丝素
丝绸
热的
材料科学
负热膨胀
化学工程
高分子科学
复合材料
热膨胀
高分子化学
热力学
工程类
物理
作者
Haitao Liu,Jianliang Xiao,Shun Wang,Shuqi Ma,Chengchen Guo,Jiajia Zhong,Lei Zhang
标识
DOI:10.1016/j.cej.2024.149167
摘要
Developing thermally contractive polymeric materials with controlled conformational changes that enable more efficient actuation mechanisms has long been an ambitious goal. However, the utilization of naturally derived assemblies with biodegradable and reversible capabilities has, thus far, been hindered by the challenges associated with organizing the hierarchical nanostructures. Herein, hierarchically structured building blocks in regenerated fibroin were utilized to construct a thermal-responsive protein film through a friction-induced assemble strategy. By preserving the protofibrils within the regenerated silk film, we enable the efficient storage and transfer of elastic energy to external loads. The freestanding fibroin film, with pre-extended molecular chains, thus produced exhibited an exceedingly high negative thermal expansion (−1220 ppm K−1) and work capacity (∼203 J kg−1). The comprehensive analysis involving synchrotron infrared spectroscopy, in-situ Raman spectroscopy, and molecular dynamics simulations has confirmed that the actuating mechanism entails a reversible conformational change initiated by H-bonds, which is then amplified into macroscopic deformations by the hierarchical structure. This newly discovered, low-energy-driven mechanism paves the way for the creation of flexible protein assemblies with high-performance actuation capabilities.
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