Research Progress on Metal-coordination-driven Self-assembly of 6,6

doi:10.6023/A23120538

Acta Chimica Sinica ›› 2024, Vol. 82 ›› Issue (3): 336-347.DOI: 10.6023/A23120538 Previous Articles Next Articles

Review

6,6″-二(2,6-二甲氧基苯)-三联吡啶及其衍生物金属配位自组装的研究进展

王敏^a, 陈帮塘^a, 陈桥林^a, 王俊^a, 陈名钊^a, 蒋志龙^a^,^*(), 王平山^a^,^b^,^*()

a 广州大学大湾区环境研究院珠江三角洲水质安全与保护教育部重点实验室广州 510006
b 中南大学化学化工学院长沙 410083

投稿日期:2023-12-19 发布日期:2024-01-18

作者简介:

王敏, 广州大学环境科学与工程学院环境工程专业在读硕士生.

蒋志龙, 广州大学大湾区环境研究院副教授, 主要的研究方向为超分子自组装及功能配合物, 参与国家自然科学基金面上项目3项, 主持贵州省科技厅科技创新项目1项, 广东省教育厅科技创新项目1项, 广州市市校联合基金1项, 目前以第一作者或者通讯作者身份在Nature Communication、J. Am. Chem. Soc.、Angew. Chem. Int. Ed.、iScience、Cell Reports Physical Science、Nano Research、Chem. Commun.、Inorg. Chem.等期刊上发表论文17篇, 授权中国发明专利6项.

王平山, 广州大学大湾区环境研究院教授, 中南大学化学化工学院特聘教授, 入选中组部海外高层次人才计划和湖南省“国家级领军人才”, 主持国家、国际环境署/环保部及美国科研项目20余项, 获省部级科技奖励3项, 目前研究领域主要集中在超分子化学、金属有机高分子能源材料和高分子环保材料, 在Science, Nat. Commun., J. Am. Chem. Soc., Angew. Chem. Int. Ed.等期刊发表学术论文100余篇, 授权国际和中国发明专利30余项, 在超大单分子的构筑策略研究领域有突出贡献, 相关成果在国内外具有重要的影响.

基金资助:
国家自然科学基金(22101060); 国家自然科学基金(21971257); 广州市科技计划项目(202201020201); 广州市科技计划项目(SL2022A03J01050)

Research Progress on Metal-coordination-driven Self-assembly of 6,6"-Bis(2,6-dimethoxy-benzene)-terpyridine and Its Derivatives

Min Wang^a, Bangtang Chen^a, Qiaolin Chen^a, Jun Wang^a, Mingzhao Chen^a, Zhilong Jiang^a(), Pingshan Wang^a^,^b()

a Institute of Environmental Research at Greater Bay Area, Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Guangzhou University, Guangzhou 510006
b College of Chemistry and Chemical Engineering, Central South University, Changsha 410083

Received:2023-12-19 Published:2024-01-18
Contact: *E-mail: jiangzl@gzhu.edu.cn;chemwps@csu.edu.cn
Supported by:
National Natural Science Foundation of China(22101060); National Natural Science Foundation of China(21971257); Science and Technology Planning Project of Guangzhou(202201020201); Science and Technology Planning Project of Guangzhou(SL2022A03J01050)

In the past few decades, coordination-driven self-assembly of metal ions and organic ligands has been extensively applied in the construction of a variety of functional two-dimensional (2D) and three-dimensional (3D) structures. The majority of these structures are consisted of one type of ligand. Nevertheless, there have been sustained efforts dedicated to constructing heteroleptic assemblies using various strategic methods in order to increase the complexity and sophistication of nano-scale structures. Heteroleptic assemblies involve the use of multiple types of ligands, to assemble metal ions into more intricate structures. This approach allows for the incorporation of different ligand geometries, charge densities, and functional groups, leading to increased structural diversity and potential for new properties. To achieve heteroleptic assemblies, various strategic methods have been employed. One common approach is the use of different ligands with complementary binding properties, allowing for the controlled formation of targeted structures. In recent years, 6,6"-bis(2,6-dimethoxy-phenyl)- terpyridine and its derivatives have received considerable attention in the research of coordination-driven supramolecular self-assembly. These ligands exhibit strong self-recognition ability and effectively suppress the formation of by-products in multicomponent self-assembly processes, giving them unique advantages in the precise construction of metal-coordination supramolecular structures involving multiple ligands. A large number of 2D and 3D supramolecular structures formed by the coordination of 6,6"-bis(2,6-dimethoxy-phenyl)-terpyridine ligands and their derivatives with metal ions have been reported. The successful construction of these 2D and 3D topological structures has not only enriched the research of terpyridine metal-coordination supramolecular structures but also demonstrated significant research value and broad prospects in fields such as luminescent materials, host-guest chemistry, drug delivery systems, and confined catalysis. Based on this, this review systematically summarizes the latest progress in the self-assembly of derivative ligands based on 6,6"-bis(2,6-dimethoxy- phenyl)-terpyridine in terms of ligand synthesis, structure construction and property study, and briefly discusses the current development opportunities and challenges faced in this field.

Key words: terpyridine, metal coordination self-assembly, metal-organic complexes, complementary terpyridine ligand pairing, functional supramolecular

Cite this article

Min Wang, Bangtang Chen, Qiaolin Chen, Jun Wang, Mingzhao Chen, Zhilong Jiang, Pingshan Wang. Research Progress on Metal-coordination-driven Self-assembly of 6,6"-Bis(2,6-dimethoxy-benzene)-terpyridine and Its Derivatives[J]. Acta Chimica Sinica, 2024, 82(3): 336-347.

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Fig. & Tab. 22

Figure 1. Self-sorting of ligands and synthesis of scalene triangle structures

Figure 2. Complementary terpyridine ligands pairing coordination process versus metal ion

Figure 3. Synthetic strategies of 6,6"-bis(2,6-dimethoxybenzene)- terpyridine ligand

Figure 4. Synthesis of heteroleptic complex 4

Figure 5. Self-assembly of triangle 5a and ditrigon 5b

Figure 6. Self-assembly of Sierpiński triangle 6a and its site-selective transmetalation

Figure 8. Self-assembly of the four-pointed star 7a and six-pointed star 7b

化合物	吸收最大值/nm	发射最大值/nm	量子产率^a/%
[Cd₄L¹₂L²₂]	286 (4.5), 355 (1.4)	467	14.4
[Cd₄L¹₂L³₂]	278 (6.7), 330 (1.1)	472	13.3
[Cd₄L¹₂L⁴₂]	283 (19.6), 343 (10.2)	473	6.2
[Cd₆L¹₃L⁵₃]	279 (13.2), 336 (1.9)	473	6.3
[Cd₄L⁵₂L⁷₂]	279 (10.1), 333 (2.5)	393, 463	14.4
[Cd₄L²₂L⁷₂]	280 (9.8), 335 (2.8)	393, 450	21.2
[Cd₉L⁷₃L⁸₃]	281 (10.5), 335 (3.9)	381, 464	8.2
[Cd₃L¹⁰₂]	278 (4.9), 325 (6.3)	407, 492	5.3
[Cd₆L¹₃L¹⁰₂]	280 (10.2), 340 (1.6)	472	2.1
[Cd₆L⁷₃L¹⁰₂]	281 (18.4), 332 (6.0)	395, 495	7.1
[Cd₆L⁹₃L¹⁰₂]	280 (10.8), 335 (1.7)	477	2.1
[Cd₁₂L¹⁰₄L¹¹₄]	286 (3.5), 330 (1.6)	472	3.4

Table 1. Absorption and emission band maxima, molar extinction coefficients, and quantum yields in MeCN

Figure 17. Catalytic study of Triakis tetrahedron 15b: (a) ESR spectra of the Triakis tetrahedron 15b mixed with 4-oxo-TMP under Xe lamp (λ>420 nm, 300 W), (b) conversion of CEES catalyzed by the Triakis tetrahedron 15b under Xe lamp (λ>420 nm, 300 W), (c) 1H NMR spectra of CEES catalyzed by the Triakis tetrahedron 15b under Xe lamp (λ>420 nm, 300 W) at different time. Reprinted with permission from Ref. [84], copyright 2023, Elsevier

Figure 18. Self-assembly of three Co2+ complexes based on complementary terpyridine ligands pairing

Figure 19. Plots of the temperature dependence of χMT under 5000 Oe dc field for (a) 16a, (b) 16b, and (c) 16c for successive cycles. Reprinted with permission from Ref. [88], copyright 2022, CCS Chinese Journal of Inorganic Chemistry

Figure 20. Synthesis of three Co2+ complexes with different linkers

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6,6″-二(2,6-二甲氧基苯)-三联吡啶及其衍生物金属配位自组装的研究进展

Research Progress on Metal-coordination-driven Self-assembly of 6,6"-Bis(2,6-dimethoxy-benzene)-terpyridine and Its Derivatives

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