Self-assembly, interlocking, interconversion and anion-binding catalysis in phenoxazine-based Pd2L4 and Pd4L8 coordination cages

Qiong-Yan Hong, Bin Huang, Meng-Xiang Wu, Jun-Yao Jiang, Hai-Bo Yang, Xiao-Li Zhao (), Guido H. Clever () and Xueliang Shi ()
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Qiong-Yan Hong: East China Normal University
Bin Huang: East China Normal University
Meng-Xiang Wu: East China Normal University
Jun-Yao Jiang: East China Normal University
Hai-Bo Yang: East China Normal University
Xiao-Li Zhao: East China Normal University
Guido H. Clever: TU Dortmund University
Xueliang Shi: East China Normal University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Interpenetration is a phenomenon frequently encountered in self-assembled Pd2L4-type coordination cages, while the mechanism of the interpenetration process remains unclear. Here we show the synthesis and solvent-mediated interconversion of highly soluble phenoxazine-based monomeric cage 1 and corresponding interlocked dimer 2. We succeed in the isolation and single-crystal structure analysis of both 1 and 2 with the same guest anion by changing the solvents utilized in self-assembly. The monomeric-to-dimeric cage conversion occurs by heating in weakly coordinating solvents, while dimeric-to-monomeric cage conversion takes place through a disassembly and reassembly process in strongly coordinating solvents at low concentration or by the addition/removal of competing ligand. The interconversion may be driven by the distinct thermodynamic stabilities of 1 and 2 in different solvents. Additionally, Cl– anions template the interpenetration of 1 because of the strong chloride binding affinity of 2 which could serve as an anion-binding catalyst for the C–Cl bond cleavage.

Date: 2025
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DOI: 10.1038/s41467-025-57876-6

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