(ii) The formation of LA clusters detected by theoretical simulations in the 1:2 ChCl:LA systems , was suggested to have a two-fold impact on the lignin processing: on one hand, it was detected that such aggregations limit chlorine's di↵usivity and therefore limited the ability of the ChCl:LA DES to disrupt the lignincellulose bonds that lead to delignification. Additionally, the forming of LA groups in 1:2 prevented the LA hydroxyl groups to be available for interacting with the lignin. Our calculations suggest that by increasing the LA ratio the Cl -ChOH interaction becomes less relevant and the Cl is more available to interact with LA, resulting in less aggregation of LA. The availability of both Cl and LA would be consequently improved, resulting in a better interaction with the lignin and therefore, the performance of the treatment, as the experimental data indicates.