{"title":"湿化学法制备 Li3InCl6:微结构控制带来高离子电导率和更强的全固态电池性能。","authors":"Jacob Otabil Bonsu, Abhirup Bhadra, Dipan Kundu","doi":"10.1002/advs.202403208","DOIUrl":null,"url":null,"abstract":"<p><p>Thanks to superionic conductivity and compatibility with >4 V cathodes, halide solid electrolytes (SEs) have elicited tremendous interest for application in all-solid-state lithium batteries (ASSLBs). Many compositions based on groups 3, 13, and divalent metals, and substituted stoichiometries have been explored, some displaying requisite properties, but the Li<sup>+</sup> conductivity still falls short of theoretical predictions and appealing sulfide-type SEs. While controlling microstructural characteristics, namely grain boundary effects and microstrain, can boost ionic conductivity, they have rarely been considered. Moving away from the standard solid-state route, here a scalable and facile wet chemical approach for obtaining highly conductive (>2 mS cm<sup>-1</sup>) Li<sub>3</sub>InCl<sub>6</sub> is presented, and it is shown that aprotic solvents can reduce grain boundaries and microstrain, leading to very high ionic conductivity of over 4 mS cm<sup>-1</sup> (at 22 °C). Minimized grain boundary area renders improved moisture stability and enhances solid-solid interfacial contact, leading to excellent LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub>-based full-cell performance, exemplified by stable room temperature (22 °C) cycling at a 0.2 C rate with 155 mAh g<sup>-1</sup> capacity and 85% retention after 1000 cycles at 60 °C with a high 99.75% Coulombic efficiency. The findings showcase the viability of the aprotic solvent-mediated route for producing high-quality Li<sub>3</sub>InCl<sub>6</sub> for all-solid-state batteries.</p>","PeriodicalId":117,"journal":{"name":"Advanced Science","volume":null,"pages":null},"PeriodicalIF":14.3000,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Wet Chemistry Route to Li<sub>3</sub>InCl<sub>6</sub>: Microstructural Control Render High Ionic Conductivity and Enhanced All-Solid-State Battery Performance.\",\"authors\":\"Jacob Otabil Bonsu, Abhirup Bhadra, Dipan Kundu\",\"doi\":\"10.1002/advs.202403208\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Thanks to superionic conductivity and compatibility with >4 V cathodes, halide solid electrolytes (SEs) have elicited tremendous interest for application in all-solid-state lithium batteries (ASSLBs). Many compositions based on groups 3, 13, and divalent metals, and substituted stoichiometries have been explored, some displaying requisite properties, but the Li<sup>+</sup> conductivity still falls short of theoretical predictions and appealing sulfide-type SEs. While controlling microstructural characteristics, namely grain boundary effects and microstrain, can boost ionic conductivity, they have rarely been considered. Moving away from the standard solid-state route, here a scalable and facile wet chemical approach for obtaining highly conductive (>2 mS cm<sup>-1</sup>) Li<sub>3</sub>InCl<sub>6</sub> is presented, and it is shown that aprotic solvents can reduce grain boundaries and microstrain, leading to very high ionic conductivity of over 4 mS cm<sup>-1</sup> (at 22 °C). Minimized grain boundary area renders improved moisture stability and enhances solid-solid interfacial contact, leading to excellent LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub>-based full-cell performance, exemplified by stable room temperature (22 °C) cycling at a 0.2 C rate with 155 mAh g<sup>-1</sup> capacity and 85% retention after 1000 cycles at 60 °C with a high 99.75% Coulombic efficiency. 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引用次数: 0
摘要
卤化物固态电解质(SE)具有超离子电导率和与 >4 V 负极的兼容性,因此在全固态锂电池(ASSLB)中的应用引起了极大的兴趣。基于第 3 族、第 13 族和二价金属以及替代化学计量的许多成分都已得到探索,其中一些显示出了必要的特性,但锂+电导率仍未达到理论预测值,因此硫化物型固态电解质很有吸引力。虽然控制微结构特性(即晶界效应和微应变)可以提高离子电导率,但人们很少考虑这些因素。摒弃标准固态路线,本文介绍了一种可扩展的简便湿化学方法,用于获得高电导率(>2 mS cm-1)的 Li3InCl6,结果表明,钝化溶剂可以减少晶界和微应变,从而获得超过 4 mS cm-1 的超高离子电导率(22 °C)。最小化的晶界面积提高了湿度稳定性并增强了固-固界面接触,从而实现了基于 LiNi0.6Mn0.2Co0.2O2 的出色全电池性能,例如在 0.2 C 的速率下以 155 mAh g-1 的容量进行稳定的室温(22 °C)循环,在 60 °C 下循环 1000 次后保持 85% 的容量,库仑效率高达 99.75%。这些研究结果展示了以钝溶剂为媒介的路线生产全固态电池用高质量 Li3InCl6 的可行性。
Wet Chemistry Route to Li3InCl6: Microstructural Control Render High Ionic Conductivity and Enhanced All-Solid-State Battery Performance.
Thanks to superionic conductivity and compatibility with >4 V cathodes, halide solid electrolytes (SEs) have elicited tremendous interest for application in all-solid-state lithium batteries (ASSLBs). Many compositions based on groups 3, 13, and divalent metals, and substituted stoichiometries have been explored, some displaying requisite properties, but the Li+ conductivity still falls short of theoretical predictions and appealing sulfide-type SEs. While controlling microstructural characteristics, namely grain boundary effects and microstrain, can boost ionic conductivity, they have rarely been considered. Moving away from the standard solid-state route, here a scalable and facile wet chemical approach for obtaining highly conductive (>2 mS cm-1) Li3InCl6 is presented, and it is shown that aprotic solvents can reduce grain boundaries and microstrain, leading to very high ionic conductivity of over 4 mS cm-1 (at 22 °C). Minimized grain boundary area renders improved moisture stability and enhances solid-solid interfacial contact, leading to excellent LiNi0.6Mn0.2Co0.2O2-based full-cell performance, exemplified by stable room temperature (22 °C) cycling at a 0.2 C rate with 155 mAh g-1 capacity and 85% retention after 1000 cycles at 60 °C with a high 99.75% Coulombic efficiency. The findings showcase the viability of the aprotic solvent-mediated route for producing high-quality Li3InCl6 for all-solid-state batteries.
期刊介绍:
Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.