选择性
电化学
催化作用
二聚体
密度泛函理论
检出限
材料科学
拉曼光谱
电子
物理
计算化学
物理化学
化学
电极
量子力学
有机化学
色谱法
光学
作者
Haiyuan Zou,Lakshitha Jasin Arachchige,Hao Dai,Hong Liu,Fangfang Jiao,Wei Hu,Fan Li,Shuting Wei,Chenghua Sun,Lele Duan
出处
期刊:Chem catalysis
[Elsevier]
日期:2023-04-01
卷期号:3 (4): 100583-100583
被引量:3
标识
DOI:10.1016/j.checat.2023.100583
摘要
Exquisite electronic perturbation of atomically dispersed catalysts (ADCs) enables optimized catalytic performance while limited synthetic approaches are engaged at atomic precision. By leveraging the electron push-and-pull effect, herein, precise electronic perturbation 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. Remarkably, the electrochemical O2-to-H2O2 conversion selectivity is directly scaled with the electron-withdrawing ability of the functional groups in a trend of –OMe < –H < –F, rendering an optimum H2O2 selectivity of 98% under alkaline conditions. In situ electrochemical Raman study with density functional theory (DFT) calculations unraveled that the dynamically evolved Au dimer with a μ-bridged hydroxyl ligand acts as the active site and that the electron-withdrawing groups near the Au dimer are critical to pushing the limit of the catalyst toward the electrocatalytic H2O2 production.
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