Journal
GREEN CHEMISTRY
Volume 22, Issue 4, Pages 1378-1387Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9gc02760b
Keywords
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Funding
- Youth Program of National Natural Science Foundation of China [31901268]
- International Cooperation Funding of Qilu University of Technology [QLUTGJHZ2018027]
- Jiangsu Provincial Key Laboratory of Pulp and Paper Science and Technology [KL201905]
- Key Laboratory of Pulp and Paper Science and Technology of Ministry of Education/Shandong Province of China [030803138606]
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Currently, recyclable acid hydrotropes (p-TsOH), deep eutectic solvents (DES, ChCl-Lac), and ionic liquids (IL, [Amim][Cl]) are receiving increasing attention due to their superior delignification performance. However, very few mechanistic studies have shed light on the questions of how these solvents achieve the rapid dissolution of lignin and why they exhibit dramatic differences in the lignin removal. In this study, we first developed a comparative study of their delignification capacities. Under the same pretreatment temperature of 80 degrees C, three solvents exhibited a remarkable difference in the lignin removal: p-TsOH hydrotrope (86%, 1.5 h) > ChCl-Lac (11%, 15 h) > [Amim][Cl] (0%, 15 h). The extracted lignin samples were characterized via FTIR, TGA, P-31 NMR, and 2D HSQC NMR spectroscopy to evaluate their structural properties. Moreover, mechanistic insights into the differences in lignin removal were analyzed via combined quantum chemistry (QC) calculations and molecular dynamics (MD) simulations. The results indicated that both C-HMIDLINE HORIZONTAL ELLIPSIS pi and strong H-bonding interactions contribute to the highest interaction energy (Delta E = 15.11 kcal mol(-1)) between p-TsOH hydrotrope and VG, which resulted in the high lignin removal.
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