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Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock

[Image: see text] The one-step ethanolysis approach to upgrade lignin to monomeric aromatics using a CuMgAl mixed oxide catalyst is studied in detail. The influence of reaction temperature (200–420 °C) on the product distribution is investigated. At low temperature (200–250 °C), recondensation is do...

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Autores principales: Huang, Xiaoming, Atay, Ceylanpinar, Zhu, Jiadong, Palstra, Sanne W. L., Korányi, Tamás I., Boot, Michael D., Hensen, Emiel J. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2017
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5678292/
https://www.ncbi.nlm.nih.gov/pubmed/29142789
http://dx.doi.org/10.1021/acssuschemeng.7b02790
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author Huang, Xiaoming
Atay, Ceylanpinar
Zhu, Jiadong
Palstra, Sanne W. L.
Korányi, Tamás I.
Boot, Michael D.
Hensen, Emiel J. M.
author_facet Huang, Xiaoming
Atay, Ceylanpinar
Zhu, Jiadong
Palstra, Sanne W. L.
Korányi, Tamás I.
Boot, Michael D.
Hensen, Emiel J. M.
author_sort Huang, Xiaoming
collection PubMed
description [Image: see text] The one-step ethanolysis approach to upgrade lignin to monomeric aromatics using a CuMgAl mixed oxide catalyst is studied in detail. The influence of reaction temperature (200–420 °C) on the product distribution is investigated. At low temperature (200–250 °C), recondensation is dominant, while char-forming reactions become significant at high reaction temperature (>380 °C). At preferred intermediate temperatures (300–340 °C), char-forming reactions are effectively suppressed by alkylation and Guerbet and esterification reactions. This shifts the reaction toward depolymerization, explaining high monomeric aromatics yield. Carbon-14 dating analysis of the lignin residue revealed that a substantial amount of the carbon in the lignin residue originates from reactions of lignin with ethanol. Recycling tests show that the activity of the regenerated catalyst was strongly decreased due to a loss of basic sites due to hydrolysis of the MgO function and a loss of surface area due to spinel oxide formation of the Cu and Al components. The utility of this one-step approach for upgrading woody biomass was also demonstrated. An important observation is that conversion of the native lignin contained in the lignocellulosic matrix is much easier than the conversion of technical lignin.
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spelling pubmed-56782922017-11-13 Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock Huang, Xiaoming Atay, Ceylanpinar Zhu, Jiadong Palstra, Sanne W. L. Korányi, Tamás I. Boot, Michael D. Hensen, Emiel J. M. ACS Sustain Chem Eng [Image: see text] The one-step ethanolysis approach to upgrade lignin to monomeric aromatics using a CuMgAl mixed oxide catalyst is studied in detail. The influence of reaction temperature (200–420 °C) on the product distribution is investigated. At low temperature (200–250 °C), recondensation is dominant, while char-forming reactions become significant at high reaction temperature (>380 °C). At preferred intermediate temperatures (300–340 °C), char-forming reactions are effectively suppressed by alkylation and Guerbet and esterification reactions. This shifts the reaction toward depolymerization, explaining high monomeric aromatics yield. Carbon-14 dating analysis of the lignin residue revealed that a substantial amount of the carbon in the lignin residue originates from reactions of lignin with ethanol. Recycling tests show that the activity of the regenerated catalyst was strongly decreased due to a loss of basic sites due to hydrolysis of the MgO function and a loss of surface area due to spinel oxide formation of the Cu and Al components. The utility of this one-step approach for upgrading woody biomass was also demonstrated. An important observation is that conversion of the native lignin contained in the lignocellulosic matrix is much easier than the conversion of technical lignin. American Chemical Society 2017-10-09 2017-11-06 /pmc/articles/PMC5678292/ /pubmed/29142789 http://dx.doi.org/10.1021/acssuschemeng.7b02790 Text en Copyright © 2017 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Huang, Xiaoming
Atay, Ceylanpinar
Zhu, Jiadong
Palstra, Sanne W. L.
Korányi, Tamás I.
Boot, Michael D.
Hensen, Emiel J. M.
Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock
title Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock
title_full Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock
title_fullStr Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock
title_full_unstemmed Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock
title_short Catalytic Depolymerization of Lignin and Woody Biomass in Supercritical Ethanol: Influence of Reaction Temperature and Feedstock
title_sort catalytic depolymerization of lignin and woody biomass in supercritical ethanol: influence of reaction temperature and feedstock
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5678292/
https://www.ncbi.nlm.nih.gov/pubmed/29142789
http://dx.doi.org/10.1021/acssuschemeng.7b02790
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