Photochemical ligation meets nanocellulose: a versatile platform for self-reporting functional materials
Photochemical ligation meets nanocellulose: a versatile platform for self-reporting functional materials
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DOI：
10.1039/c8mh00241j
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发表时间：
2018-05-01
影响因子：
13.3
通讯作者：
Walther, Andreas
中科院分区：
文献类型：
--
作者：
Hoenders, Daniel;Guo, Jiaqi;Walther, Andreas
纤维素纳米纤丝（CNFs）的可持续来源和高度有前途的机械和功能特性吸引了先进的功能材料的建设显着的兴趣。促进基于CNF的材料的功能性的一个关键方面是实施复杂的、容易的和通用的化学官能化原理，用于CNF性质的应用靶向改性，而与是否针对功能表面、水凝胶或本体材料无关。我们在此合并，第一次，自我报告的光诱导的模块化连接（UV诱导的腈亚胺介导的四唑/烯环加成，NITEC）与CNFs控制化学功能的空间和时间的可能性宏观荧光读出的反应进程。我们讨论了这种异质互补的光共轭相对于固定的光活性四唑单元CNFs在散装和分散体，并证明了三个重要的CNF为基础的材料类（表面，水凝胶和bioinspired纳米复合材料）通过修改与光互补的马来酰亚胺拴系的功能部分的应用。除了在透明纳米纸上实现选择性生物识别图案外，我们还提出了与生物材料相关的光诱导水凝胶化，以及散装生物启发纳米复合材料中的机械硬化。光化学连接在所有三种材料中顺利进行，具有截然不同的动力学（溶液到本体），因此建立了一种平台方法，以促进各种基于CNF的材料的自报告功能化。
The sustainable origin and highly promising mechanical and functional properties of cellulose nanofibrils (CNFs) attract significant interest for the construction of advanced functional materials. One key aspect of promoting the functionality of CNF-based materials is to implement sophisticated, facile and versatile chemical functionalization principles for application-targeted modification of CNF properties, independent of whether aiming for functional surfaces, hydrogels or bulk materials. We herein merge, for the first time, a self-reporting photo-induced modular ligation (the UV-induced nitrile imine-mediated tetrazole/ene cycloaddition, NITEC) with CNFs to control chemical functionality in space and time with the possibility for a macroscopic fluorescence readout of the reaction progress. We discuss this hetero-complementary photo-conjugation with respect to the immobilization of photoactive tetrazole units on CNFs in bulk and dispersion, and demonstrate the application for three important CNF-based material classes (surfaces, hydrogels and bioinspired nanocomposites) by modification with photo-complementary maleimide-tethered functional moieties. In addition to realizing selective biorecognition patterns on transparent nanopapers, we present photo-induced hydrogelation relevant for biomaterials, as well as mechanical stiffening in bioinspired nanocomposites in the bulk. The photochemical ligation proceeds smoothly in all three materials with vastly different dynamics (solution to bulk) and hence establishes a platform methodology to promote the self-reporting functionalization of diverse CNF-based materials.