Revealing the origin of single‐atom W activity in H2O2 electrocatalytic production: Charge symmetry‐breaking
Changfei Jing,
Junyang Ding,
Peipei Jia,
Mengmeng Jin,
Lihui Zhou,
Xijun Liu,
Jun Luo,
Sheng Dai
Affiliations
Changfei Jing
Institute for New Energy Materials & Low‐Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Xiqing Tianjin China
Junyang Ding
Institute for New Energy Materials & Low‐Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Xiqing Tianjin China
Peipei Jia
ShenSi Lab, Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China Longhua Shenzhen China
Mengmeng Jin
Institute for New Energy Materials & Low‐Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Xiqing Tianjin China
Lihui Zhou
Key Laboratory for Advanced Materials and Joint International Research, Laboratory of Precision Chemistry and Molecular Engineering, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering East China University of Science & Technology Xuhui Shanghai China
Xijun Liu
State Key Laboratory of Featured Metal Materials and Life−cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non‐ferrous Metals and Featured Materials, MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials, School of Resources, Environment and Materials Guangxi University Nanning Guangxi China
Jun Luo
ShenSi Lab, Shenzhen Institute for Advanced Study University of Electronic Science and Technology of China Longhua Shenzhen China
Sheng Dai
Key Laboratory for Advanced Materials and Joint International Research, Laboratory of Precision Chemistry and Molecular Engineering, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering East China University of Science & Technology Xuhui Shanghai China
Abstract The low‐energy electrochemical production of hydrogen peroxide (H2O2) has garnered significant attention as a viable alternative to traditional industrial routes, with the goal of achieving carbon neutrality. For their H2O2 selectivity in the two‐electron oxygen reduction reaction (ORR), the coordination environment of tungsten (W)‐based materials is critical. In this study, atomically dispersed W single atoms were immobilized on N‐doped carbon substrates by a facile pyrolysis method to obtain a W single‐atom catalyst (W‐SAC). The coordination environment of an isolated W single atom with a tetra‐coordinated porphyrin‐like structure in W‐SAC was determined by X‐ray photoelectron spectroscopy and X‐ray absorption spectroscopy analysis. Notably, the as‐prepared W‐SAC showed superior two‐electron ORR activity in 0.1 M KOH solution, including high onset potential (0.89 V), high H2O2 selectivity (82.5%), and excellent stability. By using differential phase contrast‐scanning transmission electron microscopy and density functional theory calculations, it is revealed that the charge symmetry‐breaking of W atoms changes the adsorption behavior of the intermediates, leading to enhanced reactivity and selectivity for two‐electron ORR. This work broadens the avenue for understanding the charge transfer of W‐based electrocatalytic materials and the in‐depth reaction mechanism of SACs in two‐electron ORR.
