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Performance of three delignifying pretreatments on hardwoods: hydrolysis yields, comprehensive mass balances, and lignin properties.

Identifieur interne : 000794 ( Main/Exploration ); précédent : 000793; suivant : 000795

Performance of three delignifying pretreatments on hardwoods: hydrolysis yields, comprehensive mass balances, and lignin properties.

Auteurs : Aditya Bhalla [États-Unis] ; Charles M. Cai [États-Unis] ; Feng Xu [États-Unis] ; Sandip K. Singh [États-Unis] ; Namita Bansal [États-Unis] ; Thanaphong Phongpreecha [États-Unis] ; Tanmoy Dutta [États-Unis] ; Cliff E. Foster [États-Unis] ; Rajeev Kumar [États-Unis] ; Blake A. Simmons [États-Unis] ; Seema Singh [États-Unis] ; Charles E. Wyman [États-Unis] ; Eric L. Hegg [États-Unis] ; David B. Hodge [États-Unis, Suède]

Source :

RBID : pubmed:31516552

Abstract

Background

In this work, three pretreatments under investigation at the DOE Bioenergy Research Centers (BRCs) were subjected to a side-by-side comparison to assess their performance on model bioenergy hardwoods (a eucalyptus and a hybrid poplar). These include co-solvent-enhanced lignocellulosic fractionation (CELF), pretreatment with an ionic liquid using potentially biomass-derived components (cholinium lysinate or [Ch][Lys]), and two-stage Cu-catalyzed alkaline hydrogen peroxide pretreatment (Cu-AHP). For each of the feedstocks, the pretreatments were assessed for their impact on lignin and xylan solubilization and enzymatic hydrolysis yields as a function of enzyme loading. Lignins recovered from the pretreatments were characterized for polysaccharide content, molar mass distributions, β-aryl ether content, and response to depolymerization by thioacidolysis.

Results

All three pretreatments resulted in significant solubilization of lignin and xylan, with the CELF pretreatment solubilizing the majority of both biopolymer categories. Enzymatic hydrolysis yields were shown to exhibit a strong, positive correlation with the lignin solubilized for the low enzyme loadings. The pretreatment-derived solubles in the [Ch][Lys]-pretreated biomass were presumed to contribute to inhibition of enzymatic hydrolysis in the eucalyptus as a substantial fraction of the pretreatment liquor was carried forward into hydrolysis for this pretreatment. The pretreatment-solubilized lignins exhibited significant differences in polysaccharide content, molar mass distributions, aromatic monomer yield by thioacidolysis, and β-aryl ether content. Key trends include a substantially higher polysaccharide content in the lignins recovered from the [Ch][Lys] pretreatment and high β-aryl ether contents and aromatic monomer yields from the Cu-AHP pretreatment. For all lignins, the

Conclusions

Overall, it was demonstrated that the three pretreatments highlighted in this study demonstrated uniquely different functionalities in reducing biomass recalcitrance and achieving higher enzymatic hydrolysis yields for the hybrid poplar while yielding a lignin-rich stream that may be suitable for valorization. Furthermore, modification of lignin during pretreatment, particularly cleavage of β-aryl ether bonds, is shown to be detrimental to subsequent depolymerization.


DOI: 10.1186/s13068-019-1546-0
PubMed: 31516552
PubMed Central: PMC6732840


Affiliations:


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<title xml:lang="en">Performance of three delignifying pretreatments on hardwoods: hydrolysis yields, comprehensive mass balances, and lignin properties.</title>
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<name sortKey="Bhalla, Aditya" sort="Bhalla, Aditya" uniqKey="Bhalla A" first="Aditya" last="Bhalla">Aditya Bhalla</name>
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<nlm:affiliation>1Department of Biochemistry & Molecular Biology, Michigan State University, East Lansing, MI 48824 USA.</nlm:affiliation>
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<wicri:cityArea>1Department of Biochemistry & Molecular Biology, Michigan State University, East Lansing</wicri:cityArea>
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<nlm:affiliation>2DOE Great Lakes Bioenergy Research Center (GLBRC), Michigan State University, East Lansing, MI 48824 USA.</nlm:affiliation>
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<region type="state">Californie</region>
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<name sortKey="Hegg, Eric L" sort="Hegg, Eric L" uniqKey="Hegg E" first="Eric L" last="Hegg">Eric L. Hegg</name>
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<nlm:affiliation>1Department of Biochemistry & Molecular Biology, Michigan State University, East Lansing, MI 48824 USA.</nlm:affiliation>
<country xml:lang="fr">États-Unis</country>
<placeName>
<region type="state">Michigan</region>
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<nlm:affiliation>2DOE Great Lakes Bioenergy Research Center (GLBRC), Michigan State University, East Lansing, MI 48824 USA.</nlm:affiliation>
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<region type="state">Montana</region>
</placeName>
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<nlm:affiliation>7Department of Chemical Engineering and Materials Science, Michigan State University, East Lansing, MI 48824 USA.</nlm:affiliation>
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<nlm:affiliation>8Division of Sustainable Process Engineering, Luleå University of Technology, Luleå, Sweden.</nlm:affiliation>
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<title level="j">Biotechnology for biofuels</title>
<idno type="ISSN">1754-6834</idno>
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<div type="abstract" xml:lang="en">
<p>
<b>Background</b>
</p>
<p>In this work, three pretreatments under investigation at the DOE Bioenergy Research Centers (BRCs) were subjected to a side-by-side comparison to assess their performance on model bioenergy hardwoods (a eucalyptus and a hybrid poplar). These include co-solvent-enhanced lignocellulosic fractionation (CELF), pretreatment with an ionic liquid using potentially biomass-derived components (cholinium lysinate or [Ch][Lys]), and two-stage Cu-catalyzed alkaline hydrogen peroxide pretreatment (Cu-AHP). For each of the feedstocks, the pretreatments were assessed for their impact on lignin and xylan solubilization and enzymatic hydrolysis yields as a function of enzyme loading. Lignins recovered from the pretreatments were characterized for polysaccharide content, molar mass distributions, β-aryl ether content, and response to depolymerization by thioacidolysis.</p>
</div>
<div type="abstract" xml:lang="en">
<p>
<b>Results</b>
</p>
<p>All three pretreatments resulted in significant solubilization of lignin and xylan, with the CELF pretreatment solubilizing the majority of both biopolymer categories. Enzymatic hydrolysis yields were shown to exhibit a strong, positive correlation with the lignin solubilized for the low enzyme loadings. The pretreatment-derived solubles in the [Ch][Lys]-pretreated biomass were presumed to contribute to inhibition of enzymatic hydrolysis in the eucalyptus as a substantial fraction of the pretreatment liquor was carried forward into hydrolysis for this pretreatment. The pretreatment-solubilized lignins exhibited significant differences in polysaccharide content, molar mass distributions, aromatic monomer yield by thioacidolysis, and β-aryl ether content. Key trends include a substantially higher polysaccharide content in the lignins recovered from the [Ch][Lys] pretreatment and high β-aryl ether contents and aromatic monomer yields from the Cu-AHP pretreatment. For all lignins, the </p>
</div>
<div type="abstract" xml:lang="en">
<p>
<b>Conclusions</b>
</p>
<p>Overall, it was demonstrated that the three pretreatments highlighted in this study demonstrated uniquely different functionalities in reducing biomass recalcitrance and achieving higher enzymatic hydrolysis yields for the hybrid poplar while yielding a lignin-rich stream that may be suitable for valorization. Furthermore, modification of lignin during pretreatment, particularly cleavage of β-aryl ether bonds, is shown to be detrimental to subsequent depolymerization.</p>
</div>
</front>
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<Month>10</Month>
<Day>01</Day>
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<Title>Biotechnology for biofuels</Title>
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<ArticleTitle>Performance of three delignifying pretreatments on hardwoods: hydrolysis yields, comprehensive mass balances, and lignin properties.</ArticleTitle>
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<AbstractText Label="Background" NlmCategory="UNASSIGNED">In this work, three pretreatments under investigation at the DOE Bioenergy Research Centers (BRCs) were subjected to a side-by-side comparison to assess their performance on model bioenergy hardwoods (a eucalyptus and a hybrid poplar). These include co-solvent-enhanced lignocellulosic fractionation (CELF), pretreatment with an ionic liquid using potentially biomass-derived components (cholinium lysinate or [Ch][Lys]), and two-stage Cu-catalyzed alkaline hydrogen peroxide pretreatment (Cu-AHP). For each of the feedstocks, the pretreatments were assessed for their impact on lignin and xylan solubilization and enzymatic hydrolysis yields as a function of enzyme loading. Lignins recovered from the pretreatments were characterized for polysaccharide content, molar mass distributions, β-aryl ether content, and response to depolymerization by thioacidolysis.</AbstractText>
<AbstractText Label="Results" NlmCategory="UNASSIGNED">All three pretreatments resulted in significant solubilization of lignin and xylan, with the CELF pretreatment solubilizing the majority of both biopolymer categories. Enzymatic hydrolysis yields were shown to exhibit a strong, positive correlation with the lignin solubilized for the low enzyme loadings. The pretreatment-derived solubles in the [Ch][Lys]-pretreated biomass were presumed to contribute to inhibition of enzymatic hydrolysis in the eucalyptus as a substantial fraction of the pretreatment liquor was carried forward into hydrolysis for this pretreatment. The pretreatment-solubilized lignins exhibited significant differences in polysaccharide content, molar mass distributions, aromatic monomer yield by thioacidolysis, and β-aryl ether content. Key trends include a substantially higher polysaccharide content in the lignins recovered from the [Ch][Lys] pretreatment and high β-aryl ether contents and aromatic monomer yields from the Cu-AHP pretreatment. For all lignins, the
<sup>13</sup>
C NMR-determined β-aryl ether content was shown to be correlated with the monomer yield with a second-order functionality.</AbstractText>
<AbstractText Label="Conclusions" NlmCategory="UNASSIGNED">Overall, it was demonstrated that the three pretreatments highlighted in this study demonstrated uniquely different functionalities in reducing biomass recalcitrance and achieving higher enzymatic hydrolysis yields for the hybrid poplar while yielding a lignin-rich stream that may be suitable for valorization. Furthermore, modification of lignin during pretreatment, particularly cleavage of β-aryl ether bonds, is shown to be detrimental to subsequent depolymerization.</AbstractText>
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<ForeName>Aditya</ForeName>
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<Affiliation>4BioEnergy Science Center (BESC) and Center for Bioenergy Innovation (CBI), Oak Ridge National Laboratory, Oak Ridge, TN 37831 USA.</Affiliation>
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<LastName>Hegg</LastName>
<ForeName>Eric L</ForeName>
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<AffiliationInfo>
<Affiliation>1Department of Biochemistry & Molecular Biology, Michigan State University, East Lansing, MI 48824 USA.</Affiliation>
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<AffiliationInfo>
<Affiliation>2DOE Great Lakes Bioenergy Research Center (GLBRC), Michigan State University, East Lansing, MI 48824 USA.</Affiliation>
<Identifier Source="ISNI">0000 0001 2150 1785</Identifier>
<Identifier Source="GRID">grid.17088.36</Identifier>
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<AffiliationInfo>
<Affiliation>6Chemical & Biological Engineering Department, Montana State University, Bozeman, MT 59715 USA.</Affiliation>
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<AffiliationInfo>
<Affiliation>7Department of Chemical Engineering and Materials Science, Michigan State University, East Lansing, MI 48824 USA.</Affiliation>
<Identifier Source="ISNI">0000 0001 2150 1785</Identifier>
<Identifier Source="GRID">grid.17088.36</Identifier>
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<AffiliationInfo>
<Affiliation>8Division of Sustainable Process Engineering, Luleå University of Technology, Luleå, Sweden.</Affiliation>
<Identifier Source="ISNI">0000 0001 1014 8699</Identifier>
<Identifier Source="GRID">grid.6926.b</Identifier>
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<Language>eng</Language>
<PublicationTypeList>
<PublicationType UI="D016428">Journal Article</PublicationType>
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<Year>2019</Year>
<Month>09</Month>
<Day>09</Day>
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<KeywordList Owner="NOTNLM">
<Keyword MajorTopicYN="N">Aromatic monomers</Keyword>
<Keyword MajorTopicYN="N">Cellulosic biofuels</Keyword>
<Keyword MajorTopicYN="N">Lignin</Keyword>
<Keyword MajorTopicYN="N">Pretreatment</Keyword>
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<CoiStatement>Competing interestsThe authors declare the following competing financial interests: DBH, ELH, AB, NB (Methods of Using Multi-Ligand Metal Complexes and to Perform Oxidative Catalytic Pretreatment of Lignocellulosic Biomass—2019/0091674 A1). As a holder of this patent, we may benefit financially from advances in the technology discussed in this manuscript.</CoiStatement>
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