Study on the Crosslinking of Glycerol Triglycidyl Ether and Lyocell Based on Molecular Dynamics Simulations and Its Anti-Fibrillation Performance: from Simulation to Experiment

Lyocell is a regenerated cellulose fiber with high potential for sustainable textile applications, but its fibrillation remains a major limitation. Crosslinking can suppress fibrillation by constructing a network structure. However, its molecular-level behavior remains unclear. Here, molecular dynamics simulations and Gibbs free energy calculations investigated the crosslinking behavior of glycerol triglycidyl ether (GTE) in lyocell fibers. Radial distribution function, mean square displacement, and diffusion coefficient analyses indicated that GTE preferentially interacts with −R3CH2−OH groups in amorphous cellulose regions. Negative Gibbs free energy change demonstrated thermodynamic feasibility and formation of a stable triple-crosslinked structure. To validate the theoretical findings, GTE crosslinking modification of lyocell fibers was experimentally conducted. XPS, FT-IR, and swelling analyses confirmed crosslinking, while GTE improved fibrillation resistance of lyocell fibers without significantly compromising whiteness, strength, or dyeing performance. This study provides a solid theoretical foundation for subsequent research on crosslinking systems in heterogeneous lyocell fibers.