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具有更高稳定性的VO/γ-Al₂O₃催化剂上羟基介导的非氧化丙烷脱氢反应

Hydroxyl-Mediated Non-oxidative Propane Dehydrogenation over VO /γ-Al O Catalysts with Improved Stability.

作者信息

Zhao Zhi-Jian, Wu Tengfang, Xiong Chuanye, Sun Guodong, Mu Rentao, Zeng Liang, Gong Jinlong

机构信息

Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering, Weijin Road 92, Tianjin, 300072, China.

出版信息

Angew Chem Int Ed Engl. 2018 Jun 4;57(23):6791-6795. doi: 10.1002/anie.201800123. Epub 2018 May 17.

Abstract

Supported vanadium oxides are one of the most promising alternative catalysts for propane dehydrogenation (PDH) and efforts have been made to improve its catalytic performance. However, unlike Pt-based catalysts, the nature of the active site and surface structure of the supported vanadium catalysts under reductive reaction conditions still remain elusive. This paper describes the surface structure and the important role of surface-bound hydroxyl groups on VO  / γ-Al O catalysts under reaction conditions employing in situ DRIFTS experiments and DFT calculations. It is shown that hydroxyl groups on the VO  /Al O catalyst (V-OH) are produced under H pre-reduction, and the catalytic performance for PDH is closely connected to the concentration of V-OH species on the catalyst. The hydroxyl groups are found to improve the catalyst that leads to better stability by suppressing the coke deposition.

摘要

负载型钒氧化物是丙烷脱氢(PDH)最有前景的替代催化剂之一,人们已努力提高其催化性能。然而,与铂基催化剂不同,负载型钒催化剂在还原反应条件下的活性位点性质和表面结构仍然难以捉摸。本文利用原位漫反射红外傅里叶变换光谱(DRIFTS)实验和密度泛函理论(DFT)计算,描述了反应条件下VO  /γ-Al₂O₃催化剂的表面结构以及表面结合羟基的重要作用。结果表明,VO  /Al₂O₃催化剂上的羟基(V-OH)是在氢气预还原条件下产生的,并且PDH的催化性能与催化剂上V-OH物种的浓度密切相关。发现羟基通过抑制积炭来改善催化剂,从而使其具有更好的稳定性。

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