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Direct Methylation of Amines with Carbon Dioxide and Molecular Hydrogen using Supported Gold Catalysts
Du, Xian-Long; Tang, Gao; Bao, Hong-Liang; Jiang, Zheng; Zhong, Xin-Hua; Su, Dang Sheng; Wang, Jian-Qiang; dssu@imr.ac.cn; wangjianqiang@sinap.ac.cn
2015
发表期刊CHEMSUSCHEM
ISSN1864-5631
卷号8期号:20页码:3489-3496
摘要The N-methylation of amines with CO2 and H-2 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 45h(-1), which is the highest TOF value ever reported for the methylation of aniline with CO2 and H-2. 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 H-2 as a reductant in the presence of the Au catalyst.
部门归属[du, xian-long ; bao, hong-liang ; jiang, zheng ; wang, jian-qiang] chinese acad sci, shanghai inst appl phys, key lab interfacial phys & technol, shanghai 201800, peoples r china ; [tang, gao ; zhong, xin-hua] e china univ sci & technol, inst appl chem, key lab adv mat, shanghai 200237, peoples r china ; [su, dang sheng] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china
关键词Amines Gold Heterogeneous Catalysis Hydrogen Supported Catalysts
资助者National Basic Research Program of China [2013CB933104]; Ministry of Science and Technology [2014DFG60230]; National Natural Science Foundation of China [21303246, 11275258, 91127001]; CFI; NSERC; NRC; CIHR; University of Saskatchewan; Government of Saskatchewan; Western Economic Diversification Canada
收录类别sci
语种英语
WOS记录号WOS:000363683000017
引用统计
被引频次:81[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/321006/74722
专题中国科学院金属研究所
通讯作者dssu@imr.ac.cn; wangjianqiang@sinap.ac.cn
推荐引用方式
GB/T 7714
Du, Xian-Long,Tang, Gao,Bao, Hong-Liang,et al. Direct Methylation of Amines with Carbon Dioxide and Molecular Hydrogen using Supported Gold Catalysts[J]. CHEMSUSCHEM,2015,8(20):3489-3496.
APA Du, Xian-Long.,Tang, Gao.,Bao, Hong-Liang.,Jiang, Zheng.,Zhong, Xin-Hua.,...&wangjianqiang@sinap.ac.cn.(2015).Direct Methylation of Amines with Carbon Dioxide and Molecular Hydrogen using Supported Gold Catalysts.CHEMSUSCHEM,8(20),3489-3496.
MLA Du, Xian-Long,et al."Direct Methylation of Amines with Carbon Dioxide and Molecular Hydrogen using Supported Gold Catalysts".CHEMSUSCHEM 8.20(2015):3489-3496.
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