三核过渡金属配合物在催化反应中的研究进展

doi:10.6023/A22100425

化学学报 ›› 2023, Vol. 81 ›› Issue (1): 84-99.DOI: 10.6023/A22100425 上一篇下一篇

综述

三核过渡金属配合物在催化反应中的研究进展

马雪璐^a^,^b^,^*(), 李蒙^a, 雷鸣^c^,^*()

a 中国矿业大学(北京) 化学与环境工程学院北京 100083
b 闽江学院福建省海洋传感功能材料重点实验室福州 350108
c 北京化工大学化工资源有效利用国家重点实验室计算化学研究所化学学院北京 100029

投稿日期:2022-10-11 发布日期:2022-12-05
通讯作者: 马雪璐, 雷鸣

作者简介:

马雪璐, 博士, 中国矿业大学(北京)化学与环境工程学院讲师, 硕士研究生导师. 2016年博士毕业于北京化工大学理学院(导师: 雷鸣教授); 同年进入清华大学化学系从事博士后研究工作(导师: 李隽教授). 2018年至今就职于中国矿业大学(北京)化学与环境工程学院, 主要研究方向为绿色催化反应体系的理论设计研究.

李蒙, 中国矿业大学(北京)2020级在读硕士研究生. 2015年获河北科技师范学院学士学位. 研究方向为均相催化剂的理论设计研究.

雷鸣, 北京化工大学化工资源有效利用国家重点实验室、计算化学研究所及化学学院物理化学系教授、博士生导师. 研究方向为计算催化化学. 在均相催化、多相催化催化机制、催化剂分子设计、理论计算化学及其交叉领域进行了探索性学术研究工作.

基金资助:
项目受中央高校基本科研业务费(2022YQHH01); 福建省海洋传感功能材料重点实验室(闽江学院)开放课题(MJUKF-FMSM202202); 国家自然科学基金(21902182)

Trinuclear Transition Metal Complexes in Catalytic Reactions

Xuelu Ma^a^,^b(), Meng Li^a, Ming Lei^c()

a School of Chemical & Environmental Engineering, China University of Mining & Technology, Beijing 100083
b Fujian Key Laboratory of Functional Marine Sensing Materials, Minjiang University, Fuzhou 350108
c State Key Laboratory of Chemical Resource Engineering, Institute of Computational Chemistry, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029

Received:2022-10-11 Published:2022-12-05
Contact: ^*E-mail: maxl@cumtb.edu.cn; leim@mail.buct.edu.cn
Supported by:
Fundamental Research Funds for the Central Universities(2022YQHH01); Open Project Program of Fujian Key Laboratory of Functional Marine Sensing Materials(MJUKF-FMSM202202); National Natural Science Foundation of China(21902182)

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摘要/Abstract

多核过渡金属配合物作为一类广泛应用的均相催化剂, 其设计灵感往往来自天然酶的多金属活性位点所发挥的重要作用. 目前, 三核金属配合物作为活化小分子的多金属催化剂受到了广泛的关注. 为深入理解三核过渡金属配合物在催化反应中作用特点, 对近年报道的代表性三核过渡金属配合物按金属中心进行分类, 并对配体环境形成特点及催化应用进行综述. 从金属中心出发, 讨论了三核过渡金属配合物的几何结构和电子特征; 从配体环境出发, 总结了关联三个独立的金属位点的配位环境特征; 在催化应用方面, 重点综述了三核过渡金属配合物在涉及特定化学键活化反应的催化作用机制, 最后对三核过渡金属配合物的催化应用前景进行展望.

关键词: 三核过渡金属配合物, 均相催化, 化学键活化, 协同作用

Polynuclear transition metal complexes are widely used as homogeneous catalysts, and the polymetallic active sites of enzymes also play an important role in the mechanism of biochemical reactions under ambient conditions. As the efficient polymetallic catalysts for the activation of small molecules, trinuclear metal complexes have been attracted extensive attention. In order to understand the role of trinuclear transition metal complexes in catalytic reactions, we have classified the trinuclear transition metal complexes according to metal centers, and summarized the characteristics of their ligands, as well as their catalytic applications. Based on the metal centers, the geometric structure and electronic characteristics of the complexes are discussed. Based on the peripheral ligands, the characteristics of the coordination environment, which enable the aggregation of three independent metal sites, are highlighted. In terms of catalytic applications of trinuclear transition metal complexes, the catalytic mechanisms involving specific chemical bonds activation are focused on. Finally, we outlook the crucial potential application in this emerging ﬁeld.

Key words: trinuclear transition metal complexes, homogeneous catalysis, chemical bond activation, synergy mechanism

引用此文

马雪璐, 李蒙, 雷鸣. 三核过渡金属配合物在催化反应中的研究进展[J]. 化学学报, 2023, 81(1): 84-99.

Xuelu Ma, Meng Li, Ming Lei. Trinuclear Transition Metal Complexes in Catalytic Reactions[J]. Acta Chimica Sinica, 2023, 81(1): 84-99.

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图/表 20

图1. 第III副族~第VII副族同核金属三中心配合物

Figure 1. Homometallic trinuclear complexes of IIIB~VIIB group transition metals

图2. 第Ⅷ族同核金属三中心配合物

Figure 2. Homometallic trinuclear complexes of VIII group transition metals

图3. 第I副族~第II副族同核金属三中心配合物

Figure 3. Homometallic trinuclear complexes of IB~IIB transition metals

图4. 异三核过渡金属配合物

Figure 4. Heterometallic trinuclear transition metal complexes

图5. 封闭环状配体

Figure 5. Closed cyclic ligands

图6. 开放空穴状配体

Figure 6. Open cavity ligands

图7. 基于相同配体环境的系列三核金属配合物

Figure 7. A series of trinuclear metal complexes based on the same ligand environment

图8. 三核金属配合物的配体特征

Figure 8. Ligand characteristics of trinuclear metal complexes

图9. 三核钛配合物1活化N2的反应机理[8]

Figure 9. Dinitrogen activation mechanism catalyzed by the trinuclear titanium complex 1[8]

图10. 三核四氢化铬配合物4对N2的活化与加氢反应[14]

Figure 10. Dinitrogen activation and hydrogenation by the trinuclear chromium tetrahydride complex 4[14]

图11. 三核铁配合物51到配合物51-A的固态转化[78]

Figure 11. The solid-state conversion of complex 51 to complex 51-A[78]

图12. 三核钴配合物15活化N2的反应[26,55]

Figure 12. Dinitrogen activation catalyzed by the trinuclear cobalt complex 15[26,55]

图13. 三核钌配合物52与取代肼的反应机理[84]

Figure 13. Plausible mechanism for the reaction of trinuclear ruthenium complex 52 with substituted hydrazines[84]

图14. 配合物37-C的合成及其形成机制[49]

Figure 14. Synthesis and the proposed formation mechanism of 37-C[49]

图15. 三核钛配合物1对苯和甲苯环的裂解和收缩的作用机理[89]

Figure 15. Proposed mechanism of the ring cleavage and contraction of benzene and toluene by the trinuclear titanium complex 1[89]

图16. 三核钯配合物53活化C=C/C≡C键的反应[91]

Figure 16. Activation of C=C/C≡C bond by the trinuclear palladium complex 53[91]

图17. 三核铱配合物54催化CO2加氢的反应机理[92]

Figure 17. The plausible reaction mechanism for the catalytic hydrogenation of CO2 using the trinuclear iridium complex 54[92]

图18. 三核锌骨架配合物33固定CO2的示意图[45]

Figure 18. CO2 fixation in the presence of tripodal Zn complex 33[45]

图19. 三核钛配合物1催化吡啶的氢化脱氮转化机制[10]

Figure 19. Hydrodenitrification and transformation of pyridine catalyzed by the trinuclear titanium complex 1 [10]

图20. 三核铜配合物30催化甲烷氧化制甲醇的反应机理[38]

Figure 20. The plausible reaction mechanism of the oxidation of methane to methanol mediated by trinuclear copper complex 30[38]

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三核过渡金属配合物在催化反应中的研究进展

Trinuclear Transition Metal Complexes in Catalytic Reactions

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