Thermodynamically stable synthesis of high entropy alloys and efficiently catalyzed oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under base-free conditions
The high activity and high selectivity in the catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) under non-alkaline conditions has always been a significant challenge in the field of biomass utilization. In this work, a thermodynamically stabilized high-entro...
Gespeichert in:
Veröffentlicht in: | Green chemistry : an international journal and green chemistry resource : GC 2024-11, Vol.26 (22), p.11316-11327 |
---|---|
Hauptverfasser: | , , , , , , , , , |
Format: | Artikel |
Sprache: | eng |
Schlagworte: | |
Online-Zugang: | Volltext |
Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
container_end_page | 11327 |
---|---|
container_issue | 22 |
container_start_page | 11316 |
container_title | Green chemistry : an international journal and green chemistry resource : GC |
container_volume | 26 |
creator | Lv, Guangqiang Liu, Shan Chen, Xiaoyan Chen, Mengxin Wu, Yanjuan Gao, Yuji Wang, Shuai Tao, Furong Wang, Jingui Niu, Liwei |
description | The high activity and high selectivity in the catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) under non-alkaline conditions has always been a significant challenge in the field of biomass utilization. In this work, a thermodynamically stabilized high-entropy alloy (HEA) structure with relatively low Pt content was synthesized
via
a simple impregnation-calcination procedure by tuning the mixing enthalpy and the Gibbs free energy of the metal-mixing system. The prepared HEA shows excellent catalytic performance in the aerobic oxidation of HMF into FDCA under base-free conditions. Experiments and DFT calculations revealed that molecular O
2
can be easily activated into highly oxidative hydroxyl radicals (&z.rad;OH) in the presence of water over the HEA surface, and facilitates the oxidation of HMF to FDCA under base-free conditions. This work provides a valuable reference for similar aerobic oxidation processes in which alkaline promoters and noble metal catalysts are needed.
In a completely non-alkaline aqueous system, a high-entropy alloy catalyst composed of FeCoNiCuGaPt activates O
2
and H
2
O molecules to form hydroxyl radicals (&z.rad;OH) and efficiently oxidizes 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid. |
doi_str_mv | 10.1039/d4gc04186k |
format | Article |
fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_crossref_primary_10_1039_D4GC04186K</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>3126673862</sourcerecordid><originalsourceid>FETCH-LOGICAL-c170t-7473c05952484b05afd1245411f7b77b0b8539a834459f7b81f212b76e0afd903</originalsourceid><addsrcrecordid>eNpF0ctKxDAUBuAiCo6XjXsh4E6s5tamXcqooyi40XVJc7EZO8mYZGDia_mCZhxRCOT2nXMWf1GcIHiJIGmvJH0TkKKmft8pJojWpGwxg7t_5xrvFwchzCFEiNV0Uny9DMovnEyWL4zg45hAiLwfFQjJxkEFE4DTYDBvA1A2erdMICuXAuBWAqW1ESZ_5DrBIx_Tp5LArY3k0Ti7Ka3KIUnv1mmh4pBGvfJ58REYGx3AF1W5uVqZh_s-q9EIwIWRYGWl8qDnQZXaKwWEy2jTNBwVe5qPQR3_7ofF693ty_S-fHqePUyvn0qBGIwlo4wIWLUVpg3tYcW1RJhWFCHNesZ62DcVaXlDKK3a_NQgjRHuWa1gpi0kh8XZtu_Su4-VCrGbu5W3eWRHEK5rRpoaZ3W-VcK7ELzS3dKbBfepQ7DbhNLd0Nn0J5THjE-32Afx5_5DI99Ej41c</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>3126673862</pqid></control><display><type>article</type><title>Thermodynamically stable synthesis of high entropy alloys and efficiently catalyzed oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under base-free conditions</title><source>Royal Society Of Chemistry Journals</source><source>Alma/SFX Local Collection</source><creator>Lv, Guangqiang ; Liu, Shan ; Chen, Xiaoyan ; Chen, Mengxin ; Wu, Yanjuan ; Gao, Yuji ; Wang, Shuai ; Tao, Furong ; Wang, Jingui ; Niu, Liwei</creator><creatorcontrib>Lv, Guangqiang ; Liu, Shan ; Chen, Xiaoyan ; Chen, Mengxin ; Wu, Yanjuan ; Gao, Yuji ; Wang, Shuai ; Tao, Furong ; Wang, Jingui ; Niu, Liwei</creatorcontrib><description>The high activity and high selectivity in the catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) under non-alkaline conditions has always been a significant challenge in the field of biomass utilization. In this work, a thermodynamically stabilized high-entropy alloy (HEA) structure with relatively low Pt content was synthesized
via
a simple impregnation-calcination procedure by tuning the mixing enthalpy and the Gibbs free energy of the metal-mixing system. The prepared HEA shows excellent catalytic performance in the aerobic oxidation of HMF into FDCA under base-free conditions. Experiments and DFT calculations revealed that molecular O
2
can be easily activated into highly oxidative hydroxyl radicals (&z.rad;OH) in the presence of water over the HEA surface, and facilitates the oxidation of HMF to FDCA under base-free conditions. This work provides a valuable reference for similar aerobic oxidation processes in which alkaline promoters and noble metal catalysts are needed.
In a completely non-alkaline aqueous system, a high-entropy alloy catalyst composed of FeCoNiCuGaPt activates O
2
and H
2
O molecules to form hydroxyl radicals (&z.rad;OH) and efficiently oxidizes 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid.</description><identifier>ISSN: 1463-9262</identifier><identifier>EISSN: 1463-9270</identifier><identifier>DOI: 10.1039/d4gc04186k</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Chemical synthesis ; Enthalpy ; Free energy ; Free radicals ; Gibbs free energy ; High entropy alloys ; Hydroxyl radicals ; Hydroxymethylfurfural ; Molecular structure ; Noble metals ; Oxidation</subject><ispartof>Green chemistry : an international journal and green chemistry resource : GC, 2024-11, Vol.26 (22), p.11316-11327</ispartof><rights>Copyright Royal Society of Chemistry 2024</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c170t-7473c05952484b05afd1245411f7b77b0b8539a834459f7b81f212b76e0afd903</cites><orcidid>0000-0003-3531-0415 ; 0000-0002-1288-3408 ; 0000-0001-9947-9821 ; 0000-0003-1610-4966</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>Lv, Guangqiang</creatorcontrib><creatorcontrib>Liu, Shan</creatorcontrib><creatorcontrib>Chen, Xiaoyan</creatorcontrib><creatorcontrib>Chen, Mengxin</creatorcontrib><creatorcontrib>Wu, Yanjuan</creatorcontrib><creatorcontrib>Gao, Yuji</creatorcontrib><creatorcontrib>Wang, Shuai</creatorcontrib><creatorcontrib>Tao, Furong</creatorcontrib><creatorcontrib>Wang, Jingui</creatorcontrib><creatorcontrib>Niu, Liwei</creatorcontrib><title>Thermodynamically stable synthesis of high entropy alloys and efficiently catalyzed oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under base-free conditions</title><title>Green chemistry : an international journal and green chemistry resource : GC</title><description>The high activity and high selectivity in the catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) under non-alkaline conditions has always been a significant challenge in the field of biomass utilization. In this work, a thermodynamically stabilized high-entropy alloy (HEA) structure with relatively low Pt content was synthesized
via
a simple impregnation-calcination procedure by tuning the mixing enthalpy and the Gibbs free energy of the metal-mixing system. The prepared HEA shows excellent catalytic performance in the aerobic oxidation of HMF into FDCA under base-free conditions. Experiments and DFT calculations revealed that molecular O
2
can be easily activated into highly oxidative hydroxyl radicals (&z.rad;OH) in the presence of water over the HEA surface, and facilitates the oxidation of HMF to FDCA under base-free conditions. This work provides a valuable reference for similar aerobic oxidation processes in which alkaline promoters and noble metal catalysts are needed.
In a completely non-alkaline aqueous system, a high-entropy alloy catalyst composed of FeCoNiCuGaPt activates O
2
and H
2
O molecules to form hydroxyl radicals (&z.rad;OH) and efficiently oxidizes 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid.</description><subject>Chemical synthesis</subject><subject>Enthalpy</subject><subject>Free energy</subject><subject>Free radicals</subject><subject>Gibbs free energy</subject><subject>High entropy alloys</subject><subject>Hydroxyl radicals</subject><subject>Hydroxymethylfurfural</subject><subject>Molecular structure</subject><subject>Noble metals</subject><subject>Oxidation</subject><issn>1463-9262</issn><issn>1463-9270</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNpF0ctKxDAUBuAiCo6XjXsh4E6s5tamXcqooyi40XVJc7EZO8mYZGDia_mCZhxRCOT2nXMWf1GcIHiJIGmvJH0TkKKmft8pJojWpGwxg7t_5xrvFwchzCFEiNV0Uny9DMovnEyWL4zg45hAiLwfFQjJxkEFE4DTYDBvA1A2erdMICuXAuBWAqW1ESZ_5DrBIx_Tp5LArY3k0Ti7Ka3KIUnv1mmh4pBGvfJ58REYGx3AF1W5uVqZh_s-q9EIwIWRYGWl8qDnQZXaKwWEy2jTNBwVe5qPQR3_7ofF693ty_S-fHqePUyvn0qBGIwlo4wIWLUVpg3tYcW1RJhWFCHNesZ62DcVaXlDKK3a_NQgjRHuWa1gpi0kh8XZtu_Su4-VCrGbu5W3eWRHEK5rRpoaZ3W-VcK7ELzS3dKbBfepQ7DbhNLd0Nn0J5THjE-32Afx5_5DI99Ej41c</recordid><startdate>20241111</startdate><enddate>20241111</enddate><creator>Lv, Guangqiang</creator><creator>Liu, Shan</creator><creator>Chen, Xiaoyan</creator><creator>Chen, Mengxin</creator><creator>Wu, Yanjuan</creator><creator>Gao, Yuji</creator><creator>Wang, Shuai</creator><creator>Tao, Furong</creator><creator>Wang, Jingui</creator><creator>Niu, Liwei</creator><general>Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7ST</scope><scope>7U6</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>JG9</scope><orcidid>https://orcid.org/0000-0003-3531-0415</orcidid><orcidid>https://orcid.org/0000-0002-1288-3408</orcidid><orcidid>https://orcid.org/0000-0001-9947-9821</orcidid><orcidid>https://orcid.org/0000-0003-1610-4966</orcidid></search><sort><creationdate>20241111</creationdate><title>Thermodynamically stable synthesis of high entropy alloys and efficiently catalyzed oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under base-free conditions</title><author>Lv, Guangqiang ; Liu, Shan ; Chen, Xiaoyan ; Chen, Mengxin ; Wu, Yanjuan ; Gao, Yuji ; Wang, Shuai ; Tao, Furong ; Wang, Jingui ; Niu, Liwei</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c170t-7473c05952484b05afd1245411f7b77b0b8539a834459f7b81f212b76e0afd903</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Chemical synthesis</topic><topic>Enthalpy</topic><topic>Free energy</topic><topic>Free radicals</topic><topic>Gibbs free energy</topic><topic>High entropy alloys</topic><topic>Hydroxyl radicals</topic><topic>Hydroxymethylfurfural</topic><topic>Molecular structure</topic><topic>Noble metals</topic><topic>Oxidation</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Lv, Guangqiang</creatorcontrib><creatorcontrib>Liu, Shan</creatorcontrib><creatorcontrib>Chen, Xiaoyan</creatorcontrib><creatorcontrib>Chen, Mengxin</creatorcontrib><creatorcontrib>Wu, Yanjuan</creatorcontrib><creatorcontrib>Gao, Yuji</creatorcontrib><creatorcontrib>Wang, Shuai</creatorcontrib><creatorcontrib>Tao, Furong</creatorcontrib><creatorcontrib>Wang, Jingui</creatorcontrib><creatorcontrib>Niu, Liwei</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Sustainability Science Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Materials Research Database</collection><jtitle>Green chemistry : an international journal and green chemistry resource : GC</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Lv, Guangqiang</au><au>Liu, Shan</au><au>Chen, Xiaoyan</au><au>Chen, Mengxin</au><au>Wu, Yanjuan</au><au>Gao, Yuji</au><au>Wang, Shuai</au><au>Tao, Furong</au><au>Wang, Jingui</au><au>Niu, Liwei</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Thermodynamically stable synthesis of high entropy alloys and efficiently catalyzed oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under base-free conditions</atitle><jtitle>Green chemistry : an international journal and green chemistry resource : GC</jtitle><date>2024-11-11</date><risdate>2024</risdate><volume>26</volume><issue>22</issue><spage>11316</spage><epage>11327</epage><pages>11316-11327</pages><issn>1463-9262</issn><eissn>1463-9270</eissn><abstract>The high activity and high selectivity in the catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) under non-alkaline conditions has always been a significant challenge in the field of biomass utilization. In this work, a thermodynamically stabilized high-entropy alloy (HEA) structure with relatively low Pt content was synthesized
via
a simple impregnation-calcination procedure by tuning the mixing enthalpy and the Gibbs free energy of the metal-mixing system. The prepared HEA shows excellent catalytic performance in the aerobic oxidation of HMF into FDCA under base-free conditions. Experiments and DFT calculations revealed that molecular O
2
can be easily activated into highly oxidative hydroxyl radicals (&z.rad;OH) in the presence of water over the HEA surface, and facilitates the oxidation of HMF to FDCA under base-free conditions. This work provides a valuable reference for similar aerobic oxidation processes in which alkaline promoters and noble metal catalysts are needed.
In a completely non-alkaline aqueous system, a high-entropy alloy catalyst composed of FeCoNiCuGaPt activates O
2
and H
2
O molecules to form hydroxyl radicals (&z.rad;OH) and efficiently oxidizes 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d4gc04186k</doi><tpages>12</tpages><orcidid>https://orcid.org/0000-0003-3531-0415</orcidid><orcidid>https://orcid.org/0000-0002-1288-3408</orcidid><orcidid>https://orcid.org/0000-0001-9947-9821</orcidid><orcidid>https://orcid.org/0000-0003-1610-4966</orcidid></addata></record> |
fulltext | fulltext |
identifier | ISSN: 1463-9262 |
ispartof | Green chemistry : an international journal and green chemistry resource : GC, 2024-11, Vol.26 (22), p.11316-11327 |
issn | 1463-9262 1463-9270 |
language | eng |
recordid | cdi_crossref_primary_10_1039_D4GC04186K |
source | Royal Society Of Chemistry Journals; Alma/SFX Local Collection |
subjects | Chemical synthesis Enthalpy Free energy Free radicals Gibbs free energy High entropy alloys Hydroxyl radicals Hydroxymethylfurfural Molecular structure Noble metals Oxidation |
title | Thermodynamically stable synthesis of high entropy alloys and efficiently catalyzed oxidation of 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid under base-free conditions |
url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-26T03%3A40%3A55IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Thermodynamically%20stable%20synthesis%20of%20high%20entropy%20alloys%20and%20efficiently%20catalyzed%20oxidation%20of%205-hydroxymethylfurfural%20into%202,5-furandicarboxylic%20acid%20under%20base-free%20conditions&rft.jtitle=Green%20chemistry%20:%20an%20international%20journal%20and%20green%20chemistry%20resource%20:%20GC&rft.au=Lv,%20Guangqiang&rft.date=2024-11-11&rft.volume=26&rft.issue=22&rft.spage=11316&rft.epage=11327&rft.pages=11316-11327&rft.issn=1463-9262&rft.eissn=1463-9270&rft_id=info:doi/10.1039/d4gc04186k&rft_dat=%3Cproquest_cross%3E3126673862%3C/proquest_cross%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=3126673862&rft_id=info:pmid/&rfr_iscdi=true |