Enhanced formability and mechanical performance of wood hydrolysate films through reductive amination chain extension

An O-acetyl-4-O-methylglucuronoxylan-rich wood hydrolysate (WH), generated by the hydrothermal treatment of hardwood, was chain extended using di- and tri-functionalized amino chain extenders through reductive amination. Chain extension was achieved via facile one- or two-step syntheses. The carbohydrate chain extension efficiency, molecular weights, and branching patterns were determined through a combination of SEC, 1HNMR, FTIR and elemental analysis. The mild reaction conditions enabled an increase in the molecular weight while preserving the initial structures of the hemicelluloses. The chain extension strategy developed in this study was demonstrated to significantly improve the formability and mechanical performance of WH films, allowing for the water-casting production of coherent films with higher ratios of WH - 70-85% (w/w) - and reducing the need for co-components. Chain-extended WHs produced stronger and more ductile films than corresponding formulations prepared from unmodified WH. Films made from ethylenediamine chain-extended WH mixed with 30% (w/w) carboxymethyl cellulose showed a tensile strength of 62 MPa and a strain-to-failure of 3.3%. Additionally, chain-extended WHs produced films with an oxygen permeability as low as 0.2 cm3 μm m−2 day−1 kPa−1 at 50% RH.