Controlling Metal-Oxide Reducibility for Efficient C-H Bond Activation in Hydrocarbons

doi:10.1002/anie.202310062

IMR OpenIR

	Controlling Metal-Oxide Reducibility for Efficient C-H Bond Activation in Hydrocarbons
	Yang, Guo-Qing 1,2; Niu, Yiming 3; Kondratenko, Vita A.2; Yi, Xianfeng 4; Liu, Chang 1; Zhang, Bingsen 3; Kondratenko, Evgenii V.2; Liu, Zhong-Wen 1
通讯作者	Zhang, Bingsen(bszhang@imr.ac.cn) ; Kondratenko, Evgenii V.(Evgenii.Kondratenko@catalysis.de) ; Liu, Zhong-Wen(zwliu@snnu.edu.cn)
	2023-10-09
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN	1433-7851
页码	11
摘要	Knowing the structure of catalytically active species/phases and providing methods for their purposeful generation are two prerequisites for the design of catalysts with desired performance. Herein, we introduce a simple method for precise preparation of supported/bulk catalysts. It utilizes the ability of metal oxides to dissolve and to simultaneously precipitate during their treatment in an aqueous ammonia solution. Applying this method for a conventional VOx-Al2O3 catalyst, the concentration of coordinatively unsaturated Al sites was tuned simply by changing the pH value of the solution. These sites affect the strength of V-O-Al bonds of isolated VOx species and thus the reducibility of the latter. This method is also applicable for controlling the reducibility of bulk catalysts as demonstrated for a CeO2-ZrO2-Al2O3 system. The application potential of the developed catalysts was confirmed in the oxidative dehydrogenation of ethylbenzene to styrene with CO2 and in the non-oxidative propane dehydrogenation to propene. Our approach is extendable to the preparation of any metal oxide catalysts dissolvable in an ammonia solution. Through catalyst post-treatment in an NH3 & sdot; H2O solution, structural and chemical properties of supported metal oxide species can be controlled because of dissolution-recrystallization of amorphous or/and low-crystalline support in the parent catalyst. The method is applicable for tailoring the catalyst reducibility and thus its activity for C-H activation in hydrocarbons.image
关键词	C-H Activation Dehydrogenation Reducibility Tailoring Catalyst Structure Vanadium Oxide
资助者	National Natural Science Foundation of China ; China Scholarship Council ; State of Mecklenburg-Vorpommern ; Projekt DEAL
DOI	10.1002/anie.202310062
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[21636006] ; China Scholarship Council ; State of Mecklenburg-Vorpommern ; Projekt DEAL
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001080665300001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：8[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/179380
专题	中国科学院金属研究所
通讯作者	Zhang, Bingsen; Kondratenko, Evgenii V.; Liu, Zhong-Wen
作者单位	1.Shaanxi Normal Univ, Sch Chem & Chem Engn, Key Lab Syngas Convers Shaanxi Prov, Xian 710119, Peoples R China 2.Leibniz Inst Katalyse e V, Albert Einstein Str 29a, D-18059 Rostock, Germany 3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 4.Chinese Acad Sci, Innovat Acad Precis Measurement Sci & Technol, Natl Ctr Magnet Resonance Wuhan, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China
推荐引用方式 GB/T 7714	Yang, Guo-Qing,Niu, Yiming,Kondratenko, Vita A.,et al. Controlling Metal-Oxide Reducibility for Efficient C-H Bond Activation in Hydrocarbons[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2023:11.
APA	Yang, Guo-Qing.,Niu, Yiming.,Kondratenko, Vita A..,Yi, Xianfeng.,Liu, Chang.,...&Liu, Zhong-Wen.(2023).Controlling Metal-Oxide Reducibility for Efficient C-H Bond Activation in Hydrocarbons.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,11.
MLA	Yang, Guo-Qing,et al."Controlling Metal-Oxide Reducibility for Efficient C-H Bond Activation in Hydrocarbons".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023):11.