Ionocovalency of the Central Metal Halide Bond-Dependent Chemical Compatibility of Halide Solid Electrolytes with Li6PS5Cl

IF 19.3 1区 材料科学 Q1 CHEMISTRY, PHYSICAL ACS Energy Letters Pub Date : 2024-07-05 DOI:10.1021/acsenergylett.4c01084
Subha Samanta, Susmita Bera, Ripan K. Biswas, Sukanta Mondal, Lily Mandal, Abhik Banerjee
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Abstract

Halide solid electrolytes (HSEs), owing to their high oxidative stability, are used with high-voltage cathodes for all-solid-state batteries (ASSBs). However, their limited reduction stability against Li metal enforces a bilayer separator configuration with sulfide solid electrolytes (SSEs) in ASSBs. However, there are indications of electrochemical incompatibility between the HSE and SSE. Here, we study the chemical reactivity between SSE Li6PS5Cl with HSEs by varying the central metal and their impact on cell performance in bilayer configuration. We performed operando electrochemical impedance spectroscopy, temperature-dependent X-ray diffraction, ex situ X-ray photoelectron spectroscopy, and differential scanning calorimetry to quantify the reactivity between the SSE and HSE. We infer that the reaction kinetics is indeed determined by the central metal of the HSE, with Li3InCl6 and Li2ZrCl6 being highly reactive with Li6PS5Cl, whereas Li3YCl6, Li3ScCl6, and Li3ErCl6 are stable. Our work provides a guideline for selecting HSE and SSE pairs for bilayer ASSBs.

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中央金属卤化物键的离子共价性依赖于卤化物固体电解质与 Li6PS5Cl 的化学相容性
卤化物固体电解质(HSE)具有很高的氧化稳定性,因此被用于全固态电池(ASSB)的高压阴极。然而,由于它们对锂金属的还原稳定性有限,因此在全固态电池中必须采用硫化物固态电解质(SSE)的双层隔膜配置。然而,有迹象表明 HSE 和 SSE 之间存在电化学不相容性。在此,我们通过改变中心金属来研究 SSE Li6PS5Cl 与 HSE 之间的化学反应性及其对双层配置电池性能的影响。我们采用了操作电化学阻抗谱、温度依赖性 X 射线衍射、原位 X 射线光电子能谱和差示扫描量热法来量化 SSE 与 HSE 之间的反应性。我们推断,反应动力学确实是由 HSE 的中心金属决定的,Li3InCl6 和 Li2ZrCl6 与 Li6PS5Cl 的反应性很高,而 Li3YCl6、Li3ScCl6 和 Li3ErCl6 则很稳定。我们的工作为选择双层 ASSB 的 HSE 和 SSE 对提供了指导。
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来源期刊
ACS Energy Letters
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍: ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.
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