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用于高效光驱动CH偶联的含镁层状双氢氧化物纳米片的拓扑转变

Topological Transformation of Mg-Containing Layered Double Hydroxide Nanosheets for Efficient Photodriven CH Coupling.

作者信息

Xu Yanqi, Sun Xiaoliang, Wang Xian, He Lunhua, Wharmby Michael T, Hua Xiao, Zhao Yufei, Song Yu-Fei

机构信息

State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.

Key Laboratory of New Processing Technology for Nonferrous Metal & Materials, Ministry of Education, Guangxi Key Laboratory of Optical and Electronic Materials and Devices, Guilin University of Technology, Guilin, 541004, P. R. China.

出版信息

Chemistry. 2021 Sep 15;27(52):13211-13220. doi: 10.1002/chem.202101428. Epub 2021 Aug 20.

Abstract

Direct conversion of methane (CH ) to fuels and other high value-added chemicals is an attractive technology in the chemical industry; however, practical challenges to sustainable processes remain. Herein, we report the preparation of a heterostructured Co-doped MgO-based catalyst through topological transformation of a MgCo-layered double hydroxide (LDH) calcination from 200 to 1100 °C. Remarkably, the catalyst can activate CH coupling to produce C H with a selectivity of 41.60 % within 3 h under full-spectrum irradiation through calcination of LDH at 800 °C. Characterization studies and catalytic results suggest that the highly dispersed active sites and large interfaces amongst the Co-doped MgO-based catalysts enable surface activation of CH to methyl (CH *), in turn promoting coupling of CH * to C H . This study introduces a promising pathway for photodriven CH coupling to give high value-added chemicals by using layered double hydroxides as a precursor.

摘要

将甲烷(CH₄)直接转化为燃料和其他高附加值化学品是化学工业中一项颇具吸引力的技术;然而,可持续工艺仍面临实际挑战。在此,我们报道了通过将MgCo层状双氢氧化物(LDH)在200至1100°C下煅烧进行拓扑转变来制备异质结构的Co掺杂MgO基催化剂。值得注意的是,通过在800°C下煅烧LDH,该催化剂在全光谱照射下3小时内可激活CH₄偶联以41.60%的选择性生成C₂H₄。表征研究和催化结果表明,Co掺杂MgO基催化剂中高度分散的活性位点和大量界面能够使CH₄在表面活化为甲基(CH₃*),进而促进CH₃*偶联生成C₂H₄。本研究引入了一条有前景的途径,即通过使用层状双氢氧化物作为前驱体,实现光驱动CH₄偶联以制备高附加值化学品。

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