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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...
Autores principales: | , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group
2017
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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. |
format | Online Article Text |
id | pubmed-5527281 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Nature Publishing Group |
record_format | MEDLINE/PubMed |
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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