Dinitrogen Activation and Transformation Promoted by Rare Earth and Actinide Complexes

doi:10.6023/A22060253

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (9): 1299-1308.DOI: 10.6023/A22060253 Previous Articles Next Articles

Review

稀土和锕系配合物促进的氮气活化与转化研究

陈霄, 许汉华, 石向辉, 魏俊年^*(), 席振峰

北京大学化学与分子工程学院北京分子科学国家研究中心生物有机与分子工程教育部重点实验室北京 100871

投稿日期:2022-06-06 发布日期:2022-07-08
通讯作者: 魏俊年

作者简介:

陈霄, 北京大学化学与分子工程学院博士后. 2012年本科毕业于吉林化工学院; 2015年硕士毕业于天津大学; 2019年博士毕业于德国卡尔斯鲁厄理工学院(导师: Peter Roesky教授); 2020.01~2022.05军事科学院防化研究院博士后(合作导师: 裴承新研究员). 2022年6月至今北京大学化学与分子工程学院博士后(合作导师: 席振峰院士).

许汉华, 北京大学化学与分子工程学院博士研究生. 2019年7月毕业于兰州大学化学系, 获理学学士学位; 2019年9月至今于北京大学化学与分子工程学院席振峰院士课题组攻读博士学位.

石向辉, 北京大学化学与分子工程学院博士研究生. 2013年本科毕业于合肥工业大学; 2016年6月硕士毕业于北京化工大学; 2016.7~2017.8长春应用化学所研究实习员; 2017.8~2021.9月长春应用化学所助理研究员; 2021年9月至今于北京大学化学与分子工程学院席振峰院士课题组攻读博士学位.

魏俊年, 北京大学化学与分子工程学院副研究员. 2010年本科毕业于北京大学化学与分子工程学院; 2015博士毕业于北京大学化学与分子工程学院(导师: 席振峰院士, 张文雄教授); 2015.08~2016.08美国加州大学洛杉矶分校博士后(合作导师: Paula Diaconescu教授); 2017.01~2020.07美国加州大学旧金山分校博士后(合作导师: Michael Evans教授); 2020年9月至今北京大学化学与分子工程学院副研究员.

席振峰, 北京大学化学与分子工程学院教授, 中国科学院院士; 1983年本科毕业于厦门大学化学系, 1989年硕士研究生毕业于南京大学配位化学所、郑州大学和河南化学所, 1996年博士研究生毕业于日本分子科学研究所. 目前研究兴趣集中在氮气的活化与转化, 致力于实现温和条件下直接从氮气高效合成含氮有机化合物. 研究内容涉及金属有机化学、配位化学、光化学、电化学、有机合成化学及催化.

基金资助:
国家自然科学基金(21988101); 北京市自然科学基金(2222008)

Dinitrogen Activation and Transformation Promoted by Rare Earth and Actinide Complexes

Xiao Chen, Hanhua Xu, Xianghui Shi, Junnian Wei(), Zhenfeng Xi

Beijing National Laboratory for Molecular Sciences (BNLMS), Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China

Received:2022-06-06 Published:2022-07-08
Contact: Junnian Wei
Supported by:
National Natural Science Foundation of China(21988101); Beijing Natural Science Foundation(2222008)

Dinitrogen gas is highly chemically inert, and the activation and transformation of dinitrogen are challenging. Nitrogen-containing organic compounds have extensive and important applications in developing the national economy. It is of great scientific and economic significance to realize the direct conversion from dinitrogen to nitrogen-containing organic compounds under mild conditions. The activation and transformation of dinitrogen via metal-nitrogen complexes are one of the research hotspots, and chemists have made significant achievements in this field during the past decades. The current research on the activation and transformation of dinitrogen mainly focuses on the main group and transition metal complexes. In contrast, the research on rare earth (RE) and actinide (An) metal-nitrogen complexes is relatively less. Although nearly one hundred crystal structures of rare earth and actinide metal-dinitrogen complexes have been reported, the vast majority of them cannot undergo further nitrogen derivatization reactions, and the types of the supporting ligands are still limited. However, due to the unique electronic structures, f-block complexes can exhibit unusual reactivity different from the main group and transition metals. For example, the f-block metals do not necessarily have to stay in a low oxidation state to activate the dinitrogen, which may lead to the discovery of new dinitrogen transformation modes. As China is rich in rare earth and thorium resources, it is vital to carry out research on dinitrogen fixation and transformation based on rare earth metals and actinides. The synthesis of rare earth and actinide dinitrogen complexes over the past five years, as well as the progress on the generation of nitrogen-containing organic compounds from dinitrogen gas promoted by rare earth and actinide complexes were summarized in this review.

Key words: lanthanide, actinide, dinitrogen complex, dinitrogen activation, dinitrogen transformation, nitrogen fixation

Cite this article

Xiao Chen, Hanhua Xu, Xianghui Shi, Junnian Wei, Zhenfeng Xi. Dinitrogen Activation and Transformation Promoted by Rare Earth and Actinide Complexes[J]. Acta Chimica Sinica, 2022, 80(9): 1299-1308.

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Fig. & Tab. 10

Figure 1. Ligands in the rare earth and actinide metal dinitrogen complexes

Figure 2. Sc complex promoted direct conversion of N2 into hydrazine derivatives

Figure 3. Preparation of (TMS)2N supported Tb and Gd dinitrogen complexes

Figure 4. N2 splitting supported by lanthanide thin film (a) and lanthanide hydride (b)

Figure 5. Preparation of UV dinitrogen complex 8

Figure 6. Binuclear U and Th complexes promoted N2 activation and transformation

Figure 7. Synthesis of phospinoamide supported U-Rh-U complex 13

Figure 8. Synthesis of binuclear uranium nitride compound 16 and its further derivatization

Figure 9. Preparation of binuclear uranium dinitrogen complex 18 and further derivatization

Figure 10. Preparation of UIV3UVIN4O2 cluster 20 and its further derivatization

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稀土和锕系配合物促进的氮气活化与转化研究

Dinitrogen Activation and Transformation Promoted by Rare Earth and Actinide Complexes

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