Regulation of the Light Absorption and Photothermal Performance of Melanin-Like Polymers

作者：Yuan Zou, Tianyou Wang, Xu Lin, Lei Yang, Yiwen Li · 发表于：Accounts of Chemical Research · 年份：2025 · DOI：10.1021/acs.accounts.5c00346 · 被引用次数：44 · 研究领域：Photochromic and Fluorescence Chemistry、Gold and Silver Nanoparticles Synthesis and Applications、Polydiacetylene-based materials and applications

ConspectusMelanin-like polymers have attracted significant attention for their excellent light absorption and photothermal conversion properties. Unlike sequence-controlled biomacromolecules such as proteins and DNA, natural melanin and its analogues derive their broadband light absorption and photothermal performance from heterogeneous polymerization of 5,6-dihydroxyindole (DHI), indolequinone (IQ), and uncycled dopamine derivatives, as well as simultaneous progressive assembly between different monomeric species or oligomers. A key challenge in this field lies in establishing their structure-property relationships as well as precisely regulating the light absorption and photothermal performance of these bioinspired polymers to meet specific application requirements.Our research has revealed that nonradiative decay dominates their photothermal behavior, with absorbed optical energy converting to thermal vibrations within 1 ns, while regulating the light harvesting ability depends on molecular control over conjugation length, bandgap, and charge-transfer pathways through deliberate chemical design. By harnessing supramolecular assembly (hydrogen bonding, π-π interaction, cation-π interaction, etc.) and chemical reactions (metal-catechol coordination, Schiff base reaction, "click" chemistry, etc.), we have developed various emerging strategies, enabling customization of the light absorption regulation of melanin-like polymers. By leveraging covalent chemical toolboxes, electro...