Canfu Zhang, Binbin Chen, Qinlong Chen, Yingchun Liu, Xueqian Kong, Liumin Suo, Jun Lu, Huilin Pan
{"title":"Regulation of Molecular Microheterogeneity in Electrolytes Enables Ampere-Hour-Level Aqueous LiMn<sub>2</sub>O<sub>4</sub>||Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> Pouch Cells.","authors":"Canfu Zhang, Binbin Chen, Qinlong Chen, Yingchun Liu, Xueqian Kong, Liumin Suo, Jun Lu, Huilin Pan","doi":"10.1002/adma.202405913","DOIUrl":null,"url":null,"abstract":"<p><p>Aqueous batteries are attractive due to their high safety and fast reaction kinetics, but the narrow electrochemical stability window of H<sub>2</sub>O limits their applications. It is a big challenge to broaden the electrochemical operation window of aqueous electrolytes while retaining fast reaction kinetics. Here, a new organic aqueous mixture electrolyte of manipulatable (3D) molecular microheterogeneity with H<sub>2</sub>O-rich and H<sub>2</sub>O-poor domains is demonstrated. H<sub>2</sub>O-poor domains molecularly surround the reformed microclusters of H<sub>2</sub>O molecules through interfacial H-bonds, which thus not only inhibit the long-range transfer of H<sub>2</sub>O but also allow fast and consecutive Li<sup>+</sup> transport. This new design enables low-voltage anodes reversibly cycling with aqueous-based electrolytes and high ionic conductivity of 4.5 mS cm<sup>-1</sup>. LiMn<sub>2</sub>O<sub>4</sub>||Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> full cells demonstrate excellent cycling stability over 1000 cycles under various C rates and a low temperature of -20 °C. 1 Ah pouch cell delivers a high energy density of 79.3 Wh kg<sup>-1</sup> and high Coulombic efficiency of 99.4% at 1 C over 200 cycles. This work provides new insights into the design of electrolytes based on the molecular microheterogeneity for rechargeable batteries.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":null,"pages":null},"PeriodicalIF":27.4000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202405913","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/8/21 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Aqueous batteries are attractive due to their high safety and fast reaction kinetics, but the narrow electrochemical stability window of H2O limits their applications. It is a big challenge to broaden the electrochemical operation window of aqueous electrolytes while retaining fast reaction kinetics. Here, a new organic aqueous mixture electrolyte of manipulatable (3D) molecular microheterogeneity with H2O-rich and H2O-poor domains is demonstrated. H2O-poor domains molecularly surround the reformed microclusters of H2O molecules through interfacial H-bonds, which thus not only inhibit the long-range transfer of H2O but also allow fast and consecutive Li+ transport. This new design enables low-voltage anodes reversibly cycling with aqueous-based electrolytes and high ionic conductivity of 4.5 mS cm-1. LiMn2O4||Li4Ti5O12 full cells demonstrate excellent cycling stability over 1000 cycles under various C rates and a low temperature of -20 °C. 1 Ah pouch cell delivers a high energy density of 79.3 Wh kg-1 and high Coulombic efficiency of 99.4% at 1 C over 200 cycles. This work provides new insights into the design of electrolytes based on the molecular microheterogeneity for rechargeable batteries.
期刊介绍:
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