物理化学学报 >> 2018, Vol. 34 >> Issue (8): 845-857.doi: 10.3866/PKU.WHXB201701081

所属专题: 绿色化学

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二氧化碳和胺催化合成甲酰胺反应研究

张玉景1,2,代兴超1,2,王红利1,石峰1,*()   

  1. 1 中国科学院兰州化学物理研究所,兰州 730000
    2 中国科学院大学,北京 100049
  • 收稿日期:2017-11-30 发布日期:2018-04-03
  • 通讯作者: 石峰 E-mail:fshi@licp.cas.cn
  • 作者简介:SHI Feng completed his Ph.D. studies in catalysis at LICP, CAS in 2004. After a three-year postdoctoral research in LIKAT in Germany, he joined the faculty of LICP in 2008 as Hundred Talents Program of CAS. Since 2016 SHI Feng is the deputy director of the State Key Laboratory for Oxo Synthesis and Selective Oxidation. His research focuses on nano-catalysis in fine chemical synthesis and C1 chemistry
  • 基金资助:
    国家自然科学基金(21633013);国家自然科学基金(91745106);国家重大研究与发展项目(2017YFA0403103)

Catalytic Synthesis of Formamides with Carbon Dioxide and Amines

Yujing ZHANG1,2,Xingchao DAI1,2,Hongli WANG1,Feng SHI1,*()   

  1. 1 State Key Laboratory for Oxo Synthesis and Selective Oxidation, Center for Green Chemistry and Catalysis, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, P. R. China
    2 University of Chinese Academy of Sciences, Beijing 100049, P. R. China
  • Received:2017-11-30 Published:2018-04-03
  • Contact: Feng SHI E-mail:fshi@licp.cas.cn
  • Supported by:
    the National Natural Science Foundation of China(21633013);the National Natural Science Foundation of China(91745106);National Key Research and Development Program of China(2017YFA0403103)

摘要:

二氧化碳是碳资源利用的最终形式,也是一种绿色的碳一资源。通过催化化学的方法将二氧化碳转化为高附加值精细化学品是二氧化碳循环利用的有效途径。酰胺类化合物是一类重要的化工原料和溶剂,广泛应用于医药、农药、日用化学品及石油化工等众多领域且需求量巨大。因此,以二氧化碳为羰源,通过高效催化体系的建立实现二氧化碳与胺反应合成甲酰胺具有重要意义。本文分别从催化体系、还原剂和反应机理等角度综述了这一领域近年来的主要研究成果。其中,催化体系可分为贵金属催化剂如Ir、Pd、Pt、Ru、Rh,非贵金属催化剂如Ni、Mo、Cu、Fe、Co、Zn、Al,有机分子催化剂和无催化剂体系,常用的还原剂为H2,硅烷和硼烷。在此基础上,对不同催化体系的典型反应机理进行了讨论。

关键词: 二氧化碳, 胺, 甲酰胺, 羰基化

Abstract:

Carbon dioxide is a green C1 resource that can be efficiently recycled by catalytic transformation into value-added chemicals. Formamides are important intermediates and solvents that are used extensively in pharmaceutical, daily-chemical, and petrochemical industry. Therefore, it is worthwhile to synthesize formamides with CO2 and amines. In this review, the main advancements in the synthesis of formamides by using CO2 as the C1 feedstock with noble metal catalysts (Ir, Pd, Pt, Ru, Rh, etc.), non-noble metal catalysts (Ni, Mo, Cu, Fe, Co, Zn, Al, etc.), organocatalysts, and catalyst-free systems have been summarized. In addition, the role of the reducing agents such as H2, silanes, and boranes involved in these transformations has also been reviewed. In addition, the reaction mechanisms with the different catalyst systems have been discussed.

Key words: Carbon dioxide, Amines, Formamides, Carbonylation

MSC2000: 

  • O643