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

Author

Listed:
  • 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)

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.

Suggested Citation

  • Zekun Zhang & Hua Guo & Shiji Li & Suihan Gao & Xinyu Wang & Mingtao Li & Wei Yan & Hao Xu, 2025. "Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity," Nature Communications, Nature, vol. 16(1), pages 1-16, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-62875-8
    DOI: 10.1038/s41467-025-62875-8
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