Bulk transparent supramolecular glass enabled by host–guest molecular recognition

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Supramolecular glass is a non-covalently cross-linked amorphous material that exhibits excellent optical properties and unique intrinsic structural features. Compared with artificial inorganic/organic glass, which has been extensively developed, supramolecular glass is still in the infancy stage, and itself is rarely recognized and studied thus far. Herein, we present the development of the host–guest molecular recognition motifs between methyl-β-cyclodextrin and para-hydroxybenzoic acid as the building blocks of supramolecular glass. Non-covalent polymerization resulting from the host–guest complexation and hydrogen bonding formation enables high transparency and bulk state to supramolecular glass. Various advantages, including recyclability, compatibility, and thermal processability, are associated with dynamic assembly pattern. Short-range order (host–guest complexation) and long-range disorder (three dimensional polymeric network) structures are identified simultaneously, thus demonstrating the typical structural characteristics of glass. This work provides a supramolecular strategy for constructing transparent materials from organic components.

In this study, the molecular recognition motif of methyl-β-cyclodextrin [M] and para-hydroxybenzoic acid [H] is used as the basic unit to construct supramolecular glass MH. The recognition behavior between M and H yields the order host–guest recognition structures on a restricted scale and actuates the supramolecular polymerization of M/H host–guest complexes into isotropic MH in bulk. The nature and intrinsic structure of MH were carefully studied via a combined experimental and theoretical investigation. The obtained MH exhibits various excellent performances in terms of high transmittance, good thermal processability, broad compatibility, and considerable recyclability.

Cai, C., Wu, S., Zhang, Y. et al. Bulk transparent supramolecular glass enabled by host–guest molecular recognition. Nat Commun 15, 3929 (2024). https://doi.org/10.1038/s41467-024-48089-4

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