Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity

Zekun Zhang, Hua Guo, Shiji Li, Suihan Gao, Xinyu Wang, Mingtao Li, Wei Yan and Hao Xu ()
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Zekun Zhang: Xi’an Jiaotong University
Hua Guo: Northwestern Polytechnical University
Shiji Li: Xi’an Jiaotong University
Suihan Gao: Xi’an Jiaotong University
Xinyu Wang: Xi’an Jiaotong University
Mingtao Li: Xi’an Jiaotong University
Wei Yan: Xi’an Jiaotong University
Hao Xu: Xi’an Jiaotong University

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

Abstract: Abstract The regulation of product selectivity in electrochemical CO2 reduction (ECO2R) remains fundamentally constrained by the dynamic equilibrium between intermediate transport and surface coverage. In this study, we report a progress in catalytic architecture through precision-engineered Au@Cu2O yolk-shell tandem nanoreactors featuring dual-tunable parameters: cavity confinement dimensions and shell thickness gradients. This structural modulation enables dynamic control over both *CO intermediate enrichment and reaction pathway bifurcation. ECO2R performance evaluations demonstrate significant product selectivity switching at −1.31 V (vs. reversible hydrogen electrode (RHE)). The Faradaic efficiency (FE) for CH4 exhibits significant architectural dependence, increasing from 43.02% (thick-shell/large-cavity) to 65.54% (medium-dimension) and then decreasing to 23.26% (thin-shell/small-cavity). Conversely, the FE for C2H4 demonstrates an inverse structural correlation, improving from 6.68% (medium-dimension) to 38.73% (thin-shell/small-cavity). The spatial domain-limiting mechanism of the yolk-shell structure directly controls the transition between protonation-dominated CH4 formation and coupling-driven C2H4 production. This work establishes a pioneering paradigm for dynamically steering catalytic selectivity through purely geometrical modulation, bypassing traditional compositional tuning limitations, thereby opening avenues for precision design of advanced electrocatalytic systems.

Date: 2025
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DOI: 10.1038/s41467-025-62875-8

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