James T. Bamford, Seamus D. Jones, Nicole S. Schauser, Benjamin J. Pedretti, Leo W. Gordon, Nathaniel A. Lynd, Raphaële J. Clément and Rachel A. Segalman*,
{"title":"在不牺牲聚合物电解质中锂离子传输性能的前提下提高机械强度","authors":"James T. Bamford, Seamus D. Jones, Nicole S. Schauser, Benjamin J. Pedretti, Leo W. Gordon, Nathaniel A. Lynd, Raphaële J. Clément and Rachel A. Segalman*, ","doi":"10.1021/acsmacrolett.4c00158","DOIUrl":null,"url":null,"abstract":"<p >Next-generation batteries demand solid polymer electrolytes (SPEs) with rapid ion transport and robust mechanical properties. However, many SPEs with liquid-like Li<sup>+</sup> transport mechanisms suffer a fundamental trade-off between conductivity and strength. Dynamic polymer networks can improve bulk mechanics with minimal impact to segmental relaxation or ionic conductivity. This study demonstrates a system where a single polymer-bound ligand simultaneously dissociates Li<sup>+</sup> and forms long-lived Ni<sup>2+</sup> networks. The polymer comprises an ethylene oxide backbone and imidazole (Im) ligands, blended with Li<sup>+</sup> and Ni<sup>2+</sup> salts. Ni<sup>2+</sup>–Im dynamic cross-links result in the formation of a rubbery plateau resulting in, consequently, storage modulus improvement by a factor of 133× with the introduction of Ni<sup>2+</sup> at <i>r</i><sub>Ni</sub> = 0.08, from 0.014 to 1.907 MPa. Even with Ni<sup>2+</sup> loading, the high Li<sup>+</sup> conductivity of 3.7 × 10<sup>–6</sup> S/cm is retained at 90 °C. This work demonstrates that decoupling of ion transport and bulk mechanics can be readily achieved by the addition of multivalent metal cations to polymers with chelating ligands.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":null,"pages":null},"PeriodicalIF":5.1000,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Improved Mechanical Strength without Sacrificing Li-Ion Transport in Polymer Electrolytes\",\"authors\":\"James T. Bamford, Seamus D. Jones, Nicole S. Schauser, Benjamin J. Pedretti, Leo W. Gordon, Nathaniel A. Lynd, Raphaële J. Clément and Rachel A. Segalman*, \",\"doi\":\"10.1021/acsmacrolett.4c00158\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Next-generation batteries demand solid polymer electrolytes (SPEs) with rapid ion transport and robust mechanical properties. However, many SPEs with liquid-like Li<sup>+</sup> transport mechanisms suffer a fundamental trade-off between conductivity and strength. Dynamic polymer networks can improve bulk mechanics with minimal impact to segmental relaxation or ionic conductivity. This study demonstrates a system where a single polymer-bound ligand simultaneously dissociates Li<sup>+</sup> and forms long-lived Ni<sup>2+</sup> networks. The polymer comprises an ethylene oxide backbone and imidazole (Im) ligands, blended with Li<sup>+</sup> and Ni<sup>2+</sup> salts. Ni<sup>2+</sup>–Im dynamic cross-links result in the formation of a rubbery plateau resulting in, consequently, storage modulus improvement by a factor of 133× with the introduction of Ni<sup>2+</sup> at <i>r</i><sub>Ni</sub> = 0.08, from 0.014 to 1.907 MPa. Even with Ni<sup>2+</sup> loading, the high Li<sup>+</sup> conductivity of 3.7 × 10<sup>–6</sup> S/cm is retained at 90 °C. This work demonstrates that decoupling of ion transport and bulk mechanics can be readily achieved by the addition of multivalent metal cations to polymers with chelating ligands.</p>\",\"PeriodicalId\":18,\"journal\":{\"name\":\"ACS Macro Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.1000,\"publicationDate\":\"2024-05-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Macro Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsmacrolett.4c00158\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"POLYMER SCIENCE\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Macro Letters","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsmacrolett.4c00158","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
Improved Mechanical Strength without Sacrificing Li-Ion Transport in Polymer Electrolytes
Next-generation batteries demand solid polymer electrolytes (SPEs) with rapid ion transport and robust mechanical properties. However, many SPEs with liquid-like Li+ transport mechanisms suffer a fundamental trade-off between conductivity and strength. Dynamic polymer networks can improve bulk mechanics with minimal impact to segmental relaxation or ionic conductivity. This study demonstrates a system where a single polymer-bound ligand simultaneously dissociates Li+ and forms long-lived Ni2+ networks. The polymer comprises an ethylene oxide backbone and imidazole (Im) ligands, blended with Li+ and Ni2+ salts. Ni2+–Im dynamic cross-links result in the formation of a rubbery plateau resulting in, consequently, storage modulus improvement by a factor of 133× with the introduction of Ni2+ at rNi = 0.08, from 0.014 to 1.907 MPa. Even with Ni2+ loading, the high Li+ conductivity of 3.7 × 10–6 S/cm is retained at 90 °C. This work demonstrates that decoupling of ion transport and bulk mechanics can be readily achieved by the addition of multivalent metal cations to polymers with chelating ligands.
期刊介绍:
ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science.
With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.