Nature-Inspired Green Procedure for Improving Performance of Protein-Based Nanocomposites via Introduction of Nanofibrillated Cellulose-Stablized Graphene/Carbon Nanotubes Hybrid

Soy protein isolate (SPI) provides a potential alternative biopolymer source to fossil fuels, but improving the mechanical properties and water resistance of SPI composites remains a huge challenge. Inspired by the synergistic effect of natural nacre, we developed a novel approach to fabricate high-performance SPI nanocomposite films based on 2D graphene (G) nanosheets and 1D carbon nanotubes (CNTs) and nanofibrillated cellulose (NFC) using a casting method. The introduction of web-like NFC promoted the uniform dispersion of graphene/CNTs in the biopolymer matrix, as well as a high extent of cross-linkage combination between the fillers and SPI matrix. The laminated and cross-linked structures of the different nanocomposite films were observed by field-emission scanning electron microscope (FE-SEM) images. Due to the synergistic interactions of π–π stacking and hydrogen bonding between the nanofillers and SPI chains, the tensile strength of SPI/G/CNT/NFC film significantly increased by 78.9% and the water vapor permeability decreased by 31.76% in comparison to neat SPI film. In addition, the ultraviolet-visible (UV-vis) light barrier performance, thermal stability, and hydrophobicity of the films were significantly improved as well. This bioinspired synergistic reinforcing strategy opens a new path for constructing high-performance nanocomposites.