High selective epoxidation of 2-methylpropene over a Mo-based oxametallacycle reinforced nano composite
作者机构：Fine Chemical Industry Research InstituteSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China School of Chemical Engineering and TechnologySun Yat-Sen UniversityZhuhai 519082China
出 版 物：《Nano Research》 (纳米研究（英文版）)
年 卷 期：2023年第16卷第1期
页 面：209-218页
核心收录：
学科分类：07[理学] 0804[工学-仪器科学与技术] 070303[理学-有机化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学]
基 金：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) the Fundamental Research Funds for the Central Universities,Sun Yatsen University(No.2021qntd13).
主 题：oxidative pretreatment Mo(O_(2))_(2)@RT composite 2-methylpropene epoxidation dual activation radical mechanism
摘 要：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(O_(2))_(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(O_(2))_(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(O_(2))_(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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