Structure–Property Relationships in Cellulose Microbeads through Different Crosslinking Architectures

Cellulose has attracted considerable attention as a sustainable material because of its biodegradability, renewability, and natural abundance. However, its inherently low mechanical stability limits its broader utilization in structural and functional applications. Chemical crosslinking is an effective strategy for reinforcing cellulose networks, yet the influence of different crosslinking architectures on the resulting structure–property relationships has not been fully clarified.

In this study, cellulose microbeads were chemically crosslinked using four representative crosslinkers: epichlorohydrin (ECH), ethylene glycol diglycidyl ether (EGDGE), citric acid (CA), and 1,2,3,4-butanetetracarboxylic acid (BTCA). The effects of crosslinking chemistry on the internal network structure and mechanical performance were systematically investigated through swelling behavior, density measurements, FT-IR spectroscopy, thermal analysis (TGA and DSC), scanning electron microscopy (SEM), and nanoindentation.

The results demonstrate that different crosslinking architectures significantly influence the porous structure, crosslinking density, thermal behavior, and stiffness of the cellulose microbeads. These findings provide valuable insights into the structure–property relationships of crosslinked cellulose systems and offer practical guidelines for designing cellulose-based materials with tailored mechanical properties through appropriate crosslinker selection.