Affiliation:
1. Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology Guangzhou 510640 P. R. China
2. Analytical and Testing Centre South China University of Technology Guangzhou 510640 P. R. China
Abstract
AbstractTuning the coordination structures of metal sites is intensively studied to improve the performances of single‐atom site catalysts (SASC). However, the pore structure of SASC, which is highly related to the accessibility of active sites, has received little attention. In this work, single‐atom ZnN4 sites embedded in P‐functionalized carbon with hollow‐wall and 3D ordered macroporous structure (denoted as H‐3DOM‐ZnN4/P‐C) are constructed. The creation of hollow walls in ordered macroporous structures can largely increase the external surface area to expose more active sites. The introduction of adjacent P atoms can optimize the electronic structure of ZnN4 sites through long‐rang regulation to enhance the intrinsic activity and selectivity. In the electrochemical CO2 reduction reaction, H‐3DOM‐ZnN4/P‐C exhibits high CO Faradaic efficiency over 90% in a wide potential window (500 mV) and a large turnover frequency up to 7.8 × 104 h−1 at −1.0 V versus reversible hydrogen electrode, much higher than its counterparts without the hierarchically ordered structure or P‐functionalization.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Guangdong Province
Fundamental Research Funds for the Central Universities
Subject
General Physics and Astronomy,General Engineering,Biochemistry, Genetics and Molecular Biology (miscellaneous),General Materials Science,General Chemical Engineering,Medicine (miscellaneous)