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Structural disruption of melanin-like polymers with boosted UV protection

Science China Chemistry 2024年第5期67卷 1653-1663页

作者： Zhen Yang Xianheng Wang Wanjie Bai Zikun Zou Haoxing Wu Yiwen Li department of Radiology Huaxi MR Research CenterFunctional and Molecular Imaging Key Laboratory of Sichuan ProvinceNational Clinical Research Center for GeriatricsWest China HospitalSichuan UniversityChengdu 610041China College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China

Manipulating the energy structure of materials represents an efficient way to regulate their light absorption behaviors. For example, constructing donor-acceptor(d-A) structures to increase the polarizability and reduce the energy bandgap of local molecules has been widely used in the field of organic photovoltaics with ordered structures. Remarkably, even in disordered and chaotic systems such as melanin-like polydopamine(PdA), visible and near-infrared light absorption can be significantly improved using this strategy. However, there has been a noticeable dearth of research on the ultraviolet(UV) light absorption regulation of bioinspired polymers with disordered and chaotic architectures by tailoring the d-A microstructures. In this study, a series of benzoheterocyclic molecules with strong electron-donating features screened by molecular simulation calculations were involved in disrupting the d-a structures within PdA. The destruction of d-a structures promoted the increase of the energy band gap and finally boosted the UV absorption of PdA. The resulting PdA nanoparticles with enhanced UV absorption were further employed to fabricate UV shielding composite films to protect the growth of plants from harmful UV radiation. This research may open up new avenues for structural disruption of bioinspired polymers for enhanced photoprotection applications.

关键词： melanin-like polymers polydopamine d-a structure UV absorption photoprotection

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Thermally Activated delayed Fluorescence of Aggregates Induced by Strongπ–πInteractions and Reversible dual-Responsive Luminescence Switching

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CCS Chemistry 2022年第2期4卷 625-637页

作者： Xiangyu Zhang Tong Lu Changjiang Zhou Haichao Liu Yating Wen Yue Shen Bao Li Shi-Tong Zhang Bing Yang State Key Laboratory of Supramolecular structure and Materials College of ChemistryJilin UniversityChangchun 130012 Shenzhen Key Laboratory of Polymer Science and Technology College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060

A reversible dual-responsive luminescent material was introduced by our group to show the simultaneous color and lifetime switching in response to external stimuli.Pristine crystalline powder of(E)-2-(benzo[d]thiazol-2-yl)-3-(pyren-1-yl)acrylonitrile(Py-BZTCN)shows the orderedπ–πstacking with only near-monomer-normal orange-yellow fluorescence,but it exhibits red emission with thermally activated delayed fluorescence(TAdF)after grinding,which can be reversibly recovered by heating or fuming treatment.Grinding disturbs the orderedπ–πstacking of pristine powder,leading to the formation of small aggregates with compressed distance and increased overlap ofπ–πstacking between adjacent molecules.The cause of switching was verified by single-crystal X-ray diffraction experiments of two corresponding crystals.This strongπ–πinteraction effectively promotes the excited-state energy splitting and substantially decreases the singlet–triplet energy gap(ΔEST)of aggregates,resulting in the red TAdF emission of aggregates through reverse intersystem crossing.This finding proposes a new route to realizing the TAdF emission of aggregates through strong intermolecular interactions based on non-TAdF monomer,thereby enabling a novel high-contrast dualresponsive luminescence switching.

关键词： one-dimensionalπ-πstacking thermally activated delayed fluorescence stimuli-responsive luminescence switches d-a structure chargetransfer state

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