Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity
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...
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Nature Portfolio
2025-08-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-62875-8 |
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| author | Zekun Zhang Hua Guo Shiji Li Suihan Gao Xinyu Wang Mingtao Li Wei Yan Hao Xu |
| author_facet | Zekun Zhang Hua Guo Shiji Li Suihan Gao Xinyu Wang Mingtao Li Wei Yan Hao Xu |
| author_sort | Zekun Zhang |
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| description | 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. |
| format | Article |
| id | doaj-art-acb6ee21be2d45ea9a0e1aba11a8a5d5 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
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| series | Nature Communications |
| spelling | doaj-art-acb6ee21be2d45ea9a0e1aba11a8a5d52025-08-20T04:03:01ZengNature PortfolioNature Communications2041-17232025-08-0116111610.1038/s41467-025-62875-8Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivityZekun Zhang0Hua Guo1Shiji Li2Suihan Gao3Xinyu Wang4Mingtao Li5Wei Yan6Hao Xu7Department of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong UniversityShaanxi Key Laboratory of Macromolecular Science and Technology, School of Chemistry and Chemical Engineering, Northwestern Polytechnical UniversityDepartment of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong UniversityDepartment of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong UniversityDepartment of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong UniversityInternational Research Center for Renewable Energy (IRCRE), State Key Laboratory of Multiphase Flow in Power Engineering (MFPE), Xi’an Jiaotong UniversityDepartment of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong UniversityDepartment of Environmental Science and Engineering, School of Energy and Power Engineering, Xi’an Jiaotong UniversityAbstract 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.https://doi.org/10.1038/s41467-025-62875-8 |
| spellingShingle | Zekun Zhang Hua Guo Shiji Li Suihan Gao Xinyu Wang Mingtao Li Wei Yan Hao Xu Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity Nature Communications |
| title | Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity |
| title_full | Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity |
| title_fullStr | Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity |
| title_full_unstemmed | Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity |
| title_short | Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity |
| title_sort | cavity confined au cu2o yolk shell nanoreactors enable switchable ch4 c2h4 selectivity |
| url | https://doi.org/10.1038/s41467-025-62875-8 |
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