Citation: Xianghe Kong, Xiaoli Liao, Zhenkun Huang, Lei Mei, Hongqing Wang, Kongqiu Hu, Weiqun Shi. Designed assembly of heterometallic cluster organic frameworks based on Th₆ cluster[J]. Chinese Chemical Letters, ;2024, 35(11): 109642. doi: 10.1016/j.cclet.2024.109642 shu

Designed assembly of heterometallic cluster organic frameworks based on Th₆ cluster

Xianghe Kong ^{a, b} ,
Xiaoli Liao ^a ,
Zhenkun Huang ^a ,
Lei Mei ^b ,
Hongqing Wang ^a ,
Kongqiu Hu ^{b, *,} ,
Weiqun Shi ^{b, *,}

a.
School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
b.
Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China

hukq@ihep.ac.cn

shiwq@ihep.ac.cn

Received Date: 18 December 2023
Revised Date: 26 January 2024
Accepted Date: 4 February 2024
Available Online: 13 February 2024

Figures(4)

Four novel compounds based on hexanuclear thorium cluster were synthesized and characterized. Compound 1 [Th₆(HPyC)₈(HCOO)₄] is formed by replacing formate ligands of preassembled thorium cluster [Th₆O₄(OH)₄(H₂O)₆(HCOO)₁₂] with eight H₂PyC (4-pyrazolecarboxylic acid) under solvothermal conditions. Each of the HPyC⁻ ligands is coordinated with one Cu²⁺ to form the (4,8)-connected -net structure of compound 2 [(CuCl₂)₂Th₆(HPyC)₈(HCOO)₄]. In compound 3 [(CuCl₂)₂Th₆(HPyC)₁₀(HCOO)₄], ten of the formate ligands of preassembled Th₆ cluster are replaced by HPyC⁻ ligands. Compared with compound 2, the two extra HPyC⁻ ligands in the equatorial plane of the Th₆ cluster in compound 3 are not further connected to copper ions. Therefore, the topology structure of compound 3 is same with that of compound 2. Compound 4 [(Cu₃Cl₂)(CuCl₂)Th₆(PyC)₃(HPyC)₄(HCOO)₅] contains three kinds of metal nodes, Th₆ cluster, Cu₃ cluster and mononuclear Cu²⁺, and exhibits a novel (5,7)-connected net structure, which was first discovered in actinide MOFs. Furthermore, considering the satisfactory stability of compound 4 and its unsaturated metal nodes and Lewis acid sites, the catalysis of cycloaddition of CO₂ was further studied. We found that this thorium-copper heterometallic cluster organic framework can be used as a potential actinide functional material for catalyzing the efficient CO₂ conversion to value-added products.
- Actinide,
- Hexanuclear thorium cluster,
- Heterometallic organic frameworks,
- Coordination chemistry,
- Catalytic cycloaddition
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Designed assembly of heterometallic cluster organic frameworks based on Th₆ cluster