Direct Methylation of Amines with Carbon Dioxide and Molecular Hydrogen using Supported Gold Catalysts

  • Xian‐Long Du
    Key Laboratory of Interfacial Physics and Technology Shanghai Institute of Applied Physics Chinese Academy of Sciences Jialuo Road 2019 Shanghai 201800 P.R. China
  • Hong‐Liang Bao
    Key Laboratory of Interfacial Physics and Technology Shanghai Institute of Applied Physics Chinese Academy of Sciences Jialuo Road 2019 Shanghai 201800 P.R. China
  • Gao Tang
    Key Laboratory for Advanced Materials Institute of Applied Chemistry East China University of Science and Technology Shanghai 200237 P.R. China
  • Zheng Jiang
    Key Laboratory of Interfacial Physics and Technology Shanghai Institute of Applied Physics Chinese Academy of Sciences Jialuo Road 2019 Shanghai 201800 P.R. China
  • Dang Sheng Su
    Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences Wenhua Road 72 Shenyang 110016 P.R. China
  • Xin‐Hua Zhong
    Key Laboratory for Advanced Materials Institute of Applied Chemistry East China University of Science and Technology Shanghai 200237 P.R. China
  • Jian‐Qiang Wang
    Key Laboratory of Interfacial Physics and Technology Shanghai Institute of Applied Physics Chinese Academy of Sciences Jialuo Road 2019 Shanghai 201800 P.R. China

書誌事項

公開日
2015-09-14
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/cssc.201500486
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>The N‐methylation of amines with CO<jats:sub>2</jats:sub> and H<jats:sub>2</jats:sub> 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<jats:sup>−1</jats:sup>, which is the highest TOF value ever reported for the methylation of aniline with CO<jats:sub>2</jats:sub> and H<jats:sub>2</jats:sub>. Furthermore, the catalyst is tolerant toward a variety of amines, which includes aromatic, aliphatic, secondary, and primary amines. Preliminary mechanistic studies suggest that the <jats:italic>N</jats:italic>‐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 CO<jats:sub>2</jats:sub> into unsymmetrical tertiary amines with H<jats:sub>2</jats:sub> as a reductant in the presence of the Au catalyst.</jats:p>

収録刊行物

  • ChemSusChem

    ChemSusChem 8 (20), 3489-3496, 2015-09-14

    Wiley

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