Chenyang Shi,Yuna Bae,Mingyi Zhang,James J. De Yoreo
Silk is a unique and exceptionally strong biological material. However, no synthetic method has yet come close to replicating the properties of natural silk. This shortfall is attributed to an insufficient understanding of both silk nanofibril structure and the mechanism of formation. Here in situ atomic force microscopy (AFM) and photo-induced force microscopy (PiFM) is utilized to investigate the formation process and define the basic structural paradigm of individual silk nanofibrils. By visualizing the multistage process of silk nanofibril formation, the importance of conformational transformations along the assembly pathway is revealed. Unfolded silk structures initially accumulate into amorphous clusters, which then evolve into crystal nuclei via conformational transformation into β-crystallites. Nanofibril elongation then occurs through the attachment of silk molecules at a single end of the nanofibril tip; this is facilitated through the formation of a new amorphous cluster that then repeats the aforementioned conformational transformation. However, enzymatic digestion of the amorphous regions leads to direct, rapid elongation of β-crystalline fibers. These findings imply that the energy landscape is characterized by shallow minima associated with intermediate states, which can be eliminated by introducing β-crystallites, and motivate research into the directed modification of the silk assembly pathway to select for features beneficial to specific applications.
Chenyang Shi,Jingjuan Wang,Maria L. Sushko,Wu Qiu,Xiaobing Yan,Xiang Yang Liu
Functionalization of flexible materials based on mesoscopic reconstruction is a key strategy in fabricating biocompatible flexible electronics. This work is to acquire new mesoscopic bioelectronic hybrid materials of silk fibroin (SF)-Ag nanoclusters (AgNCs@BSA; BSA: bovine serum albumin), which enhance significantly the performance of silk memristors. It is to build AgNCs@BSA into SF mesoscopic networks by templated β-crystallization. Atomic force microscopy potential probing indicates that AgNCs@BSA serve as electronic potential wells that change completely the transport behavior of charge particles within the SF films. This leads to significant enhancement in the switching speed (≈10 ns), very good switching stability, extremely low set/reset voltages (0.3/−0.18 V) of SF meso-hybrid memristors, compared with the original and other organic memristors, and displays unique synapse characteristics and the capability of synapse learning. Classical density functional theory Poisson–Nernst–Planck simulations indicate that the enhanced performance is subject to the low potential paths interconnecting the AgNCs@BSA, which guide charges' transport (Ag + ) and deposition in SF films.
危险品化学品经营许可证（带存储）