We elucidate the effect of residual lignin on the interfacial, physical and mechanical properties of lignocellulose nanofibrils (LCNF) and respective nanopapers.

Technical lignins are structurally heterogeneous and polydisperse. This work describes the use of a simple and green method for lignin fractionation, using different proportions of acetone (40 and 60%) in water. Lignins from three different sources (wheat straw organosolv lignin, wheat straw soda lignin and softwood kraft lignin) were used in this fractionation protocol. The obtained fractions showed different molar mass and functional groups. The lower molar mass fractions showed more phenolic hydroxyl groups and carboxylic acid moieties than higher molar mass fractions, which also possessed much higher amounts of carbohydrates. The chemical characterization of these fractionated lignins showed that the PREC fraction was exceptionally pure and homogeneous lignin. Its total lignin content was >96% for all three lignins and it was practically free from carbohydrates and inorganics (ash). Furthermore, PREC fraction possessed the highest carbon content for the three lignin samples (63.05-69.26%). These results illustrate that the proposed aqueous acetone fractionation protocol could indeed produce pure and uniform lignin fraction and it was applicable for lignins from different sources.