Abstract
Silk is a naturally occurring high-performance material that can surpass man-made polymers in toughness and strength. The remarkable mechanical properties of silk result from the primary sequence of silk fibroin, which bears semblance to a linear segmented copolymer with alternating rigid (“crystalline”) and flexible (“amorphous”) blocks. Silk-mimetic polymers are therefore of great emerging interest, as they can potentially exhibit the advantageous features of natural silk while possessing synthetic flexibility as well as non-natural compositions. This review describes the relationships between primary sequence and material properties in natural silk fibroin and furthermore discusses chemical approaches towards the synthesis of silk-mimetic polymers. In particular, step-growth polymerization, controlled radical polymerization, and copolymerization with naturally derived silk fibroin are presented as strategies for synthesizing silk-mimetic polymers with varying molecular weights and degrees of sequence control. Strategies for improving macromolecular solubility during polymerization are also highlighted. Lastly, the relationships between synthetic approach, supramolecular structure, and bulk material properties are explored in this review, with the aim of providing an informative perspective on the challenges facing chemical synthesis of silk-mimetic polymers with desirable properties.
Highlights
Silk is a protein-based material with extraordinary properties
Dragline silk produced by the major ampullate gland of these spiders is responsible for the robust framework of spider webs and has been shown to exhibit mechanical properties that are unmatched by almost any other man-made or natural material [1,2,3]
Extensive discussion of these recent research efforts has been presented in several seminal review articles [27,28] but is beyond the scope of our current review, which will focus on discussing methods and perspectives relevant to the chemical synthesis of silk-mimetic polymers
Summary
Silk is a protein-based material with extraordinary properties. Produced by many orders of arachnids and insects, such as Lepidoptera, Hymenoptera, Diptera, Neuroptera, and Araneae, silk functions as a structural fiber spun on demand for applications ranging from prey capture to egg encasement. Researchers have shown that silk can be processed by inkjet printing [22], soft lithography [23], and nanoimprinting with and without readily incorporated fluorophores [24,25] to form novel nano/micro-patterned protein-based photonic materials, such as active optofluidic devices [26]. Extensive discussion of these recent research efforts has been presented in several seminal review articles [27,28] but is beyond the scope of our current review, which will focus on discussing methods and perspectives relevant to the chemical synthesis of silk-mimetic polymers. We will discuss the current state-of-art developments in chemical synthesis of silk-mimetic polymers and summarize the principal challenges facing the field, providing outlooks towards future developments
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