4.6 Article

Ni-Zn supported defective carbon with multi-functional catalytic sites for Baeyer-Villiger reaction using air as oxidant

期刊

JOURNAL OF MATERIALS SCIENCE
卷 56, 期 26, 页码 14684-14699

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SPRINGER
DOI: 10.1007/s10853-021-06197-2

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资金

  1. National Natural Science Foundation of China [21773195]
  2. Guangdong Basic and Applied Basic Research Foundation [2020A1515110904]
  3. State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University
  4. Xiamen University

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Ni/Zn supported defective carbon catalyst with multi-functional catalytic sites was synthesized via a two-step pyrolysis-H2O2 treatment, showing high catalytic activity and selectivity for Baeyer-Villiger oxidation. The H2O2 treatment led to the formation of active N/O-group on the catalyst surface, facilitating substrate adsorption and reaction efficiency. The synergistic effect between multi-functional sites enhanced oxygen insertion efficiency for lactone formation, providing insight for exploring versatile solid catalysts for oxidative reactions.
The development of economic catalysts for aerobic oxidation procedure has attracted extensive attention. In this work, a novel Ni/Zn supported defective carbon with multi-functional catalytic sites was fabricated via a two-step pyrolysis-H2O2 treatment. The catalyst was applied to the Baeyer-Villiger (B-V) oxidation using ambient air as a green and safe oxidant. The catalyst with optimal Ni/Zn ratio of (2:1) delivers a high catalytic activity (>92%) and perfect selectivity (>99%) for the conversion of a wide range of substituted cyclic-ketones to the corresponding lactones. The characterization results have clarified that the H2O2 treatment leads to the formation of active N/O-group on the catalyst surface, which facilitates the adsorption of substrate/intermediate molecules and benefits the reaction. Moreover, the synergistic effect between multi-functional sites results in the buffering/stabilizing of free radicals, enhanced efficiency of oxygen insertion to form lactone. The design principle in this work is believed to shed light on the exploration of all-in-one solid catalyst for diverse oxidative reaction. [GRAPHICS] .

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