文献类型：期刊文献

英文题名：Investigation into the effect of solvents on lignin hydrogenation for the production of phenolic compounds

作者：Liu, Chao[1,2] Wu, Yiqiang[1] Cai, Tingting[2] Chen, Yuwei[3] Jia, Shuya[4] Zhang, Xiaolei[4] Li, Zhaoshuang[1] Wu, Zhiping[1] Qing, Yan[1] Jiang, Jianchun[2] Wang, Kui[2]

第一作者：Liu, Chao

通信作者：Wu, YQ[1];Jiang, JC[2];Wang, K[2]

机构：[1]Cent South Univ Forestry & Technol, Sch Mat Sci & Engn, Changsha 410004, Peoples R China;[2]Inst Chem Ind Forest Prod, Chinese Acad Forestry, Key Lab Biomass Energy & Mat Jiangsu Prov, Natl Engn Lab Biomass Chem Utilizat, Nanjing 210042, Jiangsu, Peoples R China;[3]Yancheng Inst Technol, Sch Automot Engn, Yancheng 224051, Peoples R China;[4]Univ Strathclyde, Dept Chem & Proc Engn, Glasgow City G1 1XJ, Scotland

年份：2024

卷号：26

期号：6

起止页码：3356-3367

外文期刊名：GREEN CHEMISTRY

收录：;EI(收录号：20240815567193);Scopus(收录号：2-s2.0-85185153834);WOS:【SCI-EXPANDED(收录号:WOS:001160953700001)】；

基金：The authors would like to thank the National Key Research and Development Program of China (2022YFB4201904) and National Natural Science Foundation (32222058) for financial support. Computational work was performed on High-Performance Computer, ARCHIE-WeSt, at the University of Strathclyde.

语种：英文

外文关键词：Free energy - Hydrogenation - Mass transfer - Molecular dynamics - Molecules - Organic solvents - Phenols - Quantum chemistry - Quantum theory

摘要：Solvents play a critical role in the lignin hydrogenation process. However, elucidating the role of solvents in lignin hydrogenation solely through experimental methods presents considerable challenges. The present report integrates experimental results, quantum chemical calculations, and molecular dynamics simulations to study the effect of solvents on the hydrogenation of lignin on Ru/C to produce phenolic compounds. Solvents not only disperse the substrate and promote the mass transfer process in the hydrogenation reaction, but also significantly affect the hydrogenation reaction rate of lignin. We show that the hydrogenation reaction rates of lignin in different solvents differ by an order of magnitude (isopropanol > methanol > water > gamma-valerolactone > tetrahydrofuran). By innovatively combining quantum chemical calculations with experimental results, it was reported for the first time that solvent affects the free energy barrier by regulating the properties of the transition state (C-O bond strength), thereby affecting the lignin hydrogenolysis reaction rate. Based on molecular dynamics simulations, this study investigated the interaction between lignin and various solvent molecules. The research results confirmed that solvent molecules regulate the solvent shell on the surface of lignin, thereby influencing the mechanism of the hydrogenation reaction process.