Peng Huisheng, Tang Jing, Pang Jiebin, Chen Daoyong, Yang Lu, Ashbaugh Henry S, Brinker C Jeffrey, Yang Zhenzhong, Lu Yunfeng
Department of Chemical and Biomolecular Engineering, Tulane University, New Orleans, Louisiana 70118, USA.
J Am Chem Soc. 2005 Sep 21;127(37):12782-3. doi: 10.1021/ja053966p.
Conjugated polydiacetylene (PDA)/silica nanocomposites with tunable mesostructures and reversible thermochromatism were synthesized through self-directed assembly of diacetylenic silanes. In contrast to the previous studies, where the PDA side chains interacted weakly through noncovalent interactions, the side chains in the present nanocomposites are covalently connected to the inorganic silica frameworks, providing control over the molecular alignment, stability, and electronic properties. Furthermore, tuning the molecular architecture (e.g., the shape and side-chain length) allows control over the mesostructure (e.g., cubic and lamellar) and chromatic response of the nanocomposites (from irreversible to partially reversible and then to completely reversible). As a result of the covalent interactions, the nanocomposites also demonstrate higher reversible chromatic transition temperatures. This work not only provides responsive robust chromatic materials toward practically reusable PDA sensors but also is of great fundamental value for the design of supramolecular assembly and the understanding of the chromatic mechanism of PDA.
通过二乙炔基硅烷的自导向组装合成了具有可调介观结构和可逆热致变色性的共轭聚二乙炔(PDA)/二氧化硅纳米复合材料。与之前的研究不同,在之前的研究中PDA侧链通过非共价相互作用弱相互作用,而在本纳米复合材料中,侧链与无机二氧化硅骨架共价连接,从而能够控制分子排列、稳定性和电子性质。此外,调节分子结构(例如形状和侧链长度)可以控制纳米复合材料的介观结构(例如立方和层状)和颜色响应(从不可逆到部分可逆,再到完全可逆)。由于共价相互作用,纳米复合材料还表现出更高的可逆颜色转变温度。这项工作不仅为实际可重复使用的PDA传感器提供了响应灵敏的坚固变色材料,而且对于超分子组装的设计和对PDA颜色机制的理解具有重要的基础价值。