Identifying the Role of the Cationic Geometric Configuration in Spinel Catalysts for Polysulfide Conversion in Sodium-Sulfur Batteries
Zhang, Chao Yue (Institut de Recerca en Energia de Catalunya)
Lu, Xuan (Institut de Recerca en Energia de Catalunya)
Han, Xu (Institut Català de Nanociència i Nanotecnologia)
Yu, Jing (Institut Català de Nanociència i Nanotecnologia)
Zhang, Chaoqi (Institut de Recerca en Energia de Catalunya)
Huang, Chen (Institut de Recerca en Energia de Catalunya)
Balcells Argemí, Lluís (Institut de Ciència de Materials de Barcelona)
Garzón-Manjón, Alba (Institut Català de Nanociència i Nanotecnologia)
Jacas Biendicho, Jordi (Institut de Recerca en Energia de Catalunya)
Li, Junshan (Chengdu University. Institute of Advanced Study)
Arbiol i Cobos, Jordi (Institut Català de Nanociència i Nanotecnologia)
Sun, Gengzhi (Nanjing Tech University. Institute of Advanced Materials)
Zhou, Jin Yuan (Qinghai Normal University)
Cabot i Codina, Andreu (Institució Catalana de Recerca i Estudis Avançats)

Date:	2023
Abstract:	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.
Grants:	Agència de Gestió d'Ajuts Universitaris i de Recerca 2021/SGR-00457 Agencia Estatal de Investigación PID2020-116093RB-C43 Ministerio de Ciencia e Innovación CEX2021-001214-S Agencia Estatal de Investigación RYC2021-033479-I Agencia Estatal de Investigación PID2021-128410OB-I00
Rights:	Aquest 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.
Language:	Anglès
Document:	Article ; recerca ; Versió sotmesa a revisió
Subject:	Active site ; Cationics ; Electrochemical activation ; Geometric configurations ; Large parts ; Polysulphides ; Sodium-sulfur batteries ; Spinel catalyst ; Spinel structure ; ]+ catalyst
Published in:	Journal of the American Chemical Society, Vol. 145, Issue 34 (August 2023) , p. 18992-19004, ISSN 1520-5126

DOI: 10.1021/jacs.3c06288

Preprint 14 p, 2.4 MB

The record appears in these collections:
Research literature > UAB research groups literature > Research Centres and Groups (research output) > Experimental sciences > Catalan Institute of Nanoscience and Nanotechnology (ICN2)
Articles > Research articles
Articles > Published articles