Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries

An AB2X4 spinel structure, with tetrahedral A and octahedral B sites, is a paradigmatic class of catalysts with several possible geometric configurations and numerous applications, including polysulfide conversion in metal-sulfur batteries. Nonetheless, the influence of the geometric configuration a...

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Autores: Zhang, Chao Yue, Lu, Xuan|||0000-0003-2453-2805, Han, Xu|||0000-0001-8319-8830, Yu, Jing|||0000-0002-7620-745X, Zhang, Chaoqi|||0000-0002-0357-235X, Huang, Chen, Balcells i Argemí, Lluís|||0000-0001-6603-7357, Garzón Manjón, Alba|||0000-0003-2954-1102, Jacas Biendicho, Jordi|||0000-0001-5981-6168, Li, Junshan|||0000-0002-1482-1972, Arbiol i Cobos, Jordi|||0000-0002-0695-1726, Sun, Gengzhi|||0000-0002-8000-8912, Zhou, Jin Yuan, Cabot i Codina, Andreu|||0000-0002-7533-3251
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:302220
Acceso en línea:https://ddd.uab.cat/record/302220
https://dx.doi.org/urn:doi:10.1021/jacs.3c06288
Access Level:acceso abierto
Palabra clave:Active site
Cationics
Electrochemical activation
Geometric configurations
Large parts
Polysulphides
Sodium-sulfur batteries
Spinel catalyst
Spinel structure
]+ catalyst
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spelling Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur BatteriesZhang, Chao YueLu, Xuan|||0000-0003-2453-2805Han, Xu|||0000-0001-8319-8830Yu, Jing|||0000-0002-7620-745XZhang, Chaoqi|||0000-0002-0357-235XHuang, ChenBalcells i Argemí, Lluís|||0000-0001-6603-7357Garzón Manjón, Alba|||0000-0003-2954-1102Jacas Biendicho, Jordi|||0000-0001-5981-6168Li, Junshan|||0000-0002-1482-1972Arbiol i Cobos, Jordi|||0000-0002-0695-1726Sun, Gengzhi|||0000-0002-8000-8912Zhou, Jin YuanCabot i Codina, Andreu|||0000-0002-7533-3251Active siteCationicsElectrochemical activationGeometric configurationsLarge partsPolysulphidesSodium-sulfur batteriesSpinel catalystSpinel structure]+ catalystAn AB2X4 spinel structure, with tetrahedral A and octahedral B sites, is a paradigmatic class of catalysts with several possible geometric configurations and numerous applications, including polysulfide conversion in metal-sulfur batteries. Nonetheless, the influence of the geometric configuration and composition on the mechanisms of catalysis and the precise manner in which spinel catalysts facilitate the conversion of polysulfides remain unknown. To enable controlled exposure of single active configurations, herein, Cotd2+ and Cooh3+ in Co3O4 catalysts for sodium polysulfide conversion are in large part replaced by Fetd2+ and Feoh3+, respectively, generating FeCo2O4 and CoFe2O4. Through an examination of electrochemical activation energies, the characterization of symmetric cells, and theoretical calculations, we determine that Cooh3+ serves as the active site for the breaking of S-S bonds, while Cotd2+ functions as the active site for the formation of S-Na bonds. The current study underlines the subtle relationship between activity and geometric configurations of spinel catalysts, providing unique insights for the rational development of improved catalysts by optimizing their atomic geometric configuration. 22023-01-0120232023-01-01Articlehttp://purl.org/coar/resource_type/c_6501SMURhttp://purl.org/coar/version/c_71e4c1898caa6e32info:eu-repo/semantics/articleapplication/pdfhttps://ddd.uab.cat/record/302220https://dx.doi.org/urn:doi:10.1021/jacs.3c06288reponame:Dipòsit Digital de Documents de la UABinstname:Universitat Autònoma de BarcelonaInglésengAgència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2021/SGR-00457Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 CEX2021-001214-SAgencia Estatal de Investigación https://doi.org/10.13039/501100011033 RYC2021-033479-IAgencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2021-128410OB-I00open accesshttp://purl.org/coar/access_right/c_abf2Aquest material està protegit per drets d'autor i/o drets afins. Podeu utilitzar aquest material en funció del que permet la legislació de drets d'autor i drets afins d'aplicació al vostre cas. Per a d'altres usos heu d'obtenir permís del(s) titular(s) de drets.https://rightsstatements.org/vocab/InC/1.0/info:eu-repo/semantics/openAccessoai:ddd.uab.cat:3022202026-06-06T12:50:31Z
dc.title.none.fl_str_mv Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
title Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
spellingShingle Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
Zhang, Chao Yue
Active site
Cationics
Electrochemical activation
Geometric configurations
Large parts
Polysulphides
Sodium-sulfur batteries
Spinel catalyst
Spinel structure
]+ catalyst
title_short Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
title_full Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
title_fullStr Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
title_full_unstemmed Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
title_sort Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
dc.creator.none.fl_str_mv Zhang, Chao Yue
Lu, Xuan|||0000-0003-2453-2805
Han, Xu|||0000-0001-8319-8830
Yu, Jing|||0000-0002-7620-745X
Zhang, Chaoqi|||0000-0002-0357-235X
Huang, Chen
Balcells i Argemí, Lluís|||0000-0001-6603-7357
Garzón Manjón, Alba|||0000-0003-2954-1102
Jacas Biendicho, Jordi|||0000-0001-5981-6168
Li, Junshan|||0000-0002-1482-1972
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Sun, Gengzhi|||0000-0002-8000-8912
Zhou, Jin Yuan
Cabot i Codina, Andreu|||0000-0002-7533-3251
author Zhang, Chao Yue
author_facet Zhang, Chao Yue
Lu, Xuan|||0000-0003-2453-2805
Han, Xu|||0000-0001-8319-8830
Yu, Jing|||0000-0002-7620-745X
Zhang, Chaoqi|||0000-0002-0357-235X
Huang, Chen
Balcells i Argemí, Lluís|||0000-0001-6603-7357
Garzón Manjón, Alba|||0000-0003-2954-1102
Jacas Biendicho, Jordi|||0000-0001-5981-6168
Li, Junshan|||0000-0002-1482-1972
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Sun, Gengzhi|||0000-0002-8000-8912
Zhou, Jin Yuan
Cabot i Codina, Andreu|||0000-0002-7533-3251
author_role author
author2 Lu, Xuan|||0000-0003-2453-2805
Han, Xu|||0000-0001-8319-8830
Yu, Jing|||0000-0002-7620-745X
Zhang, Chaoqi|||0000-0002-0357-235X
Huang, Chen
Balcells i Argemí, Lluís|||0000-0001-6603-7357
Garzón Manjón, Alba|||0000-0003-2954-1102
Jacas Biendicho, Jordi|||0000-0001-5981-6168
Li, Junshan|||0000-0002-1482-1972
Arbiol i Cobos, Jordi|||0000-0002-0695-1726
Sun, Gengzhi|||0000-0002-8000-8912
Zhou, Jin Yuan
Cabot i Codina, Andreu|||0000-0002-7533-3251
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv Active site
Cationics
Electrochemical activation
Geometric configurations
Large parts
Polysulphides
Sodium-sulfur batteries
Spinel catalyst
Spinel structure
]+ catalyst
topic Active site
Cationics
Electrochemical activation
Geometric configurations
Large parts
Polysulphides
Sodium-sulfur batteries
Spinel catalyst
Spinel structure
]+ catalyst
description An AB2X4 spinel structure, with tetrahedral A and octahedral B sites, is a paradigmatic class of catalysts with several possible geometric configurations and numerous applications, including polysulfide conversion in metal-sulfur batteries. Nonetheless, the influence of the geometric configuration and composition on the mechanisms of catalysis and the precise manner in which spinel catalysts facilitate the conversion of polysulfides remain unknown. To enable controlled exposure of single active configurations, herein, Cotd2+ and Cooh3+ in Co3O4 catalysts for sodium polysulfide conversion are in large part replaced by Fetd2+ and Feoh3+, respectively, generating FeCo2O4 and CoFe2O4. Through an examination of electrochemical activation energies, the characterization of symmetric cells, and theoretical calculations, we determine that Cooh3+ serves as the active site for the breaking of S-S bonds, while Cotd2+ functions as the active site for the formation of S-Na bonds. The current study underlines the subtle relationship between activity and geometric configurations of spinel catalysts, providing unique insights for the rational development of improved catalysts by optimizing their atomic geometric configuration.
publishDate 2023
dc.date.none.fl_str_mv 2
2023-01-01
2023
2023-01-01
dc.type.none.fl_str_mv Article
http://purl.org/coar/resource_type/c_6501
SMUR
http://purl.org/coar/version/c_71e4c1898caa6e32
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://ddd.uab.cat/record/302220
https://dx.doi.org/urn:doi:10.1021/jacs.3c06288
url https://ddd.uab.cat/record/302220
https://dx.doi.org/urn:doi:10.1021/jacs.3c06288
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv Agència de Gestió d'Ajuts Universitaris i de Recerca https://doi.org/10.13039/501100003030 2021/SGR-00457
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2020-116093RB-C43
Ministerio de Ciencia e Innovación https://doi.org/10.13039/501100004837 CEX2021-001214-S
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 RYC2021-033479-I
Agencia Estatal de Investigación https://doi.org/10.13039/501100011033 PID2021-128410OB-I00
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://rightsstatements.org/vocab/InC/1.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
https://rightsstatements.org/vocab/InC/1.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Dipòsit Digital de Documents de la UAB
instname:Universitat Autònoma de Barcelona
instname_str Universitat Autònoma de Barcelona
reponame_str Dipòsit Digital de Documents de la UAB
collection Dipòsit Digital de Documents de la UAB
repository.name.fl_str_mv
repository.mail.fl_str_mv
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