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Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and SeNi5P4
The exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self‐supported three‐dimensional (3D) SeNi5P4 nanosheet electrocatalyst was r...
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Published in: | AIChE journal 2023-10, Vol.69 (10), p.n/a |
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creator | He, Jiahui Li, Suiqin Li, Chun Li, Kai Xu, Yinjie Wang, Mengxin Zhao, Shuying Zhang, Jiefeng Zhong, Xing Li, Xiaonian Zhang, Zhengbin Wang, Jianguo |
description | The exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self‐supported three‐dimensional (3D) SeNi5P4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous SeNi5P4/graphite felt (GF), an excellent performance of ≥98% selectivity and 33.12 kg (m−3 h−1) space–time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of SeNi5P4, and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6‐tetramethyl‐1‐piperidine N‐oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale‐up experiment was conducted with stacked‐flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications. |
doi_str_mv | 10.1002/aic.18153 |
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Herein, a self‐supported three‐dimensional (3D) SeNi5P4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous SeNi5P4/graphite felt (GF), an excellent performance of ≥98% selectivity and 33.12 kg (m−3 h−1) space–time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of SeNi5P4, and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6‐tetramethyl‐1‐piperidine N‐oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale‐up experiment was conducted with stacked‐flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications.</description><identifier>ISSN: 0001-1541</identifier><identifier>EISSN: 1547-5905</identifier><identifier>DOI: 10.1002/aic.18153</identifier><language>eng</language><publisher>Hoboken, USA: John Wiley & Sons, Inc</publisher><subject>aminoxyl radicals ; Chemical industry ; Contamination ; Continuous flow ; Electrocatalysts ; electrochemical alcohol oxidation ; Electrochemistry ; Electronic structure ; Fine chemicals ; Flow system ; Heavy metals ; Mass transfer ; Oxidation ; Phosphorus ; Piperidine ; process intensification ; Selenium ; stacked electrolyzer ; sterol ; Sterols ; Synergistic effect</subject><ispartof>AIChE journal, 2023-10, Vol.69 (10), p.n/a</ispartof><rights>2023 American Institute of Chemical Engineers.</rights><rights>2023 American Institute of Chemical Engineers</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0003-2391-4529</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>He, Jiahui</creatorcontrib><creatorcontrib>Li, Suiqin</creatorcontrib><creatorcontrib>Li, Chun</creatorcontrib><creatorcontrib>Li, Kai</creatorcontrib><creatorcontrib>Xu, Yinjie</creatorcontrib><creatorcontrib>Wang, Mengxin</creatorcontrib><creatorcontrib>Zhao, Shuying</creatorcontrib><creatorcontrib>Zhang, Jiefeng</creatorcontrib><creatorcontrib>Zhong, Xing</creatorcontrib><creatorcontrib>Li, Xiaonian</creatorcontrib><creatorcontrib>Zhang, Zhengbin</creatorcontrib><creatorcontrib>Wang, Jianguo</creatorcontrib><title>Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and SeNi5P4</title><title>AIChE journal</title><description>The exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self‐supported three‐dimensional (3D) SeNi5P4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous SeNi5P4/graphite felt (GF), an excellent performance of ≥98% selectivity and 33.12 kg (m−3 h−1) space–time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of SeNi5P4, and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6‐tetramethyl‐1‐piperidine N‐oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale‐up experiment was conducted with stacked‐flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications.</description><subject>aminoxyl radicals</subject><subject>Chemical industry</subject><subject>Contamination</subject><subject>Continuous flow</subject><subject>Electrocatalysts</subject><subject>electrochemical alcohol oxidation</subject><subject>Electrochemistry</subject><subject>Electronic structure</subject><subject>Fine chemicals</subject><subject>Flow system</subject><subject>Heavy metals</subject><subject>Mass transfer</subject><subject>Oxidation</subject><subject>Phosphorus</subject><subject>Piperidine</subject><subject>process intensification</subject><subject>Selenium</subject><subject>stacked electrolyzer</subject><subject>sterol</subject><subject>Sterols</subject><subject>Synergistic effect</subject><issn>0001-1541</issn><issn>1547-5905</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNotUNtOAjEQbYwmIvrgHzTxeaFXtvtIiAoJURP1uel2WyxZttgukX6PH-In-QsW8GlmzpxzJnMAuMVohBEiY-X0CAvM6RkYYM7KgleIn4MBQggXGcCX4CrGdZ5IKcgA-LlbfbQJGmuddqbroWmN7oPXqldt6p2Gfu8a1TvfQW9h7E3wLawTjKkzYeXigZLVWXTYq43r_D61MKjGadVGqLoGvprf758nx1_YNbiwGTU3_3UI3h_u32bzYvn8uJhNl8WWcEELbhUiNRV1JVR-q0bMaIMZsYg1uKpIhSYYKVsaW2NcasuJYbRGpNRU0YY0dAjuTr7b4D93JvZy7XehyyclERMuJqwkIrPGJ9aXa02S2-A2KiSJkTyEKXOY8himnC5mx4b-AROga0A</recordid><startdate>202310</startdate><enddate>202310</enddate><creator>He, Jiahui</creator><creator>Li, Suiqin</creator><creator>Li, Chun</creator><creator>Li, Kai</creator><creator>Xu, Yinjie</creator><creator>Wang, Mengxin</creator><creator>Zhao, Shuying</creator><creator>Zhang, Jiefeng</creator><creator>Zhong, Xing</creator><creator>Li, Xiaonian</creator><creator>Zhang, Zhengbin</creator><creator>Wang, Jianguo</creator><general>John Wiley & Sons, Inc</general><general>American Institute of Chemical Engineers</general><scope>7ST</scope><scope>7U5</scope><scope>8FD</scope><scope>C1K</scope><scope>L7M</scope><scope>SOI</scope><orcidid>https://orcid.org/0000-0003-2391-4529</orcidid></search><sort><creationdate>202310</creationdate><title>Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and SeNi5P4</title><author>He, Jiahui ; Li, Suiqin ; Li, Chun ; Li, Kai ; Xu, Yinjie ; Wang, Mengxin ; Zhao, Shuying ; Zhang, Jiefeng ; Zhong, Xing ; Li, Xiaonian ; Zhang, Zhengbin ; Wang, Jianguo</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p2583-5fa02b38b98a002b04ece142f04d199290610af7efb117cf52e43b027c3a3d2d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>aminoxyl radicals</topic><topic>Chemical industry</topic><topic>Contamination</topic><topic>Continuous flow</topic><topic>Electrocatalysts</topic><topic>electrochemical alcohol oxidation</topic><topic>Electrochemistry</topic><topic>Electronic structure</topic><topic>Fine chemicals</topic><topic>Flow system</topic><topic>Heavy metals</topic><topic>Mass transfer</topic><topic>Oxidation</topic><topic>Phosphorus</topic><topic>Piperidine</topic><topic>process intensification</topic><topic>Selenium</topic><topic>stacked electrolyzer</topic><topic>sterol</topic><topic>Sterols</topic><topic>Synergistic effect</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>He, Jiahui</creatorcontrib><creatorcontrib>Li, Suiqin</creatorcontrib><creatorcontrib>Li, Chun</creatorcontrib><creatorcontrib>Li, Kai</creatorcontrib><creatorcontrib>Xu, Yinjie</creatorcontrib><creatorcontrib>Wang, Mengxin</creatorcontrib><creatorcontrib>Zhao, Shuying</creatorcontrib><creatorcontrib>Zhang, Jiefeng</creatorcontrib><creatorcontrib>Zhong, Xing</creatorcontrib><creatorcontrib>Li, Xiaonian</creatorcontrib><creatorcontrib>Zhang, Zhengbin</creatorcontrib><creatorcontrib>Wang, Jianguo</creatorcontrib><collection>Environment Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>Environment Abstracts</collection><jtitle>AIChE journal</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>He, Jiahui</au><au>Li, Suiqin</au><au>Li, Chun</au><au>Li, Kai</au><au>Xu, Yinjie</au><au>Wang, Mengxin</au><au>Zhao, Shuying</au><au>Zhang, Jiefeng</au><au>Zhong, Xing</au><au>Li, Xiaonian</au><au>Zhang, Zhengbin</au><au>Wang, Jianguo</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and SeNi5P4</atitle><jtitle>AIChE journal</jtitle><date>2023-10</date><risdate>2023</risdate><volume>69</volume><issue>10</issue><epage>n/a</epage><issn>0001-1541</issn><eissn>1547-5905</eissn><abstract>The exploration of efficient and environmentally friendly oxidation method is highly desirable to overcome the critical problems of poor selectivity and heavy metal contamination for the fine chemicals industry. Herein, a self‐supported three‐dimensional (3D) SeNi5P4 nanosheet electrocatalyst was rationally designed and fabricated. Benefiting from the synergistic effect of aminoxyl radical and mesoporous SeNi5P4/graphite felt (GF), an excellent performance of ≥98% selectivity and 33.12 kg (m−3 h−1) space–time yield was obtained for sterol intermediate oxidation with the enhanced mass transfer effect of the continuous flow system. The doping of anionic selenium and phosphorus modulated the electronic structure of SeNi5P4, and the oxyhydroxides generated by surface reconstruction accelerated the turnover of 2,2,6,6‐tetramethyl‐1‐piperidine N‐oxyl (TEMPO), thereby enhancing the intrinsic electrocatalytic activity. A scale‐up experiment was conducted with stacked‐flow electrolyzer demonstrated the application potential. This work provided an efficient synergistic electrocatalytic strategy to facilitate rapid electron and mass transfer for electrochemical alcohol oxidation and highlighted the potential for practical electrosynthesis applications.</abstract><cop>Hoboken, USA</cop><pub>John Wiley & Sons, Inc</pub><doi>10.1002/aic.18153</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0003-2391-4529</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | aminoxyl radicals Chemical industry Contamination Continuous flow Electrocatalysts electrochemical alcohol oxidation Electrochemistry Electronic structure Fine chemicals Flow system Heavy metals Mass transfer Oxidation Phosphorus Piperidine process intensification Selenium stacked electrolyzer sterol Sterols Synergistic effect |
title | Highly efficient electrocatalytic oxidation of sterol by synergistic effect of aminoxyl radicals and SeNi5P4 |
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