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Selective production of arenes via direct lignin upgrading over a niobium-based catalyst

Lignin is the only large-volume renewable source of aromatic chemicals. Efficient depolymerization and deoxygenation of lignin while retaining the aromatic functionality are attractive but extremely challenging. Here we report the selective production of arenes via direct hydrodeoxygenation of organ...

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Autores principales: Shao, Yi, Xia, Qineng, Dong, Lin, Liu, Xiaohui, Han, Xue, Parker, Stewart F., Cheng, Yongqiang, Daemen, Luke L., Ramirez-Cuesta, Anibal J., Yang, Sihai, Wang, Yanqin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5527281/
https://www.ncbi.nlm.nih.gov/pubmed/28737172
http://dx.doi.org/10.1038/ncomms16104
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author Shao, Yi
Xia, Qineng
Dong, Lin
Liu, Xiaohui
Han, Xue
Parker, Stewart F.
Cheng, Yongqiang
Daemen, Luke L.
Ramirez-Cuesta, Anibal J.
Yang, Sihai
Wang, Yanqin
author_facet Shao, Yi
Xia, Qineng
Dong, Lin
Liu, Xiaohui
Han, Xue
Parker, Stewart F.
Cheng, Yongqiang
Daemen, Luke L.
Ramirez-Cuesta, Anibal J.
Yang, Sihai
Wang, Yanqin
author_sort Shao, Yi
collection PubMed
description Lignin is the only large-volume renewable source of aromatic chemicals. Efficient depolymerization and deoxygenation of lignin while retaining the aromatic functionality are attractive but extremely challenging. Here we report the selective production of arenes via direct hydrodeoxygenation of organosolv lignin over a porous Ru/Nb(2)O(5) catalyst that enabled the complete removal of the oxygen content from lignin. The conversion of birch lignin to monomer C(7)–C(9) hydrocarbons is nearly quantitative based on its monomer content, with a total mass yield of 35.5 wt% and an exceptional arene selectivity of 71 wt%. Inelastic neutron scattering and DFT calculations confirm that the Nb(2)O(5) support is catalytically unique compared with other traditional oxide supports, and the disassociation energy of C(aromatic)–OH bonds in phenolics is significantly reduced upon adsorption on Nb(2)O(5), resulting in its distinct selectivity to arenes. This one-pot process provides a promising approach for improved lignin valorization with general applicability.
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spelling pubmed-55272812017-07-31 Selective production of arenes via direct lignin upgrading over a niobium-based catalyst Shao, Yi Xia, Qineng Dong, Lin Liu, Xiaohui Han, Xue Parker, Stewart F. Cheng, Yongqiang Daemen, Luke L. Ramirez-Cuesta, Anibal J. Yang, Sihai Wang, Yanqin Nat Commun Article Lignin is the only large-volume renewable source of aromatic chemicals. Efficient depolymerization and deoxygenation of lignin while retaining the aromatic functionality are attractive but extremely challenging. Here we report the selective production of arenes via direct hydrodeoxygenation of organosolv lignin over a porous Ru/Nb(2)O(5) catalyst that enabled the complete removal of the oxygen content from lignin. The conversion of birch lignin to monomer C(7)–C(9) hydrocarbons is nearly quantitative based on its monomer content, with a total mass yield of 35.5 wt% and an exceptional arene selectivity of 71 wt%. Inelastic neutron scattering and DFT calculations confirm that the Nb(2)O(5) support is catalytically unique compared with other traditional oxide supports, and the disassociation energy of C(aromatic)–OH bonds in phenolics is significantly reduced upon adsorption on Nb(2)O(5), resulting in its distinct selectivity to arenes. This one-pot process provides a promising approach for improved lignin valorization with general applicability. Nature Publishing Group 2017-07-24 /pmc/articles/PMC5527281/ /pubmed/28737172 http://dx.doi.org/10.1038/ncomms16104 Text en Copyright © 2017, The Author(s) http://creativecommons.org/licenses/by/4.0/ Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Shao, Yi
Xia, Qineng
Dong, Lin
Liu, Xiaohui
Han, Xue
Parker, Stewart F.
Cheng, Yongqiang
Daemen, Luke L.
Ramirez-Cuesta, Anibal J.
Yang, Sihai
Wang, Yanqin
Selective production of arenes via direct lignin upgrading over a niobium-based catalyst
title Selective production of arenes via direct lignin upgrading over a niobium-based catalyst
title_full Selective production of arenes via direct lignin upgrading over a niobium-based catalyst
title_fullStr Selective production of arenes via direct lignin upgrading over a niobium-based catalyst
title_full_unstemmed Selective production of arenes via direct lignin upgrading over a niobium-based catalyst
title_short Selective production of arenes via direct lignin upgrading over a niobium-based catalyst
title_sort selective production of arenes via direct lignin upgrading over a niobium-based catalyst
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5527281/
https://www.ncbi.nlm.nih.gov/pubmed/28737172
http://dx.doi.org/10.1038/ncomms16104
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