(i) Our studies suggest that as the LA ratio increases, a better mixing of ChCl and LA is obtained, chang-ing significantly the environment around each ChCl ion pair. Several experimental investigations report that both ChCl and LA take part in the processing of lignin by ChCl-LA 1:2 and 1:10 , the former likely by interacting via the anion with the -O-4 bond and LA with the phenolic group of lignin . Furthermore, there is indication that the lignin is attached to both LA and ChCl when dissolved in ChCl:LA . Additionally, theoretical simulations on the 1:2 ChCl:LA system suggest synergistic e↵ects of chloride anion and LA acting on the same site of lignin . Our FF3 simulations indicate that at higher ChCl:LA ratios, more LA molecules surround each ChCl pair, which might increase the probability of a simultaneous interaction of the lignin that might improve the treatment.