Theory-Driven Design of Electrocatalysts for the Two-Electron Oxygen Reduction Reaction Based on Dispersed Metal Phthalocyanines

Yang,Wang1; Zisheng,Zhang2; Xiao,Zhang3; Yubo,Yuan1; Zhan,Jiang1; Hongzhi,Zheng1; Yang-Gang,Wang2; Hua,Zhou4; Yongye,Liang1,5

2021-03-24

10.31635/ccschem.021.202000590

CCS Chemistry   影响因子和分区

2096-5745

2096-5745

The two-electron electrochemical reduction of oxygen is an appealing approach to produce hydrogen peroxide. Metal and heteroatom-doped carbon (M-X/C) materials have recently been recognized as compelling catalysts for this process, but their performance improvement is generally hindered by the ill-defined structures of active sites. Herein, we demonstrate a theory-driven design of catalysts for oxygen reduction reactions based on molecularly dispersed electrocatalysts (MDEs) with metal phthalocyanines on carbon nanotubes. Density functional theory calculations suggest that nickel phthalocyanine (NiPc) favors the formation of *H2O2 over *O, thus acting as a selective catalyst for peroxide production. NiPc MDE shows high peroxide yields of similar to 83%, superior to the aggregated NiPc and pyrolyzed Ni-N/C catalysts. The performance is further enhanced by the introduction of the cyano group (CN). NiPc-CN MDE exhibits similar to 92% peroxide yields and good stability. Our studies provide a new perspective for the development of heterogeneous electrocatalysts for hydrogen peroxide production from metal macrocyclic complexes.

metal phthalocyanine oxygen reduction reaction peroxide theory-driven design molecular engineering

ESCI

英语

第一 ; 共同第一 ; 通讯

Guangdong-Hong KongMacao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices[2019B121205001] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Chemistry

Chemistry, Multidisciplinary

WOS:000794257100019

Chinese Chemical Society

人工提交

1.Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055,
2.Department of Chemistry, Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen 518055
3.State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027,
4.X-Ray Science Division, Advanced Photon Source, Argonne National Laboratory, Lemont, IL 60439
5.Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Southern University of Science and Technology, Shenzhen 518055

Yang,Wang,Zisheng,Zhang,Xiao,Zhang,et al. Theory-Driven Design of Electrocatalysts for the Two-Electron Oxygen Reduction Reaction Based on Dispersed Metal Phthalocyanines[J]. CCS Chemistry,2021,4(1):585-593.

Yang,Wang.,Zisheng,Zhang.,Xiao,Zhang.,Yubo,Yuan.,Zhan,Jiang.,...&Yongye,Liang.(2021).Theory-Driven Design of Electrocatalysts for the Two-Electron Oxygen Reduction Reaction Based on Dispersed Metal Phthalocyanines.CCS Chemistry,4(1),585-593.

Yang,Wang,et al."Theory-Driven Design of Electrocatalysts for the Two-Electron Oxygen Reduction Reaction Based on Dispersed Metal Phthalocyanines".CCS Chemistry 4.1(2021):585-593.