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A sinter-free route stabilizes cLLZO films at half the sintering temperature by establishing a time-temperature-transformation (TTT) diagram based on amorphous-to-crystalline transformation and crystallization enthalpy analysis, confirming stabilization down to 500 °C.",{"@graph":14,"@context":72},[15,34,55],{"@type":16,"itemListElement":17},"BreadcrumbList",[18,23,27,31],{"item":19,"name":20,"@type":21,"position":22},"https://docshare.wps.com","Home","ListItem",1,{"item":24,"name":25,"@type":21,"position":26},"https://docshare.wps.com/document/","Document",2,{"item":28,"name":29,"@type":21,"position":30},"https://docshare.wps.com/document/research-report/","Research & 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is cubic LLZO (cLLZO) important for battery electrolytes?","Question",{"text":62,"@type":63},"cLLZO offers high Li-ion conductivity and a wide electrochemical stability window, supporting compatibility with high-voltage cathodes and Li-metal anodes.","Answer",{"name":65,"@type":60,"acceptedAnswer":66},"What problem does high sintering temperature create in LLZO processing?",{"text":67,"@type":63},"High sintering temperatures increase production cost and energy consumption and can negatively affect cathode interface stability during scalable manufacture.",{"name":69,"@type":60,"acceptedAnswer":70},"How does the proposed “sinter-free” method stabilize cLLZO films?",{"text":71,"@type":63},"The method uses a time-temperature-transformation (TTT) diagram to guide amorphous-to-crystalline LLZO transformation, enabling stabilization of thin-film cLLZO at record low temperatures of 500 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Chem. Int. Ed. 2023, 62, e202304581 [doi.org/10.1002/anie.202304581](doi.org/10.1002/anie.202304581)  \nTime-Temperature-Transformation (TTT) Diagram of Battery-Grade Li-Garnet Electrolytes for Low-Temperature Sustainable Synthesis  \nYuntong Zhu, Michael Chon, Carl V. Thompson, and Jennifer L. M. Rupp*  \nAbstract: Efficient and affordable synthesis of Li + functional ceramics is crucial for the scalable production of solid electrolytes for batteries. Li-garnet Li7La3Zr2O12 􀀀 d (LLZO), especially its cubic phase (cLLZO), attracts attention due to its high Li + conductivity and wide electrochemical stability window. However, high sintering temperatures raise concerns about the cathode interface stability, production costs, and energy consumption for scalable manufacture. We show an alternative “sinter-free” route to stabilize cLLZO as films at half of its sinter temperature. Specifically, we establish a time-temperature-transformation (TTT) diagram which captures the amorphousto-crystalline LLZO transformation based on crystallization enthalpy analysis and confirm stabilization of thinfilm cLLZO at record low temperatures of 500 °C. Our findings pave the way for low-temperature processing via TTT diagrams, which can be used for battery cell design targeting reduced carbon footprints in manufacturing.  \n[*] Y. Zhu, M. Chon, C. V. Thompson, J. L. M. Rupp  \nDepartment of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139 (USA)  \nE-mail: [jrupp@mit.edu](jrupp@mit.edu)  \nJ. L. M. Rupp  \nDepartment of Chemistry, Technical University Munich, Garching 85748 (Germany)  \nJ. L. M. Rupp  \nTUMint. Energy Research GmbH, Lichtenbergstr. 4, Garching 85747 (Germany)  \nJ. L. M. Rupp  \nDepartment of Electrical and Computer Engineering, Technical University Munich, 80333 Munich (Germany)  \nJ. L. M. Rupp  \nDepartment of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, MA 02139 (USA)  \n © 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.  \nIntroduction  \nBattery performance and costs are the two most important factors when evaluating specific cell design and cell chemistry for use in electric vehicles (EVs) .[1–4] The former largely determines the driving distance and lifetime of EVs, whereas the latter dictates the cost-competitiveness of EVs relative to internal combustion vehicles (ICVs) .[2,3] To date, Li-ion batteries have shown promise as the most reliable energy-storage solution for EVs owing to their improved energy density and cycle life compared with that of battery systems developed earlier (e.g., lead-acid batteries, nickelcadmium batteries) . State-of-the-art Li-ion batteries with graphite (or graphite/Si composite) anodes, LiNiMnCoO2 􀀀 d (NMC) or LiNiCoAlO2 􀀀 d (NCA) cathodes, and organic liquid electrolytes are able to achieve gravimetric energy densities of 250–300 Wh kg 􀀀 1 at the cell level,[2] associated with a cost of approximately US$100 kWh 􀀀 1.[5] To accelerate the transition from ICVs to EVs, the US Department of Energy (DOE) set long-term objectives of reaching a production cost of \u003C US$60 kWh 􀀀 1 at the cell level and a specific energy density of > 500 Wh kg 􀀀 1 at the battery level by 2030.[6] One promising approach to achieve these ambitious goals is to revive the use of a Li-metal anode inan all-solid-state or hybrid battery configuration with partial or full substitution of the state-of-the-art organic liquid electrolytes and polymer separators by thin ceramic solidelectrolyte separators to achieve high energy density while minimizing the risk of L","cbCaivbne4T0j0Y3","https://ap.wps.com/l/cbCaivbne4T0j0Y3","pdf",1334782,13,"English","# Abstract\n# Introduction","[{\"question\":\"Why is cubic LLZO (cLLZO) important for battery electrolytes?\",\"answer\":\"cLLZO offers high Li-ion conductivity and a wide electrochemical stability window, supporting compatibility with high-voltage cathodes and Li-metal anodes.\"},{\"question\":\"What problem does high sintering temperature create in LLZO processing?\",\"answer\":\"High sintering temperatures increase production cost and energy consumption and can negatively affect cathode interface stability during scalable manufacture.\"},{\"question\":\"How does the proposed “sinter-free” method stabilize cLLZO films?\",\"answer\":\"The method uses a time-temperature-transformation (TTT) diagram to guide amorphous-to-crystalline LLZO transformation, enabling stabilization of thin-film cLLZO at record low temperatures of 500 °C.\"}]","Time-Temperature-Transformation (TTT) Diagram of Battery-Grade Li-Garnet Electrolytes for Low-Temperature Sustainable Synthesis | PDF",33]