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Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock

[Image: see text] Converting abundant biomass-derived feedstocks into value-added platform chemicals has attracted increasing interest in biorefinery; however, the rigorous operating conditions that are required limit the commercialization of these processes. Nonthermal plasma-based electrification...

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Autores principales: Ma, Yichen, Conroy, Stuart, Shaw, Alexander, Alliati, Ignacio M., Sels, Bert F., Zhang, Xiaolei, Tu, Xin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10685411/
https://www.ncbi.nlm.nih.gov/pubmed/38034967
http://dx.doi.org/10.1021/jacsau.3c00468
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author Ma, Yichen
Conroy, Stuart
Shaw, Alexander
Alliati, Ignacio M.
Sels, Bert F.
Zhang, Xiaolei
Tu, Xin
author_facet Ma, Yichen
Conroy, Stuart
Shaw, Alexander
Alliati, Ignacio M.
Sels, Bert F.
Zhang, Xiaolei
Tu, Xin
author_sort Ma, Yichen
collection PubMed
description [Image: see text] Converting abundant biomass-derived feedstocks into value-added platform chemicals has attracted increasing interest in biorefinery; however, the rigorous operating conditions that are required limit the commercialization of these processes. Nonthermal plasma-based electrification using intermittent renewable energy is an emerging alternative for sustainable next-generation chemical synthesis under mild conditions. Here, we report a hydrogen-free tunable plasma process for the selective conversion of lignin-derived anisole into phenolics with a high selectivity of 86.9% and an anisole conversion of 45.6% at 150 °C. The selectivity to alkylated chemicals can be tuned through control of the plasma alkylation process by changing specific energy input. The combined experimental and computational results reveal that the plasma generated H and CH(3) radicals exhibit a “catalytic effect” that reduces the activation energy of the transalkylation reactions, enabling the selective anisole conversion at low temperatures. This work opens the way for the sustainable and selective production of phenolic chemicals from biomass-derived feedstocks under mild conditions.
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spelling pubmed-106854112023-11-30 Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock Ma, Yichen Conroy, Stuart Shaw, Alexander Alliati, Ignacio M. Sels, Bert F. Zhang, Xiaolei Tu, Xin JACS Au [Image: see text] Converting abundant biomass-derived feedstocks into value-added platform chemicals has attracted increasing interest in biorefinery; however, the rigorous operating conditions that are required limit the commercialization of these processes. Nonthermal plasma-based electrification using intermittent renewable energy is an emerging alternative for sustainable next-generation chemical synthesis under mild conditions. Here, we report a hydrogen-free tunable plasma process for the selective conversion of lignin-derived anisole into phenolics with a high selectivity of 86.9% and an anisole conversion of 45.6% at 150 °C. The selectivity to alkylated chemicals can be tuned through control of the plasma alkylation process by changing specific energy input. The combined experimental and computational results reveal that the plasma generated H and CH(3) radicals exhibit a “catalytic effect” that reduces the activation energy of the transalkylation reactions, enabling the selective anisole conversion at low temperatures. This work opens the way for the sustainable and selective production of phenolic chemicals from biomass-derived feedstocks under mild conditions. American Chemical Society 2023-11-06 /pmc/articles/PMC10685411/ /pubmed/38034967 http://dx.doi.org/10.1021/jacsau.3c00468 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Ma, Yichen
Conroy, Stuart
Shaw, Alexander
Alliati, Ignacio M.
Sels, Bert F.
Zhang, Xiaolei
Tu, Xin
Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock
title Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock
title_full Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock
title_fullStr Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock
title_full_unstemmed Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock
title_short Plasma-Enabled Selective Synthesis of Biobased Phenolics from Lignin-Derived Feedstock
title_sort plasma-enabled selective synthesis of biobased phenolics from lignin-derived feedstock
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10685411/
https://www.ncbi.nlm.nih.gov/pubmed/38034967
http://dx.doi.org/10.1021/jacsau.3c00468
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