Wet Spinning of Sodium Carboxymethyl Cellulose - Sodium Caseinate Hydrogel Fibres: Relationship between Rheology and Spinnability

Abstract

Mimicking the fibrous structures of meat is a significant challenge as natural plant protein assemblies lack the fibrous organisation ubiquitous in mammalian muscle tissues. In this work, wet-spun hydrogel fibres resembling the anisotropic fibrous microstructure of meat are fabricated using carboxymethyl cellulose as a model polysaccharide and sodium caseinate as a model protein which are crosslinked using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide (EDC). Hydrogels and spun fibres were characterised using a combination of rheology (shear, oscillatory, and extensional), microscopy (light, polarised, and fluorescence), rheo-NMR, and x-ray diffraction. Examination of structuring behaviour under shear uncovered a relationship between enhanced biopolymer orientation along the fibre axis and a viscoelastic time-dependant ageing window for optimal hydrogel spinnability. This study provides novel rheological and structural insights into mechanisms of protein-polysaccharide assembly that may prove instrumental for development of tuneable fibres for applications in plant-based foods, tissue engineering, and biomaterials.