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<p>Coordination cages with well-defined nano-cavities are a particularly attractive class of synthetic supramolecular assemblies capable of catalytically mediating chemical transformations. However, examples of coordination cages with multiple intrinsically catalytic centers suitable for promoting various reactions are relatively rare. Herein, we describe a new approach to designing coordination cages that demonstrate practically useful catalytic activity for one-pot sequential reactions. Our strategy focuses on modulating the <i>exo</i>- and <i>endo</i>-cavities by introducing a pyridine-based dicarboxylate linker with an asymmetric coordination pattern. The coordination cage (<b>Co-PYDC</b>) provides dual active regions, including multiple <i>exo</i> cavities containing coordinatively labile Co(II) sites and one large <i>endo</i> cavity with multiple built-in <i>μ</i><sub>3</sub>-H<sub>2</sub>O Brönsted acidic centers, which proved key to promoting a tandem sequence of epoxidation of olefin followed by aminolysis of epoxides. The present work provides a new paradigm for the design of multifunctional and synthetically useful supramolecular catalysts suitable for practical applications.</p>

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Exo- and endo-cavities modulated coordination cages for consecutive supramolecular catalysis

  • 期刊论文

  • 发表日期：

    2025年10月27日

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  • Chang Li,
  • Tian-Pu Sheng,
  • Zhenqiang Wang,
  • Feng-Rong Dai

摘要

Coordination cages with well-defined nano-cavities are a particularly attractive class of synthetic supramolecular assemblies capable of catalytically mediating chemical transformations. However, examples of coordination cages with multiple intrinsically catalytic centers suitable for promoting various reactions are relatively rare. Herein, we describe a new approach to designing coordination cages that demonstrate practically useful catalytic activity for one-pot sequential reactions. Our strategy focuses on modulating the exo- and endo-cavities by introducing a pyridine-based dicarboxylate linker with an asymmetric coordination pattern. The coordination cage (Co-PYDC) provides dual active regions, including multiple exo cavities containing coordinatively labile Co(II) sites and one large endo cavity with multiple built-in μ3-H2O Brönsted acidic centers, which proved key to promoting a tandem sequence of epoxidation of olefin followed by aminolysis of epoxides. The present work provides a new paradigm for the design of multifunctional and synthetically useful supramolecular catalysts suitable for practical applications.