Engineering the Artificial Cathode-Electrolyte Interphase Coating for Solid-State Batteries via Tailored Annealing

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2025-03-11 DOI:10.1021/acs.chemmater.4c03086

Maximilian Kissel, Felix Walther, Jonas Hertle, Thomas Demuth, Ruizhuo Zhang, Philipp Brüner, Torsten Brezesinski, Kerstin Volz, Jürgen Janek

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引用次数: 0

Abstract

Solid-state batteries with nickel-rich layered oxide cathode active materials (CAMs) and sulfide-based solid electrolytes (SEs) are emerging as promising candidates for next-generation energy-storage systems. However, both active and electrolyte materials suffer from poor (electro)chemical compatibility, leading to severe degradation at the SE|CAM interface which is highly detrimental to the long-term cycling stability. Inspired by the natural cathode-electrolyte interphase (CEI), a novel coating concept involves formation of a protective, artificial CEI coating prior to cell assembly. Here, we investigate the oxidative annealing process after coating Li₃PS₄ as precursor onto polycrystalline LiNi_0.85Co_0.10Mn_0.05O₂ (NCM85). A combination of microscopic (scanning transmission electron microscopy, STEM), spectroscopic/spectrometric (X-ray photoelectron spectroscopy, XPS, low energy ion scattering, LEIS, and time-of-flight secondary ion mass spectrometry, ToF-SIMS), and electrochemical methods reveals that the composition, morphology, and performance of the coating can be tailored by controlled annealing in oxidizing atmosphere. The effect on coating quality and its stabilizing effect on the SE|CAM interface are examined. Only a morphologically and compositionally optimized coating can successfully prevent interfacial degradation, highlighting the need for tailored process parameters to fully exploit the coating potential. The optimization is supported by an efficient benchmarking framework combining electrochemical and analytical methods, which can serve as a basis for further systematic coating studies.

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.