Citation: Yonggang Sun, Ganggang Li, Jie Cheng, Na Li, Xin Xing, Xin Zhang, Zhongshen Zhang. Synergistic effect of oxygen vacancies and edging/corner-connected MnO₆ structural motifs in multi-dimensional manganese oxides to enhance OVOCs catalytic oxidation[J]. Chinese Chemical Letters, ;2023, 34(12): 108437. doi: 10.1016/j.cclet.2023.108437 shu

Synergistic effect of oxygen vacancies and edging/corner-connected MnO₆ structural motifs in multi-dimensional manganese oxides to enhance OVOCs catalytic oxidation

Yonggang Sun ^{a, b} ,
Ganggang Li ^b ,
Jie Cheng ^{b, *,} ,
Na Li ^b ,
Xin Xing ^b ,
Xin Zhang ^{c, *,} ,
Zhongshen Zhang ^b

a.
State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, School of Chemistry and Chemical Engineering, Ningxia University, Yinchuan 750021, China
b.
National Engineering Laboratory for VOCs pollution Control Material & Technology, Research Center for Environmental Material and Pollution Control Technology, University of Chinese Academy of Sciences, Beijing 101408, China
c.
College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 101408, China

jiecheng@ucas.ac.cn

xzhang@ucas.ac.cn

Received Date: 28 October 2022
Revised Date: 14 March 2023
Accepted Date: 5 April 2023
Available Online: 14 April 2023

Figures(7)

The structure-activity relationships for vinyl acetate catalytic oxidation are challenging to explore at the atomic scale due to the ambiguity of the structural defect types and sites of manganese oxides. Our work elaborates, at the atomic level, through in-situ experimental and theoretical methods, the synergistic effects of two types of structural defect sites of V_O-e (edge-sharing oxygen) and V_O-c (corner-sharing oxygen) and MnO₆ structural motifs of manganese oxides. Multi-dimensional manganese oxides, namely those with corner-connected MnO₆ structural motifs and V_O-c structural oxygen defect sites, significantly improved the activation of vinyl acetate. Enhancement of enol structure formation, acetate and formate intermediate species, and tautomerism between enol structure and acetaldehyde were detected when oxygen vacancies of manganese oxides were present in combination with corner/edge-connected MnO₆. Moreover, the activation of chemical bonds and deep catalytic oxidation of vinyl acetate depend on the presence of a redox couple, surface oxygen species, and weakened MnO bonds. It provides a valuable notion for investigating and designing catalytic systems and reaction processes for the purpose of emission reduction and the management of environmental contaminants.
- Oxygen vacancies,
- Synergistic effects,
- MnO₆ structural motifs,
- In-situ technologies,
- Catalytic oxidation
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Synergistic effect of oxygen vacancies and edging/corner-connected MnO6 structural motifs in multi-dimensional manganese oxides to enhance OVOCs catalytic oxidation

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通讯作者: 陈斌, bchen63@163.com

Synergistic effect of oxygen vacancies and edging/corner-connected MnO₆ structural motifs in multi-dimensional manganese oxides to enhance OVOCs catalytic oxidation