Nano-fibrous biopolymers as building blocks for gel networks: Interactions, characterization, and applications.

Biopolymers derived from natural resources are highly abundant, biodegradable, and biocompatible, making them promising candidates to replace non-renewable fossil fuels and mitigate environmental and health impacts. Nano-fibrous biopolymers possessing advantages of biopolymers entangle with each other through inter-/intra-molecular interactions, serving as ideal building blocks for gel construction. These biopolymer nanofibers often synergize with other nano-building blocks to enhance gels with desirable functions and eco-friendliness across various applications in biomedical, environmental, and energy sectors. The inter-/intra-molecular interactions directly affect the assembly of nano-building blocks, which determines the structure of gels, and the integrity of connected nano-building blocks, influencing the mechanical properties and the performance of gels in specific applications. This review focuses on four biopolymer nanofibers (cellulose, chitin, silk, collagen), commonly used in gel preparations, as representatives for polysaccharides and polypeptides. The covalent and non-covalent interactions between biopolymers and other materials have been categorized and discussed in relation to the resulting gel network structures and properties. Nanomechanical characterization techniques, such as surface forces apparatus (SFA) and atomic force microscopy (AFM), have been employed to precisely quantify the intermolecular interactions between biopolymers and other building blocks. The applications of these gels are classified and correlated to the functions of their building blocks. The inter-/intra-molecular interactions act as "sewing threads", connecting all nano-building blocks to establish suitable network structures and functions. This review aims to provide a comprehensive understanding of the interactions involved in gel preparation and the design principles needed to achieve targeted functional gels.