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

Author

Listed:
  • 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)

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.

Suggested Citation

  • Qiong-Yan Hong & Bin Huang & Meng-Xiang Wu & Jun-Yao Jiang & Hai-Bo Yang & Xiao-Li Zhao & Guido H. Clever & Xueliang Shi, 2025. "Self-assembly, interlocking, interconversion and anion-binding catalysis in phenoxazine-based Pd2L4 and Pd4L8 coordination cages," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57876-6
    DOI: 10.1038/s41467-025-57876-6
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    References listed on IDEAS

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    1. Yasuto Murayama & Shizuko Endo & Yumiko Kurokawa & Ayako Kurita & Sanae Iwasaki & Hiroyuki Araki, 2024. "Coordination of cohesin and DNA replication observed with purified proteins," Nature, Nature, vol. 626(7999), pages 653-660, February.
    2. Fuji Sakai & Guang Yang & Manfred S. Weiss & Yijiang Liu & Guosong Chen & Ming Jiang, 2014. "Protein crystalline frameworks with controllable interpenetration directed by dual supramolecular interactions," Nature Communications, Nature, vol. 5(1), pages 1-8, December.
    3. Zai-Sheng Wu & Zhifa Shen & Kha Tram & Yingfu Li, 2014. "Engineering interlocking DNA rings with weak physical interactions," Nature Communications, Nature, vol. 5(1), pages 1-10, September.
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