Lignin is the most abundant natural aromatic polymer on earth, promising an abundant source of renewable feedstock for future material applications [1]. Lignin is closely assembled with hemicellulose and cellulose in the plant cell wall, and deeper knowledge on the interactions and influences between these biomacromolecules is needed for effective valorization [2].Polymerization of synthetic lignin from coniferyl alcohol has been carried out in both absence and presence of hemicellulose-rich cellulose nanofibril matrices, to study the effect of carbohydrate presence on the lignin inter-unit linkage sequence. Lignin populations obtained by simple solvent fractionation from the carbohydrate matrix experiments have been examined using 2D-HSQC NMR and MALDI-TOF MS, and possible oligomers have been reconstructed from the obtained data using simple algorithms. Theoretical simulations were employed to study lignin-hemicellulose-cellulose-solvent interactions under various conditions. Oligomers from experiments severed as inputs for molecular dynamic simulations (MD), by studying the binding free energy ΔG of designed systems, the forces that govern the interactions were studied. The simulation revealed how lignin oligomers with specific inter-unit linkage sequences associate with carbohydrates and provided molecular-level insights into experimental observations, advancing lignin utilization strategies.
This is a joint submitted abstract together with Shuhan Lu.