Multiscale investigation of the mechanism of biomass deconstruction in the dimethyl isosorbide/water Co-solvent pretreatment system

Yang, Shuang; Mohan, Mood; Gao, Xiangbo; Yang, Xianpeng; Zhu, Jiawei; Smith, Jeremy C.; Wang, Lei

doi:10.1039/d4gc00510d

Title: Multiscale investigation of the mechanism of biomass deconstruction in the dimethyl isosorbide/water Co-solvent pretreatment system

Journal Article · 12 March 2024 · Green Chemistry

DOI: https://doi.org/10.1039/d4gc00510d · OSTI ID:2333786

Yang, Shuang ^[1];

^[2];

^[1];

^[3]; Zhu, Jiawei ^[4];

^[5];

^[3]

Westlake Univ., Hangzhou (China); Zhejiang Univ., Hangzhou (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Westlake Univ., Hangzhou (China)
Zhejiang A&F University, Hangzhou (China)
Univ. of Tennessee, Knoxville, TN (United States)

In the context of promoting a circular bioeconomy, the development of green and efficient lignocellulosic biomass pretreatment technologies so as to realize high value-added biomass utilization is of intense interest. We demonstrated the potential of the bio-based green solvent dimethyl isosorbide (DMI) for the fractionation of Eucalyptus biomass with excellent performance. Here, to investigate the mechanisms involved in biomass fractionation, microimaging and microspectroscopic techniques were employed together with molecular dynamics (MD) simulation and COSMO-RS quantum chemical calculations to derive multiscale information. Both the microstructure and regional chemistry of the cell wall vary significantly with the volume ratio of DMI/H₂O. The strongest effects were found at DMI/H₂O = 9:1 and showed visible cell wall tearing cracks and cell wall deformation and collapse as well as the lowest values of cell wall thickness and circularity. From the MD simulations, lignin exhibits collapsed-like structure in pure H₂O with low solvent accessibility surface area (SASA) and radius of gyration (R_g). In contrast, lignin in DMI/H₂O shows extended structure with high SASA and solvent interactions dominated by van der Waals forces, with maximal contact in the 9:1 (v/v) system. Further, the COSMO-RS calculated sigma (σ-) potential suggests the intermolecular interactions in DMI and DMI/H₂O co-solvent are weak, leading to stronger interaction with lignin and correspondingly higher lignin dissolution. The radial distribution functions and σ-potential all show that again DMI/H₂O at 9:1 is an optimal volume ratio for high lignin dissolution. Finally, this study provides a solvent-ratio dependent mechanism for the action of polar aprotic solvents in the deconstruction of biomass.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2333786

Journal Information:: Green Chemistry, Journal Name: Green Chemistry Journal Issue: 8 Vol. 26; ISSN 1463-9262

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Multiscale investigation of the mechanism of biomass deconstruction in the dimethyl isosorbide/water Co-solvent pretreatment system

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