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

Zou，Haiyuan1; Arachchige，Lakshitha Jasin2,3; Dai，Hao1; Liu，Hong1; Jiao，Fangfang4; Hu，Wei4; Li，Fan1; Wei，Shuting1; Sun，Chenghua2,3; Duan，Lele1

2023-04-20

10.1016/j.checat.2023.100583

Chem Catalysis   影响因子和分区

2667-1107

2667-1093

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 O-to-HO conversion selectivity is directly scaled with the electron-withdrawing ability of the functional groups in a trend of –OMe < –H < –F, rendering an optimum HO 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 HO production.

atomically dispersed Au catalysts electrochemical O2 reduction reaction electronic perturbation functionalized graphdiyne hydrogen peroxide SDG7: Affordable and clean energy

ESCI

英语

第一 ; 通讯

Department of Education of Guangdong Province[2020KTSCX121];National Natural Science Foundation of China[22179057];

Chemistry

Chemistry, Physical

WOS:000984844800001

ELSEVIER

2-s2.0-85152583812

Scopus

1.Department of Chemistry and Shenzhen Grubbs Institute,Southern University of Science and Technology,Shenzhen,518055,China
2.Department of Chemistry & Biotechnology,Swinburne University of Technology,Hawthorn,3122,Australia
3.School of Chemical Engineering and Energy Technology,Dongguan University of Technology,Dongguan,523808,China
4.Shandong Provincial Key Laboratory of Molecular Engineering,School of Chemistry and Chemical Engineering,Qilu University of Technology-Shandong,Academy of Sciences Jinan,Shandong,250353,China

Zou，Haiyuan,Arachchige，Lakshitha Jasin,Dai，Hao,et al. Pushing the limit of atomically dispersed Au catalysts for electrochemical H2O2 production by precise electronic perturbation of the active site[J]. Chem Catalysis,2023,3(4).

Zou，Haiyuan.,Arachchige，Lakshitha Jasin.,Dai，Hao.,Liu，Hong.,Jiao，Fangfang.,...&Duan，Lele.(2023).Pushing the limit of atomically dispersed Au catalysts for electrochemical H2O2 production by precise electronic perturbation of the active site.Chem Catalysis,3(4).

Zou，Haiyuan,et al."Pushing the limit of atomically dispersed Au catalysts for electrochemical H2O2 production by precise electronic perturbation of the active site".Chem Catalysis 3.4(2023).