ARC Centre of Excellence in Convergent Bio-Nano Science and Technology, and the Department of Chemical Engineering, The University of Melbourne, Parkville, Victoria, 3010, Australia.
Angew Chem Int Ed Engl. 2020 Jan 20;59(4):1711-1717. doi: 10.1002/anie.201913509. Epub 2019 Dec 4.
Functional coatings are of considerable interest because of their fundamental implications for interfacial assembly and promise for numerous applications. Universally adherent materials have recently emerged as versatile functional coatings; however, such coatings are generally limited to catechol, (ortho-diphenol)-containing molecules, as building blocks. Here, we report a facile, biofriendly enzyme-mediated strategy for assembling a wide range of molecules (e.g., 14 representative molecules in this study) that do not natively have catechol moieties, including small molecules, peptides, and proteins, on various surfaces, while preserving the molecule's inherent function, such as catalysis (≈80 % retention of enzymatic activity for trypsin). Assembly is achieved by in situ conversion of monophenols into catechols via tyrosinase, where films form on surfaces via covalent and coordination cross-linking. The resulting coatings are robust, functional (e.g., in protective coatings, biological imaging, and enzymatic catalysis), and versatile for diverse secondary surface-confined reactions (e.g., biomineralization, metal ion chelation, and N-hydroxysuccinimide conjugation).
功能涂层因其对界面组装的重要意义和在众多应用中的广阔前景而备受关注。最近，普遍黏附的材料作为多功能功能涂层应运而生；然而，此类涂层通常仅限于儿茶酚（邻二苯酚）类分子作为构建块。在这里，我们报告了一种简便、生物友好的酶介导策略，用于在各种表面上组装广泛的分子（例如，本研究中的 14 种代表性分子），这些分子原本不具有儿茶酚部分，包括小分子、肽和蛋白质，同时保持分子的固有功能，如催化（胰蛋白酶的酶活性保留约 80%）。通过漆酶将单酚原位转化为儿茶酚来实现组装，其中通过共价和配位交联在表面上形成薄膜。所得涂层坚固、功能多样（例如，在保护性涂层、生物成像和酶催化中），并且适用于各种二次表面受限反应（例如，生物矿化、金属离子螯合和 N-羟基琥珀酰亚胺缀合）。
