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High selective epoxidation of 2-methylpropene over a Mo-based oxametallacycle reinforced nano composite

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Abstract

Compared with the gas-solid phase reactions, the epoxidation of light olefins in the liquid phase could realize the highly selective preparation of epoxides at a lower temperature. Nevertheless, the C-C bond of light olefins is more difficult to activate, and it is still a challenge to realize the dual activation of the oxidant and light olefins in one reaction system. In this contribution, an oxametallacycle reinforced nanocomposite (Mo(O2)2@RT) is prepared via an oxidative pretreatment strategy, and its epoxidation performance to 2-methylpropene in liquid-phase with tert-butyl hydroperoxide (TBHP) as an oxidant is evaluated. A set of advanced characterizations including field emission scanning electron microscopy, X-ray photoelectron spectroscopy, in-situ Fourier transform infrared spectroscopy (FT-IR), electron spin-resonance spectroscopy, and high-resolution mass spectrometer are implemented to confirm the physicochemical properties and the catalytic behaviors of Mo(O2)2@RT. This catalyst has a fast kinetic response and exhibits excellent catalytic activity in 2-methylpropene epoxidation to produce 2-methylpropylene oxide (MPO; select.: 99.7%; yield: 92%), along with good reusability and scalability. Moreover, the main epoxidation mechanism is deduced that TBHP is activated by Mo(O2)2@RT to generate the highly active tert-butyl peroxide radical, which realizes the epoxidation of 2-methylpropene to yield MPO.

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Acknowledgments

This work was financially supported by the National Key Research and Development Program Nanotechnology Specific Project (No. 2020YFA0210900), the National Natural Science Foundation of China (Nos. 21908256, 21938001, and 21878344), Guangdong Provincial Key R&D Program (No. 2019B110206002), and the Fundamental Research Funds for the Central Universities, Sun Yatsen University (No. 2021qntd13).

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Authors and Affiliations

  1. Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-Sen University, Guangzhou, 510275, China

    Chao Xiong, Hao Liu, Jie Zhou & Hongbing Ji

  2. School of Chemical Engineering and Technology, Sun Yat-Sen University, Zhuhai, 519082, China

    Dejing Xu, Yichao Liang, Xiantai Zhou & Can Xue

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  1. Chao Xiong
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  2. Hao Liu
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  3. Jie Zhou
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  7. Can Xue
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  8. Hongbing Ji
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Correspondence to Can Xue or Hongbing Ji.

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Xiong, C., Liu, H., Zhou, J. et al. High selective epoxidation of 2-methylpropene over a Mo-based oxametallacycle reinforced nano composite. Nano Res. 16, 209–218 (2023). https://doi.org/10.1007/s12274-022-4686-7

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  • DOI: https://doi.org/10.1007/s12274-022-4686-7

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