Impact of Lithium Nonstoichiometry on Ionic Diffusion in Tetragonal Garnet-Type Li7La3Zr2O12 DOI
Zihan Yan, Yizhou Zhu

Chemistry of Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 19, 2024

Understanding ion transport mechanisms on the atomistic scale in solid-state electrolytes is crucial for development of all-solid-state batteries. Li7La3Zr2O12 (LLZO) a promising oxide solid electrolyte material, whose phase transition behavior and have attracted significant research attention. Previous studies primarily focused cubic (intrinsic high-temperature or doped variants). In contrast, tetragonal LLZO, despite its close relationship with phase, has received less attention due to relatively low ionic conductivity high computational cost. A few recent shown discrepancies activation energy between calculated experimental values. Therefore, unclear LLZO are critical understanding designing electrolytes. this study, we employ state-of-the-art machine-learning-based neuroevolution potential molecular dynamics simulations investigate effects lithium nonstoichiometry stability LLZO. We demonstrate that small deviations from stoichiometry, particularly deficiency, dramatically reduce Li+ diffusion 1.227 0.425 eV, increasing room-temperature by 10 orders magnitude. The slight nonstoichiometry, which commonly occurs during synthesis, effect phase. Our findings highlight role defect chemistry enhancing performance provide insights rational design high-performance through engineering.

Язык: Английский

A Comprehensive Review of Sulfide Solid-State Electrolytes: Properties, Synthesis, Applications, and Challenges DOI Creative Commons

Baoyuan Man,

Yu Zeng, Qingrui Liu

и другие.

Crystals, Год журнала: 2025, Номер 15(6), С. 492 - 492

Опубликована: Май 22, 2025

Traditional lithium-ion batteries (LIBs) utilize liquid electrolytes, which pose significant safety risks. To address these concerns and enhance energy density, all-solid-state (ASSBs) have emerged as a safer more efficient alternative to conventional electrolyte-based systems. ASSBs offer notable advantages, including higher density improved safety, driving growing interest from both industry academia. A key component in battery (ASSB) development is the solid-state electrolyte (SSE), plays crucial role determining overall performance of batteries. Sulfide SSEs are characterized by distinctive attributes, notably high ionic conductivity remarkably low interfacial resistance with lithium metal anodes, renders them particularly advantageous for advancing ASSB technology. This paper systematically examines sulfide-based SSEs, particular emphasis on their underlying physicochemical properties, structural characteristics, essential functional attributes relevant applications. Additionally, we explore preparation methods sulfide analyze potential applications next-generation ASSBs. Considering current challenges (e.g., instability or air sensitivity) summarize strategies obstacles, aiming facilitate integration into future storage

Язык: Английский

Процитировано

0
Impact of Lithium Nonstoichiometry on Ionic Diffusion in Tetragonal Garnet-Type Li7La3Zr2O12 DOI
Zihan Yan, Yizhou Zhu

Chemistry of Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 19, 2024

Understanding ion transport mechanisms on the atomistic scale in solid-state electrolytes is crucial for development of all-solid-state batteries. Li7La3Zr2O12 (LLZO) a promising oxide solid electrolyte material, whose phase transition behavior and have attracted significant research attention. Previous studies primarily focused cubic (intrinsic high-temperature or doped variants). In contrast, tetragonal LLZO, despite its close relationship with phase, has received less attention due to relatively low ionic conductivity high computational cost. A few recent shown discrepancies activation energy between calculated experimental values. Therefore, unclear LLZO are critical understanding designing electrolytes. this study, we employ state-of-the-art machine-learning-based neuroevolution potential molecular dynamics simulations investigate effects lithium nonstoichiometry stability LLZO. We demonstrate that small deviations from stoichiometry, particularly deficiency, dramatically reduce Li+ diffusion 1.227 0.425 eV, increasing room-temperature by 10 orders magnitude. The slight nonstoichiometry, which commonly occurs during synthesis, effect phase. Our findings highlight role defect chemistry enhancing performance provide insights rational design high-performance through engineering.

Язык: Английский

Процитировано

2