Oxygen-Mediated Hydrogen Spillover Promotes Stable Synthesis of Vinyl Chloride on Ru Single-Atom Catalysts
Yurui Fan
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorCorresponding Author
Dr. Haomiao Xu
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorMingming Wang
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorZhisong Liu
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003 China
Search for more papers by this authorHongyuan Qi
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorWenjun Huang
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorLei Ma
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorFeng Yu
State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003 China
Search for more papers by this authorZan Qu
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorCorresponding Author
Dr. Pengfei Xie
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310058 China
Search for more papers by this authorBin Dai
State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003 China
Search for more papers by this authorNaiqiang Yan
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092 China
Search for more papers by this authorYurui Fan
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorCorresponding Author
Dr. Haomiao Xu
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorMingming Wang
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorZhisong Liu
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003 China
Search for more papers by this authorHongyuan Qi
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorWenjun Huang
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorLei Ma
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorFeng Yu
State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003 China
Search for more papers by this authorZan Qu
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Search for more papers by this authorCorresponding Author
Dr. Pengfei Xie
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310058 China
Search for more papers by this authorBin Dai
State Key Laboratory Incubation Base for Green Processing of Chemical Engineering, School of Chemistry and Chemical Engineering, Shihezi University, Shihezi, 832003 China
Search for more papers by this authorNaiqiang Yan
School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092 China
Search for more papers by this authorAbstract
Ru single-atom catalysts hold great promise for the robust synthesis of vinyl chloride through acetylene hydrochlorination. However, the easy over-chlorination of Ru atoms during reaction suppress the catalytic activity and stability. Herein, we have synthesized an oxygen doped Ru single-atom catalyst by a sequential oxygen etching strategy, which delivers the remarkable yield of vinyl chloride monomer (>99.38 %) and stability (>900 h, 180 h−1), far beyond those reported Ru counterparts. Experimental results and theoretical calculations reveal that the asymmetric structure of single-atom Ru promotes an unconventional oxygen-mediated hydrogen spillover after the activation of hydrogen chloride, which enables the reaction to proceed through Eley-Rideal mechanism with a reduced energy barrier of acetylene hydrochlorination compared to the traditional Langmuir–Hinshelwood pathway. As a result, the enhanced reaction kinetics further restrict over-chlorination of single-atom Ru, thereby ensuring the excellent durability. This work offers a strategy for designing multifunctional catalysts with enhanced performances for acetylene hydrochlorination.
Conflict of Interests
The authors declare no conflict of interest
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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