Architecture-governed dissolution-free conversion of lignocellulosic biomass into cellulose I beads by...

Cellulose beads are produced through dissolution-regeneration processes that are solvent- and water-intensive and disrupt the native microfibrillar organization by converting cellulose I to cellulose II. Here, we establish a dissolution-free chemomechanical pathway that converts lignocellulosic biomass into spherical cellulose assemblies via architecture-governed cell-wall remodeling and shear-driven consolidation. Six feedstocks spanning agricultural residues (date palm, rice straw, corn straw, soybean straw) and woody biomasses (pine and peach wood) were subjected to sequential alkaline extraction, oxidative bleaching, and high-shear agitation. Comparative compositional, structural, and morphological analyses reveal that successful spheronization does not depend solely on cellulose content but requires the formation of a deformable continuity-preserving fibrillar intermediate. In this state, partial matrix removal induces wall swelling and delamination while maintaining load-bearing connectors that enable fibrillar bending, entanglement, and densification under hydrodynamic shear. Date palm and rice straw satisfy these criteria and produce stable cellulose I beads with fiber-assembled interiors. In contrast, corn and soybean residues undergo excessive fragmentation into fines that disperse as pulps/flocs, whereas pine and peach wood retain stratified, locked wall domains and yield irregular, rigid fragments. These findings establish an architecture-based mechanistic framework and selection rules for solvent-minimal, dissolution-free manufacturing of cellulose beads directly from low-value lignocellulosic biomass.