Molecular Fractionation Induced by Viscosity-Driven Segregative Phase Separation Behavior of Gum Arabic/Hydroxypropyl Methylcellulose

Segregative phase separation technology demonstrates substantial potential for precise molecular fractionation in food and biomaterial applications. The investigation elucidates the causal relationship between viscosity variations and phase separation dynamics, which govern molecular fractionation in GA/HPMC composite systems. By conducting a comparative analysis of two GA subtypes (CGA and SGA) and three HPMC grades with controlled viscosity gradients, we utilized gel permeation chromatography-multi-angle laser light scattering (GPC-MALLS) coupled with rheological characterization to elucidate the critical relationship between continuous phase viscosity and fractionation efficiency. Notably, increasing HPMC viscosity significantly intensified phase separation, resulting in selective enrichment of arabinogalactan-protein complexes: from 6.3% to 8.5% in CGA/HPMC systems and from 27.3% to 36.5% in SGA/HPMC systems. Further mechanistic investigation revealed that elevated HPMC viscosity enhances thermodynamic incompatibility while slowing interfacial mass transfer, synergistically driving component redistribution. These findings establish a quantitative viscosity–fractionation relationship, offering theoretical insights for optimizing GA/HPMC systems in emulsion stabilization, microencapsulation, and functional biopolymer purification via viscosity-mediated phase engineering.