title: Direct Methylation of Amines with Carbon Dioxide and Molecular Hydrogen using Supported Gold Catalysts.
abstract: The N-methylation of amines with CO2 and H2 is an important step in the synthesis of bioactive compounds and chemical intermediates. The first heterogeneous Au catalyst is reported for this methylation reaction with good to excellent yields. The average turnover frequency (TOF) based on surface Au atoms is 45 h(-1) , which is the highest TOF value ever reported for the methylation of aniline with CO2 and H2 . Furthermore, the catalyst is tolerant toward a variety of amines, which includes aromatic, aliphatic, secondary, and primary amines. Preliminary mechanistic studies suggest that the N-alkyl formamide might be an intermediate in the N-methylation of amine process. Moreover, through a one-pot process, it is possible to convert primary amines, aldehydes, and CO2 into unsymmetrical tertiary amines with H2 as a reductant in the presence of the Au catalyst.
authors.affiliation: Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Jialuo Road 2019, Shanghai, 201800, P.R. China.
authors.forename: Xian-Long
authors.initials: XL
authors.lastname: Du
authors.affiliation: Key Laboratory for Advanced Materials, Institute of Applied Chemistry, East China University of Science and Technology, Shanghai 200237, P.R. China.
authors.forename: Gao
authors.initials: G
authors.lastname: Tang
authors.affiliation: Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Jialuo Road 2019, Shanghai, 201800, P.R. China.
authors.forename: Hong-Liang
authors.initials: HL
authors.lastname: Bao
authors.affiliation: Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Jialuo Road 2019, Shanghai, 201800, P.R. China.
authors.forename: Zheng
authors.initials: Z
authors.lastname: Jiang
authors.affiliation: Key Laboratory for Advanced Materials, Institute of Applied Chemistry, East China University of Science and Technology, Shanghai 200237, P.R. China.
authors.forename: Xin-Hua
authors.initials: XH
authors.lastname: Zhong
authors.affiliation: Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Wenhua Road 72, Shenyang, 110016, P.R. China. dssu@imr.ac.cn.
authors.forename: Dang Sheng
authors.initials: DS
authors.lastname: Su
authors.affiliation: Key Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Jialuo Road 2019, Shanghai, 201800, P.R. China. wangjianqiang@sinap.ac.cn.
authors.forename: Jian-Qiang
authors.initials: JQ
authors.lastname: Wang
mesh_terms: D000537:Aluminum Oxide / Q000737:chemistry*; D000588:Amines / Q000737:chemistry*; D002245:Carbon Dioxide / Q000737:chemistry*; D002384:Catalysis; D006046:Gold / Q000737:chemistry*; D006859:Hydrogen / Q000737:chemistry*; D008745:Methylation
chemical_list: D000588:Amines; D002245:Carbon Dioxide; D006046:Gold; D006859:Hydrogen; D000537:Aluminum Oxide
keywords: amines; gold; heterogeneous catalysis; hydrogen; supported catalysts