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Deconstruction of biomass enabled by local demixing of cosolvents at cellulose and lignin surfaces.

Identifieur interne : 000489 ( Main/Exploration ); précédent : 000488; suivant : 000490

Deconstruction of biomass enabled by local demixing of cosolvents at cellulose and lignin surfaces.

Auteurs : Sai Venkatesh Pingali [États-Unis] ; Micholas Dean Smith [États-Unis] ; Shih-Hsien Liu [États-Unis] ; Takat B. Rawal [États-Unis] ; Yunqiao Pu [États-Unis] ; Riddhi Shah [États-Unis] ; Barbara R. Evans [États-Unis] ; Volker S. Urban [États-Unis] ; Brian H. Davison [États-Unis] ; Charles M. Cai [États-Unis] ; Arthur J. Ragauskas [États-Unis] ; Hugh M. O'Neill [États-Unis] ; Jeremy C. Smith [États-Unis] ; Loukas Petridis [États-Unis]

Source :

RBID : pubmed:32636260

Descripteurs français

English descriptors

Abstract

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.

DOI: 10.1073/pnas.1922883117
PubMed: 32636260
PubMed Central: PMC7382264


Affiliations:


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Le document en format XML

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<term>Bacterial Proteins (metabolism)</term>
<term>Biomass (MeSH)</term>
<term>Biotechnology (methods)</term>
<term>Cellulase (metabolism)</term>
<term>Furans (chemistry)</term>
<term>Gluconacetobacter xylinus (enzymology)</term>
<term>Hydrolysis (MeSH)</term>
<term>Lignin (chemistry)</term>
<term>Lignin (metabolism)</term>
<term>Populus (chemistry)</term>
<term>Solvents (chemistry)</term>
<term>Surface-Active Agents (chemistry)</term>
<term>Wood (chemistry)</term>
</keywords>
<keywords scheme="KwdFr" xml:lang="fr">
<term>Biomasse (MeSH)</term>
<term>Biotechnologie (méthodes)</term>
<term>Bois (composition chimique)</term>
<term>Cellulase (métabolisme)</term>
<term>Furanes (composition chimique)</term>
<term>Gluconacetobacter xylinus (enzymologie)</term>
<term>Hydrolyse (MeSH)</term>
<term>Lignine (composition chimique)</term>
<term>Lignine (métabolisme)</term>
<term>Populus (composition chimique)</term>
<term>Protéines bactériennes (métabolisme)</term>
<term>Solvants (composition chimique)</term>
<term>Tensioactifs (composition chimique)</term>
</keywords>
<keywords scheme="MESH" type="chemical" qualifier="chemistry" xml:lang="en">
<term>Furans</term>
<term>Lignin</term>
<term>Solvents</term>
<term>Surface-Active Agents</term>
</keywords>
<keywords scheme="MESH" type="chemical" qualifier="metabolism" xml:lang="en">
<term>Bacterial Proteins</term>
<term>Cellulase</term>
<term>Lignin</term>
</keywords>
<keywords scheme="MESH" qualifier="chemistry" xml:lang="en">
<term>Populus</term>
<term>Wood</term>
</keywords>
<keywords scheme="MESH" qualifier="composition chimique" xml:lang="fr">
<term>Bois</term>
<term>Furanes</term>
<term>Lignine</term>
<term>Populus</term>
<term>Solvants</term>
<term>Tensioactifs</term>
</keywords>
<keywords scheme="MESH" qualifier="enzymologie" xml:lang="fr">
<term>Gluconacetobacter xylinus</term>
</keywords>
<keywords scheme="MESH" qualifier="enzymology" xml:lang="en">
<term>Gluconacetobacter xylinus</term>
</keywords>
<keywords scheme="MESH" qualifier="methods" xml:lang="en">
<term>Biotechnology</term>
</keywords>
<keywords scheme="MESH" qualifier="métabolisme" xml:lang="fr">
<term>Cellulase</term>
<term>Lignine</term>
<term>Protéines bactériennes</term>
</keywords>
<keywords scheme="MESH" qualifier="méthodes" xml:lang="fr">
<term>Biotechnologie</term>
</keywords>
<keywords scheme="MESH" xml:lang="en">
<term>Biomass</term>
<term>Hydrolysis</term>
</keywords>
<keywords scheme="MESH" xml:lang="fr">
<term>Biomasse</term>
<term>Hydrolyse</term>
</keywords>
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<front>
<div type="abstract" xml:lang="en">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 (R
<sub>g</sub>
∼ 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.</div>
</front>
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<Year>2020</Year>
<Month>09</Month>
<Day>07</Day>
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<Year>2020</Year>
<Month>09</Month>
<Day>07</Day>
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<ISSN IssnType="Electronic">1091-6490</ISSN>
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<Volume>117</Volume>
<Issue>29</Issue>
<PubDate>
<Year>2020</Year>
<Month>07</Month>
<Day>21</Day>
</PubDate>
</JournalIssue>
<Title>Proceedings of the National Academy of Sciences of the United States of America</Title>
<ISOAbbreviation>Proc Natl Acad Sci U S A</ISOAbbreviation>
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<ArticleTitle>Deconstruction of biomass enabled by local demixing of cosolvents at cellulose and lignin surfaces.</ArticleTitle>
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<Abstract>
<AbstractText>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 (R
<sub>g</sub>
∼ 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.</AbstractText>
<CopyrightInformation>Copyright © 2020 the Author(s). Published by PNAS.</CopyrightInformation>
</Abstract>
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<Author ValidYN="Y">
<LastName>Pingali</LastName>
<ForeName>Sai Venkatesh</ForeName>
<Initials>SV</Initials>
<AffiliationInfo>
<Affiliation>Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, ORNL TN 37830.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y">
<LastName>Smith</LastName>
<ForeName>Micholas Dean</ForeName>
<Initials>MD</Initials>
<AffiliationInfo>
<Affiliation>UT/ORNL Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
<AffiliationInfo>
<Affiliation>Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y">
<LastName>Liu</LastName>
<ForeName>Shih-Hsien</ForeName>
<Initials>SH</Initials>
<AffiliationInfo>
<Affiliation>UT/ORNL Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
</Author>
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<LastName>Rawal</LastName>
<ForeName>Takat B</ForeName>
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<Identifier Source="ORCID">0000-0003-3191-7770</Identifier>
<AffiliationInfo>
<Affiliation>UT/ORNL Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
<AffiliationInfo>
<Affiliation>Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996.</Affiliation>
</AffiliationInfo>
</Author>
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<LastName>Pu</LastName>
<ForeName>Yunqiao</ForeName>
<Initials>Y</Initials>
<AffiliationInfo>
<Affiliation>Biosciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
</Author>
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<LastName>Shah</LastName>
<ForeName>Riddhi</ForeName>
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<Affiliation>Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
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</AffiliationInfo>
</Author>
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<LastName>Davison</LastName>
<ForeName>Brian H</ForeName>
<Initials>BH</Initials>
<Identifier Source="ORCID">0000-0002-7408-3609</Identifier>
<AffiliationInfo>
<Affiliation>Biosciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
</Author>
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<LastName>Cai</LastName>
<ForeName>Charles M</ForeName>
<Initials>CM</Initials>
<Identifier Source="ORCID">0000-0002-5047-0815</Identifier>
<AffiliationInfo>
<Affiliation>Center for Environmental Research and Technology, Bourns College of Engineering, University of California, Riverside, CA 92521.</Affiliation>
</AffiliationInfo>
<AffiliationInfo>
<Affiliation>Center for Bioenergy Innovation, Oak Ridge National Laboratory, Oak Ridge, TN 37831.</Affiliation>
</AffiliationInfo>
</Author>
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<LastName>Ragauskas</LastName>
<ForeName>Arthur J</ForeName>
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<Identifier Source="ORCID">0000-0002-3536-554X</Identifier>
<AffiliationInfo>
<Affiliation>Biosciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
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</Author>
<Author ValidYN="Y">
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<ForeName>Hugh M</ForeName>
<Initials>HM</Initials>
<AffiliationInfo>
<Affiliation>Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, ORNL TN 37830.</Affiliation>
</AffiliationInfo>
<AffiliationInfo>
<Affiliation>Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y">
<LastName>Smith</LastName>
<ForeName>Jeremy C</ForeName>
<Initials>JC</Initials>
<AffiliationInfo>
<Affiliation>UT/ORNL Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830.</Affiliation>
</AffiliationInfo>
<AffiliationInfo>
<Affiliation>Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996.</Affiliation>
</AffiliationInfo>
</Author>
<Author ValidYN="Y">
<LastName>Petridis</LastName>
<ForeName>Loukas</ForeName>
<Initials>L</Initials>
<AffiliationInfo>
<Affiliation>UT/ORNL Center for Molecular Biophysics, Oak Ridge National Laboratory, Oak Ridge, TN 37830; petridisl@ornl.gov.</Affiliation>
</AffiliationInfo>
<AffiliationInfo>
<Affiliation>Department of Biochemistry and Cellular and Molecular Biology, University of Tennessee, Knoxville, TN 37996.</Affiliation>
</AffiliationInfo>
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<PublicationType UI="D013486">Research Support, U.S. Gov't, Non-P.H.S.</PublicationType>
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<Month>07</Month>
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<MeshHeading>
<DescriptorName UI="D032107" MajorTopicYN="N">Populus</DescriptorName>
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<MeshHeading>
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<Keyword MajorTopicYN="Y">pretreatment</Keyword>
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</record>

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EXPLOR_STEP=$WICRI_ROOT/Bois/explor/PoplarV1/Data/Main/Exploration
HfdSelect -h $EXPLOR_STEP/biblio.hfd -nk 000489 | SxmlIndent | more

Ou

HfdSelect -h $EXPLOR_AREA/Data/Main/Exploration/biblio.hfd -nk 000489 | SxmlIndent | more

Pour mettre un lien sur cette page dans le réseau Wicri

{{Explor lien
   |wiki=    Bois
   |area=    PoplarV1
   |flux=    Main
   |étape=   Exploration
   |type=    RBID
   |clé=     pubmed:32636260
   |texte=   Deconstruction of biomass enabled by local demixing of cosolvents at cellulose and lignin surfaces.
}}

Pour générer des pages wiki

HfdIndexSelect -h $EXPLOR_AREA/Data/Main/Exploration/RBID.i   -Sk "pubmed:32636260" \
       | HfdSelect -Kh $EXPLOR_AREA/Data/Main/Exploration/biblio.hfd   \
       | NlmPubMed2Wicri -a PoplarV1 

Wicri

This area was generated with Dilib version V0.6.37.
Data generation: Wed Nov 18 12:07:19 2020. Site generation: Wed Nov 18 12:16:31 2020