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Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study

The conversion of biomass-derived glycerol into valuable products is an alternative strategy for alleviating energy scarcity and environmental issues. The authors recently uncovered an activated carbon composite electrode with an Amberlyst-15 mediator able to generate 1,2-propanediol, diethylene gly...

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Autores principales: Md. Rahim, Siti Aqilah Nadhirah, Lee, Ching Shya, Aroua, Mohamed Kheireddine, Wan Daud, Wan Mohd Ashri, Abnisa, Faisal, Cognet, Patrick, Pérès, Yolande
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Frontiers Media S.A. 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8914049/
https://www.ncbi.nlm.nih.gov/pubmed/35281562
http://dx.doi.org/10.3389/fchem.2022.845614
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author Md. Rahim, Siti Aqilah Nadhirah
Lee, Ching Shya
Aroua, Mohamed Kheireddine
Wan Daud, Wan Mohd Ashri
Abnisa, Faisal
Cognet, Patrick
Pérès, Yolande
author_facet Md. Rahim, Siti Aqilah Nadhirah
Lee, Ching Shya
Aroua, Mohamed Kheireddine
Wan Daud, Wan Mohd Ashri
Abnisa, Faisal
Cognet, Patrick
Pérès, Yolande
author_sort Md. Rahim, Siti Aqilah Nadhirah
collection PubMed
description The conversion of biomass-derived glycerol into valuable products is an alternative strategy for alleviating energy scarcity and environmental issues. The authors recently uncovered an activated carbon composite electrode with an Amberlyst-15 mediator able to generate 1,2-propanediol, diethylene glycol, and acetol via a glycerol electrocatalytic reduction. However, less attention to mechanistic insights makes its application to industrial processes challenging. Herein, two proposed intermediates, acetol and ethylene glycol, were employed as the feedstocks to fill the gap in the mechanistic understanding of the reactions. The results discovered the importance of acetol in producing 1,2-propanediol and concluded the glycerol electrocatalytic reduction process has a two-step reduction pathway, where glycerol was initially reduced to acetol and consecutively hydrogenated to 1,2-propanediol. At 353 K and 0.28 A/cm(2), 1,2-propanediol selectivity achieved 77% (with 59.8 C mol% yield) after 7 h of acetol (3.0 mol/L) electrolysis. Finally, the influences of the temperature, glycerol initial concentration, and current density on the glycerol electrocatalytic reduction were evaluated. The initial step involved the C-O and C-C bonds cleavage in glycerol plays a crucial role in producing either acetol or ethylene glycol intermediate. This was controlled by the temperature, which low to moderate value is needed to maintain a selective acetol-1,2-propanediol route. Additionally, medium glycerol initial concentration reduced the hydrogen formation and indirectly improved 1,2-propanediol yield. A mild current density raised the conversion rate and minimized the growth of intermediates. At 353 K and 0.21 A/cm(2), glycerol (3.0 mol/L) electrocatalytic reduction to 1,2-propanediol reached the maximum yield of 42.3 C mol%.
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spelling pubmed-89140492022-03-12 Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study Md. Rahim, Siti Aqilah Nadhirah Lee, Ching Shya Aroua, Mohamed Kheireddine Wan Daud, Wan Mohd Ashri Abnisa, Faisal Cognet, Patrick Pérès, Yolande Front Chem Chemistry The conversion of biomass-derived glycerol into valuable products is an alternative strategy for alleviating energy scarcity and environmental issues. The authors recently uncovered an activated carbon composite electrode with an Amberlyst-15 mediator able to generate 1,2-propanediol, diethylene glycol, and acetol via a glycerol electrocatalytic reduction. However, less attention to mechanistic insights makes its application to industrial processes challenging. Herein, two proposed intermediates, acetol and ethylene glycol, were employed as the feedstocks to fill the gap in the mechanistic understanding of the reactions. The results discovered the importance of acetol in producing 1,2-propanediol and concluded the glycerol electrocatalytic reduction process has a two-step reduction pathway, where glycerol was initially reduced to acetol and consecutively hydrogenated to 1,2-propanediol. At 353 K and 0.28 A/cm(2), 1,2-propanediol selectivity achieved 77% (with 59.8 C mol% yield) after 7 h of acetol (3.0 mol/L) electrolysis. Finally, the influences of the temperature, glycerol initial concentration, and current density on the glycerol electrocatalytic reduction were evaluated. The initial step involved the C-O and C-C bonds cleavage in glycerol plays a crucial role in producing either acetol or ethylene glycol intermediate. This was controlled by the temperature, which low to moderate value is needed to maintain a selective acetol-1,2-propanediol route. Additionally, medium glycerol initial concentration reduced the hydrogen formation and indirectly improved 1,2-propanediol yield. A mild current density raised the conversion rate and minimized the growth of intermediates. At 353 K and 0.21 A/cm(2), glycerol (3.0 mol/L) electrocatalytic reduction to 1,2-propanediol reached the maximum yield of 42.3 C mol%. Frontiers Media S.A. 2022-02-25 /pmc/articles/PMC8914049/ /pubmed/35281562 http://dx.doi.org/10.3389/fchem.2022.845614 Text en Copyright © 2022 Md. Rahim, Lee, Aroua, Wan Daud, Abnisa, Cognet and Pérès. https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.
spellingShingle Chemistry
Md. Rahim, Siti Aqilah Nadhirah
Lee, Ching Shya
Aroua, Mohamed Kheireddine
Wan Daud, Wan Mohd Ashri
Abnisa, Faisal
Cognet, Patrick
Pérès, Yolande
Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study
title Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study
title_full Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study
title_fullStr Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study
title_full_unstemmed Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study
title_short Glycerol Electrocatalytic Reduction Using an Activated Carbon Composite Electrode: Understanding the Reaction Mechanisms and an Optimization Study
title_sort glycerol electrocatalytic reduction using an activated carbon composite electrode: understanding the reaction mechanisms and an optimization study
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8914049/
https://www.ncbi.nlm.nih.gov/pubmed/35281562
http://dx.doi.org/10.3389/fchem.2022.845614
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