Feng Jin, Laras Fadillah, Hung Quoc Nguyen, Torgeir Matre Sandvik, Yu Liu, Adrián García-Martín, Elena Salagre, Enrique G. Michel, Dragos Stoian, Kenneth Marshall, Wouter Van Beek, Günther Redhammer, Mir Mehraj Ud Din* and Daniel Rettenwander*,
{"title":"阐明 Li3InCl6 包覆 LiNi0.8Co0.15Al0.05O2 对基于 Li6PS5Cl 的固态电池电化学力学的影响","authors":"Feng Jin, Laras Fadillah, Hung Quoc Nguyen, Torgeir Matre Sandvik, Yu Liu, Adrián García-Martín, Elena Salagre, Enrique G. Michel, Dragos Stoian, Kenneth Marshall, Wouter Van Beek, Günther Redhammer, Mir Mehraj Ud Din* and Daniel Rettenwander*, ","doi":"10.1021/acs.chemmater.4c00515","DOIUrl":null,"url":null,"abstract":"<p >Li<sub>6</sub>PS<sub>5</sub>Cl has attracted significant attention due to its high Li-ion conductivity and processability, facilitating large-scale solid-state battery applications. However, when paired with high-voltage cathodes, it experiences adverse side reactions. Li<sub>3</sub>InCl<sub>6</sub> (LIC), known for its higher stability at high voltages and moderate Li-ion conductivity, is considered a catholyte to address the limitations of Li<sub>6</sub>PS<sub>5</sub>Cl. To extend the stability of Li<sub>6</sub>PS<sub>5</sub>Cl toward LiNi<sub>0.8</sub>Co<sub>0.15</sub>Al<sub>0.05</sub>O<sub>2</sub> (NCA), we applied nanocrystalline LIC as a 180 nm-thick protective coating in a core–shell-like fashion (LIC@NCA) via mechanofusion. Solid-state batteries with LIC@NCA allow an initial discharge specific capacity of 148 mA h/g at 0.1C and 80% capacity retention for 200 cycles at 0.2C with a cutoff voltage of 4.2 V (vs Li/Li<sup>+</sup>), while cells without LIC coating suffers from low initial discharge capacity and poor retention. Using a wide spectrum of advanced characterization techniques, such as operando XRD, XPS, FIB-SEM, and TOF-SIMS, we reveal that the superior performance of solid-state batteries employing LIC@NCA is related to the suppression of detrimental interfacial reactions of NCA with Li<sub>6</sub>PS<sub>5</sub>Cl, delamination, and particle cracking compared to uncoated NCA.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2024-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c00515","citationCount":"0","resultStr":"{\"title\":\"Elucidating the Impact of Li3InCl6-Coated LiNi0.8Co0.15Al0.05O2 on the Electro-Chemo-Mechanics of Li6PS5Cl-Based Solid-State Batteries\",\"authors\":\"Feng Jin, Laras Fadillah, Hung Quoc Nguyen, Torgeir Matre Sandvik, Yu Liu, Adrián García-Martín, Elena Salagre, Enrique G. Michel, Dragos Stoian, Kenneth Marshall, Wouter Van Beek, Günther Redhammer, Mir Mehraj Ud Din* and Daniel Rettenwander*, \",\"doi\":\"10.1021/acs.chemmater.4c00515\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Li<sub>6</sub>PS<sub>5</sub>Cl has attracted significant attention due to its high Li-ion conductivity and processability, facilitating large-scale solid-state battery applications. However, when paired with high-voltage cathodes, it experiences adverse side reactions. Li<sub>3</sub>InCl<sub>6</sub> (LIC), known for its higher stability at high voltages and moderate Li-ion conductivity, is considered a catholyte to address the limitations of Li<sub>6</sub>PS<sub>5</sub>Cl. To extend the stability of Li<sub>6</sub>PS<sub>5</sub>Cl toward LiNi<sub>0.8</sub>Co<sub>0.15</sub>Al<sub>0.05</sub>O<sub>2</sub> (NCA), we applied nanocrystalline LIC as a 180 nm-thick protective coating in a core–shell-like fashion (LIC@NCA) via mechanofusion. Solid-state batteries with LIC@NCA allow an initial discharge specific capacity of 148 mA h/g at 0.1C and 80% capacity retention for 200 cycles at 0.2C with a cutoff voltage of 4.2 V (vs Li/Li<sup>+</sup>), while cells without LIC coating suffers from low initial discharge capacity and poor retention. 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Elucidating the Impact of Li3InCl6-Coated LiNi0.8Co0.15Al0.05O2 on the Electro-Chemo-Mechanics of Li6PS5Cl-Based Solid-State Batteries
Li6PS5Cl has attracted significant attention due to its high Li-ion conductivity and processability, facilitating large-scale solid-state battery applications. However, when paired with high-voltage cathodes, it experiences adverse side reactions. Li3InCl6 (LIC), known for its higher stability at high voltages and moderate Li-ion conductivity, is considered a catholyte to address the limitations of Li6PS5Cl. To extend the stability of Li6PS5Cl toward LiNi0.8Co0.15Al0.05O2 (NCA), we applied nanocrystalline LIC as a 180 nm-thick protective coating in a core–shell-like fashion (LIC@NCA) via mechanofusion. Solid-state batteries with LIC@NCA allow an initial discharge specific capacity of 148 mA h/g at 0.1C and 80% capacity retention for 200 cycles at 0.2C with a cutoff voltage of 4.2 V (vs Li/Li+), while cells without LIC coating suffers from low initial discharge capacity and poor retention. Using a wide spectrum of advanced characterization techniques, such as operando XRD, XPS, FIB-SEM, and TOF-SIMS, we reveal that the superior performance of solid-state batteries employing LIC@NCA is related to the suppression of detrimental interfacial reactions of NCA with Li6PS5Cl, delamination, and particle cracking compared to uncoated NCA.
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.