globalchange  > 气候变化与战略
DOI: 10.1073/pnas.1922883117
论文题名:
Deconstruction of biomass enabled by local demixing of cosolvents at cellulose and lignin surfaces
作者: Pingali S.V.; Smith M.D.; Liu S.-H.; Rawal T.B.; Pu Y.; Shah R.; Evans B.R.; Urban V.S.; Davison B.H.; Cai C.M.; Ragauskas A.J.; O'Neill H.M.; Smith J.C.; Petridis L.
刊名: Proceedings of the National Academy of Sciences of the United States of America
ISSN: 0027-8424
出版年: 2020
卷: 117, 期:29
起始页码: 16776
结束页码: 16781
语种: 英语
英文关键词: Biomass ; Pretreatment ; Solvents
Scopus关键词: cellulose ; lignin ; tetrahydrofuran ; bacterial protein ; cellulase ; furan derivative ; lignin ; solvent ; surfactant ; Article ; biomass ; chemical structure ; concentration (parameter) ; fractionation ; hydrophobicity ; membrane permeability ; molecular dynamics ; neutron scattering ; particle size ; physical chemistry ; physical parameters ; priority journal ; surface property ; temperature measurement ; biomass ; biotechnology ; chemistry ; enzymology ; Gluconacetobacter xylinus ; hydrolysis ; metabolism ; Populus ; procedures ; wood ; Bacterial Proteins ; Biomass ; Biotechnology ; Cellulase ; Furans ; Gluconacetobacter xylinus ; Hydrolysis ; Lignin ; Populus ; Solvents ; Surface-Active Agents ; Wood
英文摘要: A particularly promising approach to deconstructing and fractionating lignocellulosic biomass to produce green renewable fuels and high-value chemicals pretreats the biomass with organic solvents in aqueous solution. Here, neutron scattering and molecular-dynamics simulations reveal the temperature-dependent morphological changes in poplar wood biomass during tetrahydrofuran (THF):water pretreatment and provide a mechanism by which the solvent components drive efficient biomass breakdown. Whereas lignin dissociates over a wide temperature range (>25 °C) cellulose disruption occurs only above 150 °C. Neutron scattering with contrast variation provides direct evidence for the formation of THF-rich nanoclusters (Rg ∼ 0.5 nm) on the nonpolar cellulose surfaces and on hydrophobic lignin, and equivalent water-rich nanoclusters on polar cellulose surfaces. The disassembly of the amphiphilic biomass is thus enabled through the local demixing of highly functional cosolvents, THF and water, which preferentially solvate specific biomass surfaces so as to match the local solute polarity. A multiscale description of the efficiency of THF:water pretreatment is provided: matching polarity at the atomic scale prevents lignin aggregation and disrupts cellulose, leading to improvements in deconstruction at the macroscopic scale. © 2020 National Academy of Sciences. All rights reserved.
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/163429
Appears in Collections:气候变化与战略

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作者单位: Pingali, S.V., Neutron Scattering Division, Oak Ridge National Laboratory, ORNL, Oak Ridge, TN 37830, United States; Smith, M.D., UT, ORNL, Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States, Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996, United States; Liu, S.-H., UT, ORNL, Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States; Rawal, T.B., UT, ORNL, Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States, Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996, United States; Pu, Y., Biosciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States; Shah, R., Neutron Scattering Division, Oak Ridge National Laboratory, ORNL, Oak Ridge, TN 37830, United States; Evans, B.R., Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States; Urban, V.S., Neutron Scattering Division, Oak Ridge National Laboratory, ORNL, Oak Ridge, TN 37830, United States; Davison, B.H., Biosciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States; Cai, C.M., Center for Environmental Research and Technology, Bourns College of Engineering, University of California, Riverside, CA 92521, United States, Center for Bioenergy Innovation, Oak Ridge National Laboratory, Oak Ridge, TN 37831, United States; Ragauskas, A.J., Biosciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States; O'Neill, H.M., Neutron Scattering Division, Oak Ridge National Laboratory, ORNL, Oak Ridge, TN 37830, United States, Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996, United States; Smith, J.C., UT, ORNL, Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States, Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996, United States; Petridis, L., UT, ORNL, Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830, United States, Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996, United States

Recommended Citation:
Pingali S.V.,Smith M.D.,Liu S.-H.,et al. Deconstruction of biomass enabled by local demixing of cosolvents at cellulose and lignin surfaces[J]. Proceedings of the National Academy of Sciences of the United States of America,2020-01-01,117(29)
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