{"title":"Cu3VSe4 Cathode for Rechargeable Magnesium Batteries: Favorable Chemical and Electronic Structures Inducing Intercalation and Displacement Reactions","authors":"Donggang Tao, Ting Li, Yudi Tang, Hongda Gui, Yuliang Cao, Fei Xu","doi":"10.1002/adfm.202411223","DOIUrl":null,"url":null,"abstract":"Rechargeable Mg batteries are an advantageous energy-storage technology with low cost and high safety, but the design of high-performance cathode materials is currently the major difficulty. Herein, a new cathode material of Cu<sub>3</sub>VSe<sub>4</sub> is fabricated with a comprehensive consideration of the chemical and electronic structures. The intermediate band semiconductor Cu<sub>3</sub>VSe<sub>4</sub> has a cubic crystal structure containing interlaced 3D tunnels. The V and Se atoms form chemical bonds with high covalent proportions and facilitate the charge delocalization via the V‒Se bonds. Because of these features, Cu<sub>3</sub>VSe<sub>4</sub> provides a high capacity of 251 mAh g<sup>‒1</sup> with co-redox of Cu, V, and Se elements and an outstanding rate performance of 44 mAh g<sup>‒1</sup> at 15 A g<sup>‒1</sup>. Prominently, a high mass load of 3.0 mg cm<sup>‒2</sup> is achieved without obvious rate capability decay, which is quite favorable to pair with the high-capacity Mg metal anode in practical application. The mechanism investigation and theoretical computation demonstrate that Cu<sub>3</sub>VSe<sub>4</sub> undergoes first a Mg-intercalation and then a displacement reaction, during which the crystal structure is maintained, assisting the reaction reversibility and cycling stability. These findings reveal a rational design principle of rechargeable Mg battery cathodes based on a comprehensive consideration of chemical and electronic structures.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":18.5000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adfm.202411223","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Rechargeable Mg batteries are an advantageous energy-storage technology with low cost and high safety, but the design of high-performance cathode materials is currently the major difficulty. Herein, a new cathode material of Cu3VSe4 is fabricated with a comprehensive consideration of the chemical and electronic structures. The intermediate band semiconductor Cu3VSe4 has a cubic crystal structure containing interlaced 3D tunnels. The V and Se atoms form chemical bonds with high covalent proportions and facilitate the charge delocalization via the V‒Se bonds. Because of these features, Cu3VSe4 provides a high capacity of 251 mAh g‒1 with co-redox of Cu, V, and Se elements and an outstanding rate performance of 44 mAh g‒1 at 15 A g‒1. Prominently, a high mass load of 3.0 mg cm‒2 is achieved without obvious rate capability decay, which is quite favorable to pair with the high-capacity Mg metal anode in practical application. The mechanism investigation and theoretical computation demonstrate that Cu3VSe4 undergoes first a Mg-intercalation and then a displacement reaction, during which the crystal structure is maintained, assisting the reaction reversibility and cycling stability. These findings reveal a rational design principle of rechargeable Mg battery cathodes based on a comprehensive consideration of chemical and electronic structures.
期刊介绍:
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