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Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy

Adipic acid is an important building block of polymers, and is commercially produced by thermo-catalytic oxidation of ketone-alcohol oil (a mixture of cyclohexanol and cyclohexanone). However, this process heavily relies on the use of corrosive nitric acid while releases nitrous oxide as a potent gr...

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Autores principales: Li, Zhenhua, Li, Xiaofan, Zhou, Hua, Xu, Yan, Xu, Si-Min, Ren, Yue, Yan, Yifan, Yang, Jiangrong, Ji, Kaiyue, Li, Li, Xu, Ming, Shao, Mingfei, Kong, Xianggui, Sun, Xiaoming, Duan, Haohong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9411531/
https://www.ncbi.nlm.nih.gov/pubmed/36008416
http://dx.doi.org/10.1038/s41467-022-32769-0
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author Li, Zhenhua
Li, Xiaofan
Zhou, Hua
Xu, Yan
Xu, Si-Min
Ren, Yue
Yan, Yifan
Yang, Jiangrong
Ji, Kaiyue
Li, Li
Xu, Ming
Shao, Mingfei
Kong, Xianggui
Sun, Xiaoming
Duan, Haohong
author_facet Li, Zhenhua
Li, Xiaofan
Zhou, Hua
Xu, Yan
Xu, Si-Min
Ren, Yue
Yan, Yifan
Yang, Jiangrong
Ji, Kaiyue
Li, Li
Xu, Ming
Shao, Mingfei
Kong, Xianggui
Sun, Xiaoming
Duan, Haohong
author_sort Li, Zhenhua
collection PubMed
description Adipic acid is an important building block of polymers, and is commercially produced by thermo-catalytic oxidation of ketone-alcohol oil (a mixture of cyclohexanol and cyclohexanone). However, this process heavily relies on the use of corrosive nitric acid while releases nitrous oxide as a potent greenhouse gas. Herein, we report an electrocatalytic strategy for the oxidation of cyclohexanone to adipic acid coupled with H(2) production over a nickel hydroxide (Ni(OH)(2)) catalyst modified with sodium dodecyl sulfonate (SDS). The intercalated SDS facilitates the enrichment of immiscible cyclohexanone in aqueous medium, thus achieving 3.6-fold greater productivity of adipic acid and higher faradaic efficiency (FE) compared with pure Ni(OH)(2) (93% versus 56%). This strategy is demonstrated effective for a variety of immiscible aldehydes and ketones in aqueous solution. Furthermore, we design a realistic two-electrode flow electrolyzer for electrooxidation of cyclohexanone coupling with H(2) production, attaining adipic acid productivity of 4.7 mmol coupled with H(2) productivity of 8.0 L at 0.8 A (corresponding to 30 mA cm(−2)) in 24 h.
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spelling pubmed-94115312022-08-27 Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy Li, Zhenhua Li, Xiaofan Zhou, Hua Xu, Yan Xu, Si-Min Ren, Yue Yan, Yifan Yang, Jiangrong Ji, Kaiyue Li, Li Xu, Ming Shao, Mingfei Kong, Xianggui Sun, Xiaoming Duan, Haohong Nat Commun Article Adipic acid is an important building block of polymers, and is commercially produced by thermo-catalytic oxidation of ketone-alcohol oil (a mixture of cyclohexanol and cyclohexanone). However, this process heavily relies on the use of corrosive nitric acid while releases nitrous oxide as a potent greenhouse gas. Herein, we report an electrocatalytic strategy for the oxidation of cyclohexanone to adipic acid coupled with H(2) production over a nickel hydroxide (Ni(OH)(2)) catalyst modified with sodium dodecyl sulfonate (SDS). The intercalated SDS facilitates the enrichment of immiscible cyclohexanone in aqueous medium, thus achieving 3.6-fold greater productivity of adipic acid and higher faradaic efficiency (FE) compared with pure Ni(OH)(2) (93% versus 56%). This strategy is demonstrated effective for a variety of immiscible aldehydes and ketones in aqueous solution. Furthermore, we design a realistic two-electrode flow electrolyzer for electrooxidation of cyclohexanone coupling with H(2) production, attaining adipic acid productivity of 4.7 mmol coupled with H(2) productivity of 8.0 L at 0.8 A (corresponding to 30 mA cm(−2)) in 24 h. Nature Publishing Group UK 2022-08-25 /pmc/articles/PMC9411531/ /pubmed/36008416 http://dx.doi.org/10.1038/s41467-022-32769-0 Text en © The Author(s) 2022 https://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/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Li, Zhenhua
Li, Xiaofan
Zhou, Hua
Xu, Yan
Xu, Si-Min
Ren, Yue
Yan, Yifan
Yang, Jiangrong
Ji, Kaiyue
Li, Li
Xu, Ming
Shao, Mingfei
Kong, Xianggui
Sun, Xiaoming
Duan, Haohong
Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy
title Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy
title_full Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy
title_fullStr Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy
title_full_unstemmed Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy
title_short Electrocatalytic synthesis of adipic acid coupled with H(2) production enhanced by a ligand modification strategy
title_sort electrocatalytic synthesis of adipic acid coupled with h(2) production enhanced by a ligand modification strategy
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9411531/
https://www.ncbi.nlm.nih.gov/pubmed/36008416
http://dx.doi.org/10.1038/s41467-022-32769-0
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