Dual-functional single-atomic Mo/Fe clusters–decorated C 3 N 5 via three electron-pathway in oxygen reduction reaction for tandemly removing contaminants from water

Author:

Dong Chencheng1ORCID,Wang Zhi-qiang2,Yang Chao1ORCID,Hu Xiaomeng1,Wang Pei1,Gong Xue-qing2,Lin Lin3ORCID,Li Xiao-yan13ORCID

Affiliation:

1. Department of Civil Engineering, The University of Hong Kong, Pokfulam, Hong Kong, China

2. Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

3. Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518000, China

Abstract

Inspired by the development of single-atom catalysts (SACs), the fabrication of multimetallic SACs can be a promising technical approach for the in situ electro-Fenton (EF) process. Herein, dual-functional atomically dispersed Mo–Fe sites embedded in carbon nitride (C 3 N 5 ) (i.e., MoFe/C 3 N 5 ) were synthesized via a facile SiO 2 template method. The atomically isolated bimetallic configuration in MoFe/C 3 N 5 was identified by combining the microscopic and spectroscopic techniques. The MoFe/C 3 N 5 catalyst on the cathode exhibited a remarkable catalytic activity toward the three electron-dominated oxygen reduction reaction in sodium sulfate, leading to a highly effective EF reaction with a low overpotential for the removal of organic contaminants from wastewater. The new catalyst showed a superior performance over its conventional counterparts, owing to the dual functions of the dual-metal active sites. Density functional theory (DFT) analysis revealed that the dual-functional 50-MoFe/C 3 N 5 catalyst enabled a synergistic action of the Mo–Fe dual single atomic centers, which can alter the adsorption/dissociation behavior and decrease the overall reaction barriers for effective organic oxidation during the EF process. This study not only sheds light on the controlled synthesis of atomically isolated catalyst materials but also provides deeper understanding of the structure–performance relationship of the nanocatalysts with dual active sites for the catalytic EF process. Additionally, the findings will promote the advanced catalysis for the treatment of emerging organic contaminants in water and wastewater.

Funder

Research Grants Council, University Grants Committee

MOST | National Natural Science Foundation of China

Innovation and Technology Fund

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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