{"title":"Manipulating cation-anion coordination in fire-retardant electrolytes to enable high-areal-capacity fluoride conversion batteries","authors":"","doi":"10.1016/j.matt.2024.07.007","DOIUrl":null,"url":null,"abstract":"<div><div>Resource-abundant and multi-redox iron fluorides are considered promising cathodes for large-scale battery systems. However, existing research often overlooks the critical issues at the fluoride-electrolyte interface that cause voltage plateau blurring and capacity degradation. Here, we propose an interfacial engineering strategy for the conversion-type FeF<sub>3</sub> cathode enabled by manipulating the cation-anion coordination in a fire-retardant electrolyte. Lithium difluoro(oxalato)borate has strong electron affinity and induces an anion-rich inner solvation sheath, thereby dominating the construction of the cathode-electrolyte interphase (CEI). The inorganic-enriched CEI layer features electron insulation and facile mass transport, which could suppress interfacial parasitic reactions and promote fluoride structural reversibility. The Li-FeF<sub>3</sub> cell enables well-preserved voltage plateaus and a high capacity of 412 mAh g<sup>−1</sup> with inspiring cycle durability. The superior electrolyte wettability further contributes to a reversible areal capacity as high as 2.94 mAh cm<sup>−2</sup> for fluoride cathode under high FeF<sub>3</sub> mass loading of ∼7.0 mg cm<sup>−2</sup> and lean electrolyte conditions.</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":17.3000,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Matter","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2590238524004004","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Resource-abundant and multi-redox iron fluorides are considered promising cathodes for large-scale battery systems. However, existing research often overlooks the critical issues at the fluoride-electrolyte interface that cause voltage plateau blurring and capacity degradation. Here, we propose an interfacial engineering strategy for the conversion-type FeF3 cathode enabled by manipulating the cation-anion coordination in a fire-retardant electrolyte. Lithium difluoro(oxalato)borate has strong electron affinity and induces an anion-rich inner solvation sheath, thereby dominating the construction of the cathode-electrolyte interphase (CEI). The inorganic-enriched CEI layer features electron insulation and facile mass transport, which could suppress interfacial parasitic reactions and promote fluoride structural reversibility. The Li-FeF3 cell enables well-preserved voltage plateaus and a high capacity of 412 mAh g−1 with inspiring cycle durability. The superior electrolyte wettability further contributes to a reversible areal capacity as high as 2.94 mAh cm−2 for fluoride cathode under high FeF3 mass loading of ∼7.0 mg cm−2 and lean electrolyte conditions.
期刊介绍:
Matter, a monthly journal affiliated with Cell, spans the broad field of materials science from nano to macro levels,covering fundamentals to applications. Embracing groundbreaking technologies,it includes full-length research articles,reviews, perspectives,previews, opinions, personnel stories, and general editorial content.
Matter aims to be the primary resource for researchers in academia and industry, inspiring the next generation of materials scientists.