Supramolecular encapsulation of redox-active monomers to enable free-radical polymerisation

Herein, multilevel supramolecular assemblies are reported based on sulfobutylether‐β‐cyclodextrin (SBE‐βCD) and cucurbit[8]uril (CB[8]), which can control the topological morphology from nanoparticles to nanosheets and modulate the multicolor luminescence. Benefiting from the large cavity of CB[8] and its strong binding affinity with positively charged tetraphenylethylene pyridinium (TPE‐Py), a 1:2 stoichiometric supramolecular assembly is formed through host–guest interactions with binding constants of 2.95 × 1011 M−2 and fluorescence bathochromic shift about 35 nm due to the macrocyclic confinement effect, thereby endowing the fluorescence enhancement about 20 times when further assembled with negatively charged SBE‐βCD to form nanosheets through electrostatic interactions. In contrast, the direct assembly of TPE‐Py and SBE‐βCD can form nanoparticles through electrostatic interactions, showing only tenfold enhancement and no bathochromic shift due to the lack of macrocyclic confinement effect. After doping the near‐infrared dye acceptor sulfonated aluminum phthalocyanine (AlPcS4), the nanosheets structure exhibits a higher energy transfer efficiency of about 75% and a larger antenna effect of 29.3 than that of nanoparticles. The multilevel supramolecular assemblies can be used in multicolor luminescence information storage and multiple logical gate systems, providing an efficient approach for configurationally confined topological morphology regulation and luminescent materials.

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Configurationally Confined Multilevel Supramolecular Assemblies for Modulating Multicolor Luminescence

Tian

Wang

Yuan

et al. 2023

Adv Funct Materials

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Biofuel‐Driven Stepping Chiral Supramolecular Transfer Container

Yu,

Qiu

et al. 2024

Angewandte Chemie

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Herein, we reported a biofuel‐driven recyclable chiral supramolecular transfer container based on hexacationic triphenylamine cage and nucleotides. Possessing rotatable paddle rigid backbones, the artificial receptor effectively encapsulated nucleotides with a high binding constant up to 5.37×105 M‐1 in water, displaying guest‐induced efficient fluorescence enhancement with quantum yield increased from 6.5% to 16.6%. Especially, the achiral cage could effectively bind with adenosine triphosphate to activate chirality transfer from substrates to the single molecular container, giving circularly polarized luminescence at 575 nm and positive Cotton effect peaks with significant asymmetric factor (gabs = +6.4×10‐4). Meanwhile, the adaptive chiral supramolecule not only has reversible thermal responsiveness but also could stepwise regulate chirality transfer by the catalysis of hexokinase and apyrase in tandem, showing recovery adaptive chirality after refueled, achieving dynamically regulated programmable multistate chiral luminescent supramolecules. Therefore, the biofuel‐driven chiral supramolecular transfer container could be successfully applied in chiral logic gates and multilevel information encryption, providing new insight into intelligent chiral materials.

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Biofuel‐Driven Stepping Chiral Supramolecular Transfer Container

Yu,

Qiu

et al. 2024

Angew Chem Int Ed

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Supramolecular encapsulation of redox-active monomers to enable free-radical polymerisation

Abstract: Extended polymeric structures based on redox-active species are of great interest in emerging technologies related to energy conversion and storage. However, redox-active monomers tend to inhibit radical polymerisation processes and...

Cited by 5 publications

References 50 publications

Configurationally Confined Multilevel Supramolecular Assemblies for Modulating Multicolor Luminescence

Configurationally Confined Multilevel Supramolecular Assemblies for Modulating Multicolor Luminescence

Biofuel‐Driven Stepping Chiral Supramolecular Transfer Container

Biofuel‐Driven Stepping Chiral Supramolecular Transfer Container

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