hindered its further development. Here, we report a strategy that manipulates the interfacial microenvironment of Cu nanoparticles in an MEA to suppress hydrogen evolution reaction and enhance C2H4 conversion. In situ multimodal characterizations consistently reveal well-stabilized Cuδ+-OH species as active sites during MEA testing. The OH radicals generated in situ from water create a locally oxidative microenvironment on the copper surface, stabilizing the Cuδ+ species and leading to an irreversible and asynchronous change in morphology and valence, yielding high-curvature nanowhiskers. Consequently, we deliver a selective C2H4 production with a Faradaic efficiency of 55.6% ± 2.8 at 316 mA cm−2 in neutral media.

Date: 2024
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DOI: 10.1038/s41467-024-52004-2

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