Huilin Zhu
(, ), Shiwei Deng
(, ), Xinyi Kong
(, ), Xing Xiang
(, ), Yan Duan
(, ), Jian-Fang Wu
(, ), Jilei Liu
(, )
{"title":"在Li-LLTO复合阳极中通过过渡金属离子还原实现锂离子超快扩散的混合离子/电子导电框架","authors":"Huilin Zhu \n (, ), Shiwei Deng \n (, ), Xinyi Kong \n (, ), Xing Xiang \n (, ), Yan Duan \n (, ), Jian-Fang Wu \n (, ), Jilei Liu \n (, )","doi":"10.1007/s40843-025-3452-9","DOIUrl":null,"url":null,"abstract":"<div><p>The development of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) solid electrolytes is challenged by the unstable Li/LLZO interface during lithium stripping and plating processes, which impedes interfacial charge transport and accelerates lithium dendrite growth. Here, a freestanding ultrathin Li-Li<sub>0.3</sub>La<sub>0.5</sub>TiO<sub>3</sub> (LLTO) composite anode with a three-dimensional interconnected mixed ionic/electronic conducting LLTO framework was developed. The mixed ionic/electronic conduction of LLTO arises from the <i>in-situ</i> reduction of transition metal ions (Ti<sup>4+</sup>) by metallic lithium. The Li-LLTO composite anode possesses good affinity toward LLZO solid electrolytes, achieving a low interfacial resistance of 11.7 Ω cm<sup>2</sup>, and a high lithium self-diffusion coefficient reaching 4.5×10<sup>−11</sup> cm<sup>2</sup>/s, about one order of magnitude higher than that of pure lithium anode. These features collectively enhance the Li-LLTO/LLZO interfacial stability, increasing the critical current density fourfold and enabling a 1300-h symmetrical cell cycling life. It delivers high-performance solid-state lithium batteries with an 80% capacity retention after 220 cycles. This advancement not only improves the performance of lithium metal anodes in solid-state batteries but also offers promising insights for next-generation high-energy-density electrochemical energy storage systems.</p></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"68 8","pages":"2775 - 2782"},"PeriodicalIF":7.4000,"publicationDate":"2025-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mixed ionic/electronic conducting framework enabled by transition metal-ion reduction in Li-LLTO composite anodes for ultrafast lithium diffusion\",\"authors\":\"Huilin Zhu \\n (, ), Shiwei Deng \\n (, ), Xinyi Kong \\n (, ), Xing Xiang \\n (, ), Yan Duan \\n (, ), Jian-Fang Wu \\n (, ), Jilei Liu \\n (, )\",\"doi\":\"10.1007/s40843-025-3452-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The development of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) solid electrolytes is challenged by the unstable Li/LLZO interface during lithium stripping and plating processes, which impedes interfacial charge transport and accelerates lithium dendrite growth. Here, a freestanding ultrathin Li-Li<sub>0.3</sub>La<sub>0.5</sub>TiO<sub>3</sub> (LLTO) composite anode with a three-dimensional interconnected mixed ionic/electronic conducting LLTO framework was developed. The mixed ionic/electronic conduction of LLTO arises from the <i>in-situ</i> reduction of transition metal ions (Ti<sup>4+</sup>) by metallic lithium. The Li-LLTO composite anode possesses good affinity toward LLZO solid electrolytes, achieving a low interfacial resistance of 11.7 Ω cm<sup>2</sup>, and a high lithium self-diffusion coefficient reaching 4.5×10<sup>−11</sup> cm<sup>2</sup>/s, about one order of magnitude higher than that of pure lithium anode. These features collectively enhance the Li-LLTO/LLZO interfacial stability, increasing the critical current density fourfold and enabling a 1300-h symmetrical cell cycling life. It delivers high-performance solid-state lithium batteries with an 80% capacity retention after 220 cycles. This advancement not only improves the performance of lithium metal anodes in solid-state batteries but also offers promising insights for next-generation high-energy-density electrochemical energy storage systems.</p></div>\",\"PeriodicalId\":773,\"journal\":{\"name\":\"Science China Materials\",\"volume\":\"68 8\",\"pages\":\"2775 - 2782\"},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2025-07-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s40843-025-3452-9\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Materials","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s40843-025-3452-9","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Mixed ionic/electronic conducting framework enabled by transition metal-ion reduction in Li-LLTO composite anodes for ultrafast lithium diffusion
The development of Li7La3Zr2O12 (LLZO) solid electrolytes is challenged by the unstable Li/LLZO interface during lithium stripping and plating processes, which impedes interfacial charge transport and accelerates lithium dendrite growth. Here, a freestanding ultrathin Li-Li0.3La0.5TiO3 (LLTO) composite anode with a three-dimensional interconnected mixed ionic/electronic conducting LLTO framework was developed. The mixed ionic/electronic conduction of LLTO arises from the in-situ reduction of transition metal ions (Ti4+) by metallic lithium. The Li-LLTO composite anode possesses good affinity toward LLZO solid electrolytes, achieving a low interfacial resistance of 11.7 Ω cm2, and a high lithium self-diffusion coefficient reaching 4.5×10−11 cm2/s, about one order of magnitude higher than that of pure lithium anode. These features collectively enhance the Li-LLTO/LLZO interfacial stability, increasing the critical current density fourfold and enabling a 1300-h symmetrical cell cycling life. It delivers high-performance solid-state lithium batteries with an 80% capacity retention after 220 cycles. This advancement not only improves the performance of lithium metal anodes in solid-state batteries but also offers promising insights for next-generation high-energy-density electrochemical energy storage systems.
期刊介绍:
Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.