TY - JOUR
T1 - Cavity-confined Au@Cu2O yolk-shell nanoreactors enable switchable CH4/C2H4 selectivity
AU - Zhang, Zekun
AU - Guo, Hua
AU - Li, Shiji
AU - Gao, Suihan
AU - Wang, Xinyu
AU - Li, Mingtao
AU - Yan, Wei
AU - Xu, Hao
N1 - Publisher Copyright:
© The Author(s) 2025.
PY - 2025/12
Y1 - 2025/12
N2 - 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.
AB - 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.
UR - https://www.scopus.com/pages/publications/105013327826
U2 - 10.1038/s41467-025-62875-8
DO - 10.1038/s41467-025-62875-8
M3 - 文章
C2 - 40813392
AN - SCOPUS:105013327826
SN - 2041-1723
VL - 16
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 7559
ER -