Mesoscale Reaction-Diffusion Phenomena Governing Lignin-First Biomass Fractionation.
Identifieur interne : 000276 ( Main/Exploration ); précédent : 000275; suivant : 000277Mesoscale Reaction-Diffusion Phenomena Governing Lignin-First Biomass Fractionation.
Auteurs : Nicholas E. Thornburg [États-Unis] ; M Brennan Pecha [États-Unis] ; David G. Brandner [États-Unis] ; Michelle L. Reed [États-Unis] ; Josh V. Vermaas [États-Unis] ; William E. Michener [États-Unis] ; Rui Katahira [États-Unis] ; Todd B. Vinzant [États-Unis] ; Thomas D. Foust [États-Unis] ; Bryon S. Donohoe [États-Unis] ; Yuriy Román-Leshkov [États-Unis] ; Peter N. Ciesielski [États-Unis] ; Gregg T. Beckham [États-Unis]Source :
- ChemSusChem [ 1864-564X ] ; 2020.
Abstract
Lignin solvolysis from the plant cell wall is the critical first step in lignin depolymerization processes involving whole biomass feedstocks. However, little is known about the coupled reaction kinetics and transport phenomena that govern the effective rates of lignin extraction. Here, we report a validated simulation framework that determines intrinsic, transport-independent kinetic parameters for the solvolysis of lignin, hemicellulose, and cellulose upon incorporation of feedstock characteristics for the methanol-based extraction of poplar as an example fractionation process. Lignin fragment diffusion is predicted to compete on the same time and length scales as reactions of lignin within cell walls and longitudinal pores of typical milled particle sizes, and mass transfer resistances are predicted to dominate the solvolysis of poplar particles that exceed approximately 2 mm in length. Beyond the approximately 2 mm threshold, effectiveness factors are predicted to be below 0.25, which implies that pore diffusion resistances may attenuate observable kinetic rate measurements by at least 75 % in such cases. Thus, researchers are recommended to conduct kinetic evaluations of lignin-first catalysts using biomass particles smaller than approximately 0.2 mm in length to avoid feedstock-specific mass transfer limitations in lignin conversion studies. Overall, this work highlights opportunities to improve lignin solvolysis by genetic engineering and provides actionable kinetic information to guide the design and scale-up of emerging biorefinery strategies.
DOI: 10.1002/cssc.202000558
PubMed: 32246557
Affiliations:
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Thornburg</name><affiliation wicri:level="1"><nlm:affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Pecha, M Brennan" sort="Pecha, M Brennan" uniqKey="Pecha M" first="M Brennan" last="Pecha">M Brennan Pecha</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Brandner, David G" sort="Brandner, David G" uniqKey="Brandner D" first="David G" last="Brandner">David G. Brandner</name><affiliation wicri:level="1"><nlm:affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Reed, Michelle L" sort="Reed, Michelle L" uniqKey="Reed M" first="Michelle L" last="Reed">Michelle L. Reed</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Vermaas, Josh V" sort="Vermaas, Josh V" uniqKey="Vermaas J" first="Josh V" last="Vermaas">Josh V. Vermaas</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Michener, William E" sort="Michener, William E" uniqKey="Michener W" first="William E" last="Michener">William E. Michener</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Katahira, Rui" sort="Katahira, Rui" uniqKey="Katahira R" first="Rui" last="Katahira">Rui Katahira</name><affiliation wicri:level="1"><nlm:affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Vinzant, Todd B" sort="Vinzant, Todd B" uniqKey="Vinzant T" first="Todd B" last="Vinzant">Todd B. Vinzant</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Foust, Thomas D" sort="Foust, Thomas D" uniqKey="Foust T" first="Thomas D" last="Foust">Thomas D. Foust</name><affiliation wicri:level="1"><nlm:affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Donohoe, Bryon S" sort="Donohoe, Bryon S" uniqKey="Donohoe B" first="Bryon S" last="Donohoe">Bryon S. Donohoe</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Roman Leshkov, Yuriy" sort="Roman Leshkov, Yuriy" uniqKey="Roman Leshkov Y" first="Yuriy" last="Román-Leshkov">Yuriy Román-Leshkov</name><affiliation wicri:level="1"><nlm:affiliation>Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139</wicri:regionArea><wicri:noRegion>02139</wicri:noRegion></affiliation></author><author><name sortKey="Ciesielski, Peter N" sort="Ciesielski, Peter N" uniqKey="Ciesielski P" first="Peter N" last="Ciesielski">Peter N. Ciesielski</name><affiliation wicri:level="1"><nlm:affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author><author><name sortKey="Beckham, Gregg T" sort="Beckham, Gregg T" uniqKey="Beckham G" first="Gregg T" last="Beckham">Gregg T. Beckham</name><affiliation wicri:level="1"><nlm:affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401</wicri:regionArea><wicri:noRegion>80401</wicri:noRegion></affiliation></author></analytic><series><title level="j">ChemSusChem</title><idno type="eISSN">1864-564X</idno><imprint><date when="2020" type="published">2020</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Lignin solvolysis from the plant cell wall is the critical first step in lignin depolymerization processes involving whole biomass feedstocks. However, little is known about the coupled reaction kinetics and transport phenomena that govern the effective rates of lignin extraction. Here, we report a validated simulation framework that determines intrinsic, transport-independent kinetic parameters for the solvolysis of lignin, hemicellulose, and cellulose upon incorporation of feedstock characteristics for the methanol-based extraction of poplar as an example fractionation process. Lignin fragment diffusion is predicted to compete on the same time and length scales as reactions of lignin within cell walls and longitudinal pores of typical milled particle sizes, and mass transfer resistances are predicted to dominate the solvolysis of poplar particles that exceed approximately 2 mm in length. Beyond the approximately 2 mm threshold, effectiveness factors are predicted to be below 0.25, which implies that pore diffusion resistances may attenuate observable kinetic rate measurements by at least 75 % in such cases. Thus, researchers are recommended to conduct kinetic evaluations of lignin-first catalysts using biomass particles smaller than approximately 0.2 mm in length to avoid feedstock-specific mass transfer limitations in lignin conversion studies. Overall, this work highlights opportunities to improve lignin solvolysis by genetic engineering and provides actionable kinetic information to guide the design and scale-up of emerging biorefinery strategies.</div></front></TEI><pubmed><MedlineCitation Status="Publisher" Owner="NLM"><PMID Version="1">32246557</PMID><DateRevised><Year>2020</Year><Month>05</Month><Day>08</Day></DateRevised><Article PubModel="Print-Electronic"><Journal><ISSN IssnType="Electronic">1864-564X</ISSN><JournalIssue CitedMedium="Internet"><PubDate><Year>2020</Year><Month>Apr</Month><Day>03</Day></PubDate></JournalIssue><Title>ChemSusChem</Title><ISOAbbreviation>ChemSusChem</ISOAbbreviation></Journal><ArticleTitle>Mesoscale Reaction-Diffusion Phenomena Governing Lignin-First Biomass Fractionation.</ArticleTitle><ELocationID EIdType="doi" ValidYN="Y">10.1002/cssc.202000558</ELocationID><Abstract><AbstractText>Lignin solvolysis from the plant cell wall is the critical first step in lignin depolymerization processes involving whole biomass feedstocks. However, little is known about the coupled reaction kinetics and transport phenomena that govern the effective rates of lignin extraction. Here, we report a validated simulation framework that determines intrinsic, transport-independent kinetic parameters for the solvolysis of lignin, hemicellulose, and cellulose upon incorporation of feedstock characteristics for the methanol-based extraction of poplar as an example fractionation process. Lignin fragment diffusion is predicted to compete on the same time and length scales as reactions of lignin within cell walls and longitudinal pores of typical milled particle sizes, and mass transfer resistances are predicted to dominate the solvolysis of poplar particles that exceed approximately 2 mm in length. Beyond the approximately 2 mm threshold, effectiveness factors are predicted to be below 0.25, which implies that pore diffusion resistances may attenuate observable kinetic rate measurements by at least 75 % in such cases. Thus, researchers are recommended to conduct kinetic evaluations of lignin-first catalysts using biomass particles smaller than approximately 0.2 mm in length to avoid feedstock-specific mass transfer limitations in lignin conversion studies. Overall, this work highlights opportunities to improve lignin solvolysis by genetic engineering and provides actionable kinetic information to guide the design and scale-up of emerging biorefinery strategies.</AbstractText><CopyrightInformation>© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.</CopyrightInformation></Abstract><AuthorList CompleteYN="Y"><Author ValidYN="Y"><LastName>Thornburg</LastName><ForeName>Nicholas E</ForeName><Initials>NE</Initials><Identifier Source="ORCID">http://orcid.org/0000-0002-4680-2733</Identifier><AffiliationInfo><Affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Pecha</LastName><ForeName>M Brennan</ForeName><Initials>MB</Initials><Identifier Source="ORCID">http://orcid.org/0000-0002-0894-8504</Identifier><AffiliationInfo><Affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Brandner</LastName><ForeName>David G</ForeName><Initials>DG</Initials><Identifier Source="ORCID">http://orcid.org/0000-0003-4296-4855</Identifier><AffiliationInfo><Affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Reed</LastName><ForeName>Michelle L</ForeName><Initials>ML</Initials><AffiliationInfo><Affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Vermaas</LastName><ForeName>Josh V</ForeName><Initials>JV</Initials><Identifier Source="ORCID">http://orcid.org/0000-0003-3139-6469</Identifier><AffiliationInfo><Affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Michener</LastName><ForeName>William E</ForeName><Initials>WE</Initials><AffiliationInfo><Affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Katahira</LastName><ForeName>Rui</ForeName><Initials>R</Initials><AffiliationInfo><Affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Vinzant</LastName><ForeName>Todd B</ForeName><Initials>TB</Initials><AffiliationInfo><Affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Foust</LastName><ForeName>Thomas D</ForeName><Initials>TD</Initials><Identifier Source="ORCID">http://orcid.org/0000-0002-3995-8254</Identifier><AffiliationInfo><Affiliation>National Bioenergy Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Donohoe</LastName><ForeName>Bryon S</ForeName><Initials>BS</Initials><Identifier Source="ORCID">http://orcid.org/0000-0002-2272-5059</Identifier><AffiliationInfo><Affiliation>Biosciences Center, National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO, 80401, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Román-Leshkov</LastName><ForeName>Yuriy</ForeName><Initials>Y</Initials><Identifier Source="ORCID">http://orcid.org/0000-0002-0025-4233</Identifier><AffiliationInfo><Affiliation>Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Ciesielski</LastName><ForeName>Peter N</ForeName><Initials>PN</Initials><Identifier 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Ciesielski</name><name sortKey="Donohoe, Bryon S" sort="Donohoe, Bryon S" uniqKey="Donohoe B" first="Bryon S" last="Donohoe">Bryon S. Donohoe</name><name sortKey="Foust, Thomas D" sort="Foust, Thomas D" uniqKey="Foust T" first="Thomas D" last="Foust">Thomas D. Foust</name><name sortKey="Katahira, Rui" sort="Katahira, Rui" uniqKey="Katahira R" first="Rui" last="Katahira">Rui Katahira</name><name sortKey="Michener, William E" sort="Michener, William E" uniqKey="Michener W" first="William E" last="Michener">William E. Michener</name><name sortKey="Pecha, M Brennan" sort="Pecha, M Brennan" uniqKey="Pecha M" first="M Brennan" last="Pecha">M Brennan Pecha</name><name sortKey="Reed, Michelle L" sort="Reed, Michelle L" uniqKey="Reed M" first="Michelle L" last="Reed">Michelle L. Reed</name><name sortKey="Roman Leshkov, Yuriy" sort="Roman Leshkov, Yuriy" uniqKey="Roman Leshkov Y" first="Yuriy" last="Román-Leshkov">Yuriy Román-Leshkov</name><name sortKey="Vermaas, Josh V" sort="Vermaas, Josh V" uniqKey="Vermaas J" first="Josh V" last="Vermaas">Josh V. Vermaas</name><name sortKey="Vinzant, Todd B" sort="Vinzant, Todd B" uniqKey="Vinzant T" first="Todd B" last="Vinzant">Todd B. Vinzant</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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|wiki= Bois
|area= PoplarV1
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|texte= Mesoscale Reaction-Diffusion Phenomena Governing Lignin-First Biomass Fractionation.
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