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首页> 外文期刊>chem catalysis >Pushing the limit of atomically dispersed Au catalysts for electrochemical H2O2 production by precise electronic perturbation of the active site
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Pushing the limit of atomically dispersed Au catalysts for electrochemical H2O2 production by precise electronic perturbation of the active site

机译：Pushing the limit of atomically dispersed Au catalysts for electrochemical H2O2 production by precise electronic perturbation of the active site

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摘要

Exquisite electronic perturbation of atomically dispersed catalysts (ADCs) enables optimized catalytic performance while limited syn-thetic approaches are engaged at atomic precision. By leveraging the electron push-and-pull effect, herein, precise electronic pertur-bation of Au ADCs is achieved on electron-withdrawing/-donating group-functionalized graphdiyne (R-GDY; R = -OMe, -H, and -F), leading to the distinct Au charge states of +0.8, +1.2, and +1.5 for Au/OMe-GDY, Au/H-GDY, and Au/F-GDY, respectively. Remark-ably, the electrochemical O2-to-H2O2 conversion selectivity is directly scaled with the electron-withdrawing ability of the func-tional groups in a trend of -OMe < -H < -F, rendering an optimum H2O2 selectivity of 98 under alkaline conditions. In situ electro-chemical Raman study with density functional theory (DFT) calcula-tions unraveled that the dynamically evolved Au dimer with a m-bridged hydroxyl ligand acts as the active site and that the elec-tron-withdrawing groups near the Au dimer are critical to pushing the limit of the catalyst toward the electrocatalytic H2O2 production.

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