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化学进展 2021, Vol. 33 Issue (6): 907-913 DOI: 10.7536/PC200671 前一篇   后一篇

• 综述 •

铀催化的氮气活化

陶学兵1, 于吉攀2, 梅雷2, 聂长明1,*(), 柴之芳2,3, 石伟群2,*()   

  1. 1 南华大学化学化工学院 衡阳 421000
    2 中国科学院高能物理研究所核能放射化学实验室 北京 100049
    3 中国科学院宁波材料技术与工程研究所 先进能源材料工程实验室 宁波 315201
  • 收稿日期:2020-06-24 修回日期:2020-08-19 出版日期:2021-06-20 发布日期:2020-12-22
  • 通讯作者: 聂长明, 石伟群
  • 基金资助:
    国家自然科学(21806167); 国家自然科学(21925603); 科学挑战计划(TZ2016004); 中国科学院青年创新促进会基金(2017020)
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Dinitrogen Activation by Uranium Complex

Xuebing Tao1, Jipan Yu2, Lei Mei2, Changming Nie1,*(), Zhifang Chai2,3, Weiqun Shi2,*()   

  1. 1 School of Chemistry and Chemical Engineering, University of South China,Hengyang 421000, China
    2 Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences,Beijing 100049, China
    3 Engineering Laboratory of Advanced Energy Materials, Ningbo Institute of Materials Technology & Engineering, Chinese Academy of Sciences, Ningbo 315201, China
  • Received:2020-06-24 Revised:2020-08-19 Online:2021-06-20 Published:2020-12-22
  • Contact: Changming Nie, Weiqun Shi
  • About author:
    * Corresponding author e-mail: (Changming Nie);
    (Weiqun Shi)
    † These authors contributed equally to this work.
  • Supported by:
    National Natural Science Foundation of China(21806167); National Natural Science Foundation of China(21925603); Science Challenge Project(TZ2016004); Youth Innovation Promotion Association of CAS(2017020)

氮气约占空气总体积的78%,是大自然赋予人类的宝贵资源。如何实现氮气转化为动植物可利用的含氮化合物,关系着人类的未来和社会的可持续发展。氮气活化,作为一个非常重要的研究领域,一直以来都是科学家面临的重大挑战。目前,低价铀金属有机化合物展现出良好的小分子活化能力。本综述主要介绍了含铀化合物对氮气活化的研究进展,并对其未来进行了展望。

关键词： 氮气活化, 含铀金属化合物, 低价态, 配位化学

Dinitrogen is the most abundant gas in the air(approximately 78% of the total air volume), which is a precious resource endowed by nature. How to make use of dinitrogen and transform it into useful nitrogenous compounds is important for humans and sustainable development of society. Dinitrogen activation, as a very important research field, has always been a major challenge. At present, low valent uranium complexes exhibit excellent performance in the small molecule activation. This review mainly introduces and summarizes the application of uranium complexes in dinitrogen activation and transformation, and the prospect of this field is prognosticated.

Contents

1 Introduction

2 Uranium-catalyzed dinitrogen activation

3 Conclusion

Key words: dinitrogen activation, uranium complex, low valence, coordination chemistry
()
图1 金属-N2复合物的质子化过程
Fig.1 Proposed mechanisms A-C protonation of M-N2 complexes
图2 {U(NN'3)}2(μ2-η2:η2-N2) 的合成[27,28]
Fig.2 Synthesis of{U(NN'3)}2(μ2-η2:η2-N2) Complex[27,28]
图3 铀/钼杂双金属氮气复合物的合成[31]
Fig.3 Synthesis of Heterodinuclear Uranium/Molybdenum Dinitrogen Complexes[31]
图4 并环戊二烯基铀复合物活化氮气[32]
Fig.4 Activation of N2 by Uranium(Ⅲ) Complex with Pentalene Ligand[32]
图5 三茂铀-氮气络合物的合成[34]
Fig.5 Synthesis of(C5Me5)3U(N2) Complex[34]
图6 三价铀复合物活化氮气[35]
Fig.6 Activation of N2 by Uranium(Ⅲ) Complex[35]
图7 大位阻硅醇配体螯合的三价铀复合物活化氮气[36]
Fig.7 Activation of N2 by uranium(Ⅲ) complex with large steric resistance silanol ligand[36]
图8 大位阻硅醇配体螯合的三价铀复合物活化氮气[37]
Fig.8 Activation of N2 by uranium(Ⅲ) complex with large steric resistance silanol ligand[37]
图9 基于四齿芳酚配体双核铀复合物活化氮气[38]
Fig.9 Activation of N2 by binuclear uranium(Ⅲ) complex with phenol ligand[38]
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摘要

铀催化的氮气活化