Linking Local Ionic Conductivity, Microstructure, and Nanomechanical Properties to Bulk Performance for Enhanced Design of Solid Polymer Electrolytes

IF 9.6 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-04-10 DOI:10.1021/acsmaterialslett.5c0022210.1021/acsmaterialslett.5c00222

Vinay Saini, Gleb Bobrov, Hai Le, Philip Egberts* and Milana Trifkovic*,

{"title":"Linking Local Ionic Conductivity, Microstructure, and Nanomechanical Properties to Bulk Performance for Enhanced Design of Solid Polymer Electrolytes","authors":"Vinay Saini, Gleb Bobrov, Hai Le, Philip Egberts* and Milana Trifkovic*, ","doi":"10.1021/acsmaterialslett.5c0022210.1021/acsmaterialslett.5c00222","DOIUrl":null,"url":null,"abstract":"Poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) incorporating LiTFSI and LiClO4 are widely studied, yet the impact of salt type on Li+ ion transport and morphology remains poorly understood. Here, we use current-sensing atomic force microscopy (CS-AFM) to probe the Li+ migration and nanomechanical properties in SPEs with varying salt loadings. Topological and ionic current mapping over 80 × 80 μm2 under 0.5 V bias reveals that LiClO4 induces rapid spherulitic growth, expelling salt and causing spatial heterogeneity in conductivity. In contrast, LiTFSI yields more homogeneous structures and conduction. Elemental and nanomechanical mapping confirms these patterns, showing distinct moduli and hardness between crystalline and amorphous regions in LiClO4-based SPEs, while LiTFSI-based systems remain more uniform. These spatial variations adversely affect electrode contact and long-term stability. Our findings highlight the importance of understanding multiscale ionic transport and morphology to guide the design of next-generation SPEs for solid-state batteries.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1830–1836 1830–1836"},"PeriodicalIF":9.6000,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Materials Letters","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsmaterialslett.5c00222","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) incorporating LiTFSI and LiClO₄ are widely studied, yet the impact of salt type on Li⁺ ion transport and morphology remains poorly understood. Here, we use current-sensing atomic force microscopy (CS-AFM) to probe the Li⁺ migration and nanomechanical properties in SPEs with varying salt loadings. Topological and ionic current mapping over 80 × 80 μm² under 0.5 V bias reveals that LiClO₄ induces rapid spherulitic growth, expelling salt and causing spatial heterogeneity in conductivity. In contrast, LiTFSI yields more homogeneous structures and conduction. Elemental and nanomechanical mapping confirms these patterns, showing distinct moduli and hardness between crystalline and amorphous regions in LiClO₄-based SPEs, while LiTFSI-based systems remain more uniform. These spatial variations adversely affect electrode contact and long-term stability. Our findings highlight the importance of understanding multiscale ionic transport and morphology to guide the design of next-generation SPEs for solid-state batteries.

Abstract Image

查看原文本刊更多论文

链接局部离子电导率，微观结构和纳米力学性能，以提高固体聚合物电解质的整体性能

含有LiTFSI和LiClO4的聚环氧乙烷（PEO）基固体聚合物电解质（spe）被广泛研究，但盐类型对Li+离子传输和形态的影响尚不清楚。在这里，我们使用电流传感原子力显微镜（CS-AFM）来探测不同盐负载下spe中Li+的迁移和纳米力学性能。在0.5 V偏置下，在80 × 80 μm2以上的拓扑电流和离子电流映射表明，LiClO4诱导了快速的球晶生长，排斥了盐，导致了电导率的空间异质性。相比之下，LiTFSI产生更均匀的结构和传导。元素和纳米力学映射证实了这些模式，显示出liclo4基SPEs晶体和非晶态区域之间不同的模量和硬度，而基于litfsi的SPEs系统保持更均匀。这些空间变化对电极接触和长期稳定性有不利影响。我们的研究结果强调了理解多尺度离子传输和形态对指导下一代固态电池spe设计的重要性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.