Preparation of methyl acrylate from methyl acetate and methanol with mild catalysis of cobalt complex

doi:10.1016/j.cej.2018.11.106

	Preparation of methyl acrylate from methyl acetate and methanol with mild catalysis of cobalt complex
	Wang, Gang 1,2; Li, Zengxi 1,2; Li, Chunshan 1,2; Zhang, Suojiang 2
刊名	CHEMICAL ENGINEERING JOURNAL
	2019-03-01
卷号	359 页码:863-873
关键词	Methyl acrylate Cobalt complex Aldol condensation Mechanism Kinetic
ISSN号	1385-8947
DOI	10.1016/j.cej.2018.11.106
英文摘要	The activation and selectivity are the challenging problems always existing in the utilization of methanol as C-1 resource. Herein, a novel cobalt complex catalyzed process for preparation of methyl acrylate from methyl acetate and methanol at 50 degrees C-80 degrees C was firstly developed. Such cobalt complex stabilized with a PN5P-type pincer ligand, which can be easily prepared in gram scale, has high catalytic performance with the loading amount of only 5 mol.%. Systematic mechanism investigation revealed the cobalt complex activated by sodium methoxide via salt elimination could simultaneously interact with and catalyze the dehydrogenation of two-fold methanol into formaldehyde, followed by proceeding aldol condensation with methyl acetate in the presence of sodium methoxide. Besides the reaction atmosphere of O-2 was proved to be crucial for preventing the further hydrogenation of methyl acrylate into methyl propionate. Also, the mechanism-based kinetic model indicated the dehydrogenation of methanol was rate-controlling step with the activation energy of 89.0 +/- 1.1 kJ/mol.
资助项目	National Key Projects for Fundamental Research and Development of China[2016YFB0601303] ; Key Research Program of Frontier Sciences[QYZDB-SSW-SLH022] ; International Cooperation and Exchange of the National Natural Science Foundation of China[51561145020] ; National Natural Science Fund for Distinguished Young Scholars[21425625] ; Key Program of National Natural Science Foundation of China[91434203] ; National Natural Science Foundation of China[21676270] ; NSFC-Key Projects of Shanxi Coal Based Low Carbon Joint Foundation[U1610222] ; National Natural Science Funds of Key Research Program of Frontier Sciences, CAS[QYZDB-SSW-SLH022] ; National Natural Science Funds[21878293]
WOS关键词	ALPHA-ALKYLATION ; ALDOL CONDENSATION ; ONE-STEP ; TRANSFER HYDROGENATION ; N-ALKYLATION ; C-ALKYLATION ; ALCOHOLS ; KETONES ; PROPANE ; AMINES
WOS研究方向	Engineering
语种	英语
出版者	ELSEVIER SCIENCE SA
WOS记录号	WOS:000454137400084
资助机构	National Key Projects for Fundamental Research and Development of China ; Key Research Program of Frontier Sciences ; International Cooperation and Exchange of the National Natural Science Foundation of China ; National Natural Science Fund for Distinguished Young Scholars ; Key Program of National Natural Science Foundation of China ; National Natural Science Foundation of China ; NSFC-Key Projects of Shanxi Coal Based Low Carbon Joint Foundation ; National Natural Science Funds of Key Research Program of Frontier Sciences, CAS ; National Natural Science Funds
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/27668]
专题	中国科学院过程工程研究所
通讯作者	Li, Chunshan
作者单位	1.Univ Chinese Acad Sci, Sch Chem Sci, Beijing 100049, Peoples R China 2.Chinese Acad Sci, Natl Key Lab Clean & Efficient Coking Technol, Beijing Key Lab Ion Liquids Clean Proc, Inst Proc Engn,State Key Lab Multiphase Complex S, Beijing 100190, Peoples R China
推荐引用方式 GB/T 7714	Wang, Gang,Li, Zengxi,Li, Chunshan,et al. Preparation of methyl acrylate from methyl acetate and methanol with mild catalysis of cobalt complex[J]. CHEMICAL ENGINEERING JOURNAL,2019,359:863-873.
APA	Wang, Gang,Li, Zengxi,Li, Chunshan,&Zhang, Suojiang.(2019).Preparation of methyl acrylate from methyl acetate and methanol with mild catalysis of cobalt complex.CHEMICAL ENGINEERING JOURNAL,359,863-873.
MLA	Wang, Gang,et al."Preparation of methyl acrylate from methyl acetate and methanol with mild catalysis of cobalt complex".CHEMICAL ENGINEERING JOURNAL 359(2019):863-873.