Manipulating cation-anion coordination in fire-retardant electrolytes to enable high-areal-capacity fluoride conversion batteries

IF 17.3 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Matter Pub Date : 2024-11-06 DOI:10.1016/j.matt.2024.07.007
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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.

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操纵阻燃电解质中的阳离子-阴离子配位,实现高铝容量氟化物转换电池
资源丰富的多氧化还原氟化铁被认为是有希望用于大规模电池系统的阴极。然而,现有研究往往忽视了氟化物-电解质界面的关键问题,这些问题会导致电压高原模糊和容量下降。在此,我们提出了一种界面工程策略,通过操纵阻燃电解质中阳离子与阴离子的配位,实现转换型 FeF3 阴极。二氟(草酸)硼酸锂具有很强的电子亲和性,能诱导出富含阴离子的内部溶解鞘,从而主导阴极-电解质间相 (CEI) 的构建。富含无机物的 CEI 层具有电子绝缘和易于质量传输的特点,可抑制界面寄生反应并促进氟化物结构的可逆性。锂-铁-FeF3 电池能很好地保留电压高原,并具有 412 mAh g-1 的高容量和令人振奋的循环耐久性。优越的电解质润湿性进一步促进了氟化阴极在 FeF3 质量负荷为 7.0 mg cm-2 和贫电解质条件下的可逆面积容量高达 2.94 mAh cm-2。
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来源期刊
Matter
Matter MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
26.30
自引率
2.60%
发文量
367
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.
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