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<p>Metal-organic cages can undergo structural transformations due to the dynamic nature of dative bonds, however, the mechanism of transformation processes is often unclear. Herein we report four metal-organic cages featuring Pd<sub>3</sub>L<sub>6</sub>-type and Pd<sub>4</sub>L<sub>8</sub>-type tubular structures by self-assembly of Pd(II) and two types of bidentate metalloligands. The Pd<sub>3</sub>L<sub>6</sub>-type MOCs were synthesized in H<sub>2</sub>O while the Pd<sub>4</sub>L<sub>8</sub>-type cages were formed in dimethyl sulfoxide (DMSO), indicating the solvent is critical for the assembly. The structure transformation between Pd<sub>3</sub>L<sub>6</sub> and Pd<sub>4</sub>L<sub>8</sub> metal-organic cages can be interconverted when switching the DMSO and H<sub>2</sub>O in a relatively high concentration. The cages partly disassemble into the metalloligands and Pd<sup>2+</sup> ions due to the competitive coordination of DMSO/H<sub>2</sub>O at low concentrations, achieving a concentration-controlled transformation process. Moreover, the structure transformation was monitored by ESI-MS, and the species of intermediate were detected, which provided direct clues for deciphering the mechanism of structural transformation.</p>

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Deciphering the mechanism of structural transformation between Pd3L6 and Pd4L8 metal-organic cages

  • 期刊论文

  • 发表日期：

    2025年1月20日

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  • Xian-Chao Zhou,
  • Yong-Zhen Tan,
  • Ying-Ying Ge,
  • Ya-Liang Lai,
  • Dong Luo,
  • Xiao-Ping Zhou,
  • Dan Li

摘要

Metal-organic cages can undergo structural transformations due to the dynamic nature of dative bonds, however, the mechanism of transformation processes is often unclear. Herein we report four metal-organic cages featuring Pd3L6-type and Pd4L8-type tubular structures by self-assembly of Pd(II) and two types of bidentate metalloligands. The Pd3L6-type MOCs were synthesized in H2O while the Pd4L8-type cages were formed in dimethyl sulfoxide (DMSO), indicating the solvent is critical for the assembly. The structure transformation between Pd3L6 and Pd4L8 metal-organic cages can be interconverted when switching the DMSO and H2O in a relatively high concentration. The cages partly disassemble into the metalloligands and Pd2+ ions due to the competitive coordination of DMSO/H2O at low concentrations, achieving a concentration-controlled transformation process. Moreover, the structure transformation was monitored by ESI-MS, and the species of intermediate were detected, which provided direct clues for deciphering the mechanism of structural transformation.