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Multicomponent supramolecular polymer gels are a class of soft matter materials which form via the assembly of two or more small molecules. Different structures can be generated with interesting potential functions and applications. Insight into the assembly mechanism is key in the design of these systems for specific applications. Herein, a series of hydrogels with diverse structures and functionalities were synthesised. Using dynamic covalent chemistry as a key tool we show that it is possible to control the monomer assembly, forming both self-sorted and co-assembled polymers and gels from the same initial components. The hierarchical structure of the gels is difficult to elucidate. We emphasise the significance of small-angle neutron scattering (SANS) and spin-echo SANS (SESANS) measurements in characterising these intricate assemblies and demonstrate that these techniques are able to differentiate among self-sorted and co-assembled structures even when using chemically similar components.
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http://dx.doi.org/10.1038/s42004-025-01657-1 | DOI Listing |
J Am Chem Soc
September 2025
Department of Chemistry, National Taiwan University, Taipei 106319, Taiwan.
The exclusive formation of artificial multicomponent assemblies remains a significant challenge, in contrast to the well-established organization observed in natural systems, due to intrinsic entropic constraints. To overcome this limitation, recent efforts have been focused on developing precision self-assembly strategies for the rational construction of such architectures. Here, we construct an ideal complementary pair of 2,2':6',2″-terpyridine (tpy)-based ligands by fine-tuning the substituent bulkiness, which enables the quantitative formation of robust nested cages through efficient dynamic heteroleptic complexation with multivalent coordination.
View Article and Find Full Text PDFJ Am Chem Soc
September 2025
School of Chemistry and RNA Institute, University of New South Wales, 2052 Sydney, Australia.
The diversity of noncovalent interactions makes the design space of multicomponent molecular systems highly complex. To efficiently explore supramolecular design space, data-driven strategies are needed. Here, we demonstrate a methodological framework for the targeted design of multicomponent molecular systems with noncovalent interactions using Bayesian optimization.
View Article and Find Full Text PDFZhongguo Ying Yong Sheng Li Xue Za Zhi
September 2025
Department of Pharmaceutics, SMBT College Of Pharmacy, Nashik, Maharashtra, India.
Pharmaceutical cocrystals have emerged as a transformative approach in drug development, enhancing the physicochemical properties of active pharmaceutical ingredients (APIs) such as solubility, bioavailability, stability, and dissolution rate without altering their pharmacological characteristics. Defined as multicomponent crystalline solids composed of two or more neutral molecules in a stoichiometric ratio, cocrystals are formed through non-ionic interactions like hydrogen bonding and π-π stacking. This review explores the evolution, design, preparation, and applications of pharmaceutical cocrystals, highlighting their ability to improve drug performance, enable controlled release, and offer intellectual property opportunities.
View Article and Find Full Text PDFCommun Chem
August 2025
School of Chemistry, Joseph Black Laboratories, University of Lincoln, Lincoln, LN6 7TS, UK.
Multicomponent supramolecular polymer gels are a class of soft matter materials which form via the assembly of two or more small molecules. Different structures can be generated with interesting potential functions and applications. Insight into the assembly mechanism is key in the design of these systems for specific applications.
View Article and Find Full Text PDFJ Am Chem Soc
September 2025
Department of Chemistry, Graduate School of Advanced Science and Engineering, Hiroshima University, 1-3-1 Kagamiyama, Higashi-Hiroshima, Hiroshima 739-8526, Japan.
Nature precisely regulates multicomponent assemblies with the assistance of cooperativity. However, establishing such high precision in multicomponent assemblies of artificial supramolecular structures remains challenging. Here, we successfully position multiple distinct guest molecules within two equivalent binding cavities of a zinc-metalated trisporphyrin host by combining two distinct negative cooperative interactions, including donor-acceptor π-stacking and metal-ligand coordination.
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