Cation-Vacancy Engineering Modulated Perovskite Oxide for Boosting Electrocatalytic Conversion of Polysulfides

Bai, Z; Wang, Z; Wang, T; Wu, Z; Gao, X; Bai, Y; Wang, G; Sun, K

Cation-Vacancy Engineering Modulated Perovskite Oxide for Boosting Electrocatalytic Conversion of Polysulfides

Bai, Z Wang, Z Wang, T Wu, Z Gao, X Bai, Y Wang, G

Sun, K

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Publisher:: Wiley
Publication Type:: Journal Article
Citation:: Advanced Functional Materials, 2024
Issue Date:: 2024-01-01

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Field	Value	Language
dc.contributor.author	Bai, Z
dc.contributor.author	Wang, Z
dc.contributor.author	Wang, T
dc.contributor.author	Wu, Z
dc.contributor.author	Gao, X
dc.contributor.author	Bai, Y
dc.contributor.author	Wang, G https://orcid.org/0000-0003-4295-8578
dc.contributor.author	Sun, K
dc.date.accessioned	2025-02-03T00:06:25Z
dc.date.available	2025-02-03T00:06:25Z
dc.date.issued	2024-01-01
dc.identifier.citation	Advanced Functional Materials, 2024
dc.identifier.issn	1616-301X
dc.identifier.issn	1616-3028
dc.identifier.uri	http://hdl.handle.net/10453/184811
dc.description.abstract	Lithium-sulfur batteries face challenges like polysulfide shuttle and slow conversion kinetics, hindering their practical applications in renewable energy storage and electric vehicles. Herein, a solution to solve this issue is reported by using a cation vacancy engineering strategy with rational synthesis of La-deficient LaCoO3 (LCO-VLa). The introduction of cation vacancies in LCO-VLa modifies the geometric structure of coordinating atoms, exposing Co-rich surface with more catalytically active surfaces. Meanwhile, the d-band center of LCO-VLa shifts toward the Fermi level, enhancing polysulfide adsorption. Furthermore, multivalent cobalt ions (Co3+/Co4+) induced by charge compensation enhance the electrical conductivity of LCO-VLa, accelerating electron transfer processes and improving catalytic performance. Theoretical calculations and experimental characterizations demonstrate that La-deficient LCO-VLa effectively suppresses the polysulfide shuttle, reduces the energy barrier for polysulfide conversion, and accelerates redox reaction kinetics. LCO-VLa-based batteries demonstrate exceptional rate performance and cycling stability, retaining 70% capacity after nearly 500 cycles at 1.0 C, with a minimal decay rate of 0.055% per cycle. These findings highlight the significance of cation vacancy engineering for exploring precise structure-activity relationships during polysulfides conversion, facilitating the rational design of catalysts at the atomic level for lithium-sulfur batteries.
dc.language	en
dc.publisher	Wiley
dc.relation.ispartof	Advanced Functional Materials
dc.relation.isbasedon	10.1002/adfm.202419105
dc.rights	info:eu-repo/semantics/closedAccess
dc.subject	02 Physical Sciences, 03 Chemical Sciences, 09 Engineering
dc.subject.classification	Materials
dc.subject.classification	34 Chemical sciences
dc.subject.classification	40 Engineering
dc.subject.classification	51 Physical sciences
dc.title	Cation-Vacancy Engineering Modulated Perovskite Oxide for Boosting Electrocatalytic Conversion of Polysulfides
dc.type	Journal Article
utslib.for	02 Physical Sciences
utslib.for	03 Chemical Sciences
utslib.for	09 Engineering
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
pubs.organisational-group	University of Technology Sydney/UTS Groups
pubs.organisational-group	University of Technology Sydney/UTS Groups/Centre for Clean Energy Technology (CCET)
utslib.copyright.status	closed_access	*
dc.date.updated	2025-02-03T00:06:23Z
pubs.publication-status	Published

Abstract:

Lithium-sulfur batteries face challenges like polysulfide shuttle and slow conversion kinetics, hindering their practical applications in renewable energy storage and electric vehicles. Herein, a solution to solve this issue is reported by using a cation vacancy engineering strategy with rational synthesis of La-deficient LaCoO3 (LCO-VLa). The introduction of cation vacancies in LCO-VLa modifies the geometric structure of coordinating atoms, exposing Co-rich surface with more catalytically active surfaces. Meanwhile, the d-band center of LCO-VLa shifts toward the Fermi level, enhancing polysulfide adsorption. Furthermore, multivalent cobalt ions (Co3+/Co4+) induced by charge compensation enhance the electrical conductivity of LCO-VLa, accelerating electron transfer processes and improving catalytic performance. Theoretical calculations and experimental characterizations demonstrate that La-deficient LCO-VLa effectively suppresses the polysulfide shuttle, reduces the energy barrier for polysulfide conversion, and accelerates redox reaction kinetics. LCO-VLa-based batteries demonstrate exceptional rate performance and cycling stability, retaining 70% capacity after nearly 500 cycles at 1.0 C, with a minimal decay rate of 0.055% per cycle. These findings highlight the significance of cation vacancy engineering for exploring precise structure-activity relationships during polysulfides conversion, facilitating the rational design of catalysts at the atomic level for lithium-sulfur batteries.

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http://hdl.handle.net/10453/184811