Product-Triggered Adaptive Evolution From a Pd₄L₂ to a Pd₆L₃ Conjoined Cage via Catalytic Dehydration of p‑Quinone Methide Precursors.

Authors

Chen-Chen Li, Ke-Han Tang, Pei-Ming Cheng, Shao-Jun Hu, Li-Peng Zhou, Li-Xuan Cai, Qing-Fu Sun

Published in

Angewandte Chemie (International ed. in English). Pages e8746400. Sep 24, 2026. Epub Sep 24, 2026.

Abstract

Supramolecular chemistry aims to emulate the dynamic structural adaptations and induced-fit conformational changes of enzymes that are fundamental to their biological function. In this work, we synthesized an adaptive Pd₄L₂ coordination cage using the newly developed pyridinium-based ligand L with cis-capped Pd (II) salt. Upon guest encapsulation, conformational adjustment provides direct structural evidence for the adaptive nature of cage 1 by X-ray crystallographic study. Within the hydrophobic pocket of the capsule, 4-(1-hydroxy-1-phenylethyl) phenol (S1), a known para-quinone methide (p-QM) precursor, undergoes spontaneous dehydration to the alkene product P1 in water. Kinetic studies and control experiments reveal that the cage 1 plays a vital role in significantly accelerating the dehydration process, affording the alkene product with markedly enhanced efficiency compared to the background reaction. Then generated alkene products act as a chemical stimulus driving the transformation of Pd₄L₂ to a Pd₆L₃ conjoined cage through an induced-fit mechanism, as unambiguously confirmed by SCXRD. This work offers fresh insights into enzyme-like adaptive behavior and unveils responsive supramolecular catalysis.

PMID:
42779348
Bibliographic data and abstract were imported from PubMed on 24 Sep 2026.

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