Research Progress of Actinide-Ligand Multiple Bonding Supported by Tripodal Ligands

doi:10.6023/A21040140

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (8): 986-998.DOI: 10.6023/A21040140 Previous Articles Next Articles

Review

基于三脚架配体构筑的锕系-配体多重键的研究进展

李斌^a, 于吉攀^b, 刘康^b, 吴群燕^b, 刘琦^a^,^*(), 石伟群^b^,^*()

a 哈尔滨工程大学材料科学与化学工程学院哈尔滨 150001
b 中国科学院高能物理研究所北京 100049

投稿日期:2021-04-09 发布日期:2021-05-25
通讯作者: 刘琦, 石伟群

作者简介:

李斌, 2019年6月毕业于郑州大学化学学院, 获理学学士学位; 2019年9月至今为哈尔滨工程大学和中国科学院高能物理研究所联合培养研究生.

于吉攀, 博士, 助理研究员. 2008年获江苏师范大学学士学位; 2011年获南开大学硕士学位; 2014年获清华大学博士学位; 2014.07~2016.07清华大学化学系博士后; 2016年7月加入中国科学院高能物理研究所核能放射化学实验室. 目前主要研究方向: 锕系元素化学.

刘康, 2016年6月毕业于湖北大学化学化工学院, 获理学学士学位; 2016年9月至今在中国科学院高能物理研究所攻读博士学位.

吴群燕, 博士, 副研究员. 2006年获曲阜师范大学硕士学位; 2010年获北京理工大学博士学位; 2010~2013清华大学化学系博士后; 2013年6月加入中国科学院高能物理研究所核能放射化学实验室, 主要从事与核能相关的锕系化学理论方面的研究工作.

刘琦, 博士, 副教授. 2007年获哈尔滨工程大学环境工程专业学士学位; 2009年获哈尔滨工程大学应用化学专业硕士学位; 2016年获哈尔滨工程大学材料学专业博士学位; 2009年6月进入哈尔滨工程大学材料科学与化学工程学院工作, 目前主要从事海水提铀吸附剂材料的设计研究.

石伟群, 研究员, 国家杰出青年科学基金获得者, 长期致力于核燃料循环化学与锕系元素化学相关基础研究, 在JACS、Angew. Chem、Chem、CCS Chem.、Nat. Commun、Adv. Mater.、Environ. Sci. Technol.等国际知名期刊发表SCI 论文200余篇, 成果被国内外同行广泛关注和引用, 文章总引7400余次, H因子44 (Google Scholar). 分别担任英文期刊《Journal of Nuclear Fuel Cycle and Waste Technology》和《Journal of Nuclear Science and Technology》的编委与国际顾问编委, 中文期刊《核化学与放射化学》编委. 现为中国化学会核化学与放射化学专业委员会委员、中国核学会锕系物理与化学分会常务理事、中国有色金属学会熔盐化学与技术专业委员会副主任委员、中国核学会核化工分会理事兼副秘书长.

† These two authors contributed equally to this work.

基金资助:
国家自然科学基金项目(21925603); 国家自然科学基金项目(21806167)

Research Progress of Actinide-Ligand Multiple Bonding Supported by Tripodal Ligands

Bin Li^a, Jipan Yu^b, Kang Liu^b, Qunyan Wu^b, Qi Liu^a(), Weiqun Shi^b()

a College of Materials Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China
b Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

Received:2021-04-09 Published:2021-05-25
Contact: Qi Liu, Weiqun Shi
Supported by:
National Natural Science Foundation of China(21925603); National Natural Science Foundation of China(21806167)

Nonaqueous actinide chemistry is a challenging frontier field, which has made rapid progress in molecular magnetism, multiple bonds and small molecular activation in recent years. Chemical bond is an important basic concept in chemical science, and metal-ligand multiple bond becomes important research content in this field. The formation of multiple bonds is closely related to the electronic configuration of actinides. The s and p-orbitals of actinides contract toward the nucleus and thus produce lower energy level, which increase the shielding effect on nuclear charge. This leads to indirect relativistic effects where the d and f-orbitals experience expansion and destabilization. This destabilization decreases the binding energy of 5f electrons and make them more easily to leave, giving rise to a large range of available oxidation states. Due to higher principle quantum number and relativistic effects, the 5f orbitals of actinides have a much greater radial extension, and the electronic effect of 5f orbitals has a greater influence. At present, the research of actinide-ligand multiple bonds has become one of the most remarkable fields in actinide chemistry and received extensive attention. It is a great challenge to synthesize and separate compounds with actinide-ligand multiple bonds due to their strong radioactivity and toxicity and complex electronic structures. To study actinide-ligand multiple bonds, especially double- and triple-bonded complexes, will assist us to understand their electronic structure, reactivity and physical properties such as electrical conductivity, magnetism, and photochemistry. Tripodal ligands with pocket topology have been widely used in the research of actinide-ligand multiple bonds. This gives a window into exploring the diverse chemical behavior of actinide multiple bonds and observing how actinides can utilize its 5f electrons to exhibit interesting and novel chemistry. The research progress of actinide-ligand multiple bonds based on tripodal ligand is summarized in this review, and the prospect of this field is prognosticated.

Key words: actinide element, tripodal ligand, coordination complex, actinide-ligand multiple bond, small molecule activation

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Bin Li, Jipan Yu, Kang Liu, Qunyan Wu, Qi Liu, Weiqun Shi. Research Progress of Actinide-Ligand Multiple Bonding Supported by Tripodal Ligands[J]. Acta Chimica Sinica, 2021, 79(8): 986-998.

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Fig. & Tab. 26

Figure 1. Syntheses of Tren, Tacn and TriNOx ligands

Figure 2. Syntheses of uranium and thorium complexes supported by tren ligand

Figure 3. Synthesis of U(V)≡N triple bond complex supported by tren ligand

Figure 4. Syntheses of U(VI)≡N triple bond complexes

Figure 5. Synthesis of [U(O)(TrenTIPS)] complex

Figure 6. Study the reactivity of uranium-nitride complex

Figure 7. Syntheses of uranium-imido and uranium-nitride complexes

Figure 8. Syntheses of uranium nitride complexes by reduction of U(IV)-N3 using alkali metal

Figure 9. Study the reactivity of the terminal uranium(V/VI) nitride complexes with CO2 and CS2

Figure 10. Treatment of uranium nitride complexes with frustrated Lewis pair promoted ammonia synthesis

Figure 11. Syntheses of transient thorium(IV) nitride complexes

Figure 12. Syntheses of uranium(IV) phosphinidene complexes

Figure 13. Syntheses of dinuclear uranium complexes with UPU core

Figure 14. Syntheses of uranium-arsenide multiple bond complexes

Figure 15. Syntheses of dinuclear uranium-nitride multiple bond complexes

Figure 16. Syntheses of uranium arsonium- and phosphonium-carbene complexes

Figure 17. Syntheses of thorium-phosphorus multiple bond complexes

Figure 18. Synthetic routes to thorium-arsonium multiple bond complexes

Figure 19. Trivalent uranium precursor complex promoted syntheses of uranium nitride complexes

Figure 20. Syntheses and reactivity of uranium(V)-imido complexes and uranium(V)-oxo complexes

Figure 21. Reaction scheme for the syntheses of U(VI), U(V) and U(IV) oxo multiple bond complexes (a phenolate rings, including the neopentyl and methyl substituent, are omitted for clarity)

Figure 22. Reaction scheme for the syntheses of the uranium imido, amido and oxo multiple bond complexes (a phenolate rings, including the neopentyl and methyl substituent, are omitted for clarity)

Figure 23. Syntheses of the terminal U(IV)≡S complexes

Figure 24. Synthetic route to the terminal uranium(IV) chalcogenido triple bond complexes

Figure 25. Syntheses of uranium oxo double bond complexes

Figure 26. Comparison of covalency in thorium(IV)- and cerium(IV)-imido complexes

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基于三脚架配体构筑的锕系-配体多重键的研究进展

Research Progress of Actinide-Ligand Multiple Bonding Supported by Tripodal Ligands

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Fig. & Tab. 26

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