Li-ion transport mechanisms in Ge/Cl dual-doped Li10GeP2S12 solid electrolytes: Synergistic insights from experimental structural characterization and machine-learning-assisted atomistic modeling

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Carbon Energy Pub Date : 2024-07-02 DOI:10.1002/cey2.594
Yong-Seok Choi, Jiwon Jeong, Youngin Lee, Hyuna Ahn, David O. Scanlon, Kyung Yoon Chung, Jae-Chul Lee
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Abstract

Enhancing the ionic conductivity of sulfide solid electrolytes (SEs) through dual-doping is a well-established approach, yet the atomic-level mechanisms driving these improvements remain elusive. By dual-doping Ge and Cl into the Li10GeP2S12 (LGPS) framework, we synthesized Ge/Cl-doped LGPS (Li10+xGe1+2xP2−2xS12−xClx, x = 0.3) with an ionic conductivity of 12.4 mS/cm at 25°C, a value that stands among the highest for LGPS-type SEs. This achievement emphasizes the pivotal role of dopant selection in modulating Li-ion transport mechanisms, thereby enhancing SE performance. Our research elucidates the intricate atomic mechanisms responsible for this enhanced ionic conductivity, with a particular focus on the synergistic effects of Ge and Cl dual-doping. Integrating advanced multianalytical techniques, including experiments and atomistic modeling (machine-learning-assisted molecular dynamics simulations and density functional theory calculations), we provide comprehensive insights into the structure–property relationship in Ge/Cl-doped LGPS SEs. Our findings reveal that Cl doping significantly enhances the paddle-wheel dynamics, while Ge doping promotes cooperative Li diffusion through the formation of Li interstitials. This dual-doping approach not only elucidates the structural and functional dynamics of SEs but also paves the way for designing dopants to enhance ionic conductivity. The insights gained from this study offer a strategic direction for developing higher-performance SEs, highlighting the importance of tailored dopant selection in advancing energy storage technologies.

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Ge/Cl 双掺杂 Li10GeP2S12 固体电解质中的锂离子传输机制:来自实验结构表征和机器学习辅助原子模型的协同见解
通过双重掺杂提高硫化物固体电解质(SEs)的离子电导率是一种行之有效的方法,但驱动这些改进的原子级机制仍然难以捉摸。通过在 Li10GeP2S12(LGPS)框架中双掺杂 Ge 和 Cl,我们合成了掺杂 Ge/Cl 的 LGPS(Li10+xGe1+2xP2-2xS12-xClx,x = 0.3),其在 25°C 时的离子电导率为 12.4 mS/cm,是 LGPS 型 SE 的最高值之一。这一成就强调了掺杂剂选择在调节锂离子传输机制,从而提高 SE 性能方面的关键作用。我们的研究阐明了导致离子传导性增强的复杂原子机制,尤其关注 Ge 和 Cl 双掺杂的协同效应。通过整合先进的多分析技术,包括实验和原子建模(机器学习辅助分子动力学模拟和密度泛函理论计算),我们对掺杂 Ge/Cl 的 LGPS SE 的结构-性能关系有了全面的了解。我们的研究结果表明,Cl 掺杂显著增强了桨轮动力学,而 Ge 掺杂则通过形成锂间隙促进了锂的协同扩散。这种双重掺杂方法不仅阐明了 SE 的结构和功能动力学,还为设计掺杂剂以增强离子导电性铺平了道路。从这项研究中获得的启示为开发更高性能的 SE 提供了一个战略方向,突出了量身定制的掺杂剂选择在推动储能技术发展中的重要性。
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来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
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Issue Information Cover Image, Volume 6, Number 10, October 2024 Back Cover Image, Volume 6, Number 10, October 2024 Interface and doping engineering of V2C-MXene-based electrocatalysts for enhanced electrocatalysis of overall water splitting Issue Information
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