Jie Zhang, Jun Jin, Ouwei Sheng, Ya Chen, Yan Lu, Zhaoyin Wen
{"title":"通过物理抑制和化学清除锂枝晶的协同夹层提高基于 LGPS 的锂金属电池的临界电流密度","authors":"Jie Zhang, Jun Jin, Ouwei Sheng, Ya Chen, Yan Lu, Zhaoyin Wen","doi":"10.1021/acsami.4c14887","DOIUrl":null,"url":null,"abstract":"Li<sub>10.35</sub>Ge<sub>1.35</sub>P<sub>1.65</sub>S<sub>12</sub> (LGPS) electrolyte has garnered attention due to its high ionic conductivity and processability. However, its strong incompatibility with lithium metal hinders its practical application. Conventional interlayer strategy isolates Li from LGPS, avoiding the detrimental side reactions, but lithium dendrite penetration is still a problem. To address the aforementioned challenges, we develop a PVDF-HFP-supported PDOL-based interlayer (PDOL/PVDF-HFP), which stabilizes the LGPS/Li interface by synergistically physically inhibiting and chemically scavenging lithium dendrites. The multifunctional feature of the interlayer comes from the use of a bifunctional initiator, InCl<sub>3</sub>. On the one hand, InCl<sub>3</sub> induces the polymerization of DOL, forming a physical separator and protecting lithium from LGPS; on the other hand, in situ reactions between In<sup>3+</sup>/Cl<sup>–</sup> and Li form a LiCl/LiF/LiIn hybrid SEI, homogenizing the surface Li<sup>+</sup> flux and suppressing lithium dendrite formation and penetration. In addition, an unexpected dynamic microdendrite scavenging is realized by virtue of the side reactions of LGPS/Li, which converts the undesirable reaction to be an advantage in our design. Benefiting from the comprehensive advantages of such design, the constructed sulfide-based solid-state batteries achieve a super low interfacial impedance of 5.1 Ω, a high critical current density (CCD) value over 5 mA/cm<sup>2</sup>, and a super long cycling stability over 8000 h. Our synergistic interlayer strategy would open an effective avenue for solving interfacial challenges for practical sulfide-based solid-state batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3000,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Achieving Higher Critical Current Density in LGPS-Based Lithium Metal Batteries via a Synergistic Interlayer for Physical Inhibition and Chemical Scavenging of Lithium Dendrites\",\"authors\":\"Jie Zhang, Jun Jin, Ouwei Sheng, Ya Chen, Yan Lu, Zhaoyin Wen\",\"doi\":\"10.1021/acsami.4c14887\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Li<sub>10.35</sub>Ge<sub>1.35</sub>P<sub>1.65</sub>S<sub>12</sub> (LGPS) electrolyte has garnered attention due to its high ionic conductivity and processability. However, its strong incompatibility with lithium metal hinders its practical application. Conventional interlayer strategy isolates Li from LGPS, avoiding the detrimental side reactions, but lithium dendrite penetration is still a problem. To address the aforementioned challenges, we develop a PVDF-HFP-supported PDOL-based interlayer (PDOL/PVDF-HFP), which stabilizes the LGPS/Li interface by synergistically physically inhibiting and chemically scavenging lithium dendrites. The multifunctional feature of the interlayer comes from the use of a bifunctional initiator, InCl<sub>3</sub>. On the one hand, InCl<sub>3</sub> induces the polymerization of DOL, forming a physical separator and protecting lithium from LGPS; on the other hand, in situ reactions between In<sup>3+</sup>/Cl<sup>–</sup> and Li form a LiCl/LiF/LiIn hybrid SEI, homogenizing the surface Li<sup>+</sup> flux and suppressing lithium dendrite formation and penetration. In addition, an unexpected dynamic microdendrite scavenging is realized by virtue of the side reactions of LGPS/Li, which converts the undesirable reaction to be an advantage in our design. Benefiting from the comprehensive advantages of such design, the constructed sulfide-based solid-state batteries achieve a super low interfacial impedance of 5.1 Ω, a high critical current density (CCD) value over 5 mA/cm<sup>2</sup>, and a super long cycling stability over 8000 h. 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Achieving Higher Critical Current Density in LGPS-Based Lithium Metal Batteries via a Synergistic Interlayer for Physical Inhibition and Chemical Scavenging of Lithium Dendrites
Li10.35Ge1.35P1.65S12 (LGPS) electrolyte has garnered attention due to its high ionic conductivity and processability. However, its strong incompatibility with lithium metal hinders its practical application. Conventional interlayer strategy isolates Li from LGPS, avoiding the detrimental side reactions, but lithium dendrite penetration is still a problem. To address the aforementioned challenges, we develop a PVDF-HFP-supported PDOL-based interlayer (PDOL/PVDF-HFP), which stabilizes the LGPS/Li interface by synergistically physically inhibiting and chemically scavenging lithium dendrites. The multifunctional feature of the interlayer comes from the use of a bifunctional initiator, InCl3. On the one hand, InCl3 induces the polymerization of DOL, forming a physical separator and protecting lithium from LGPS; on the other hand, in situ reactions between In3+/Cl– and Li form a LiCl/LiF/LiIn hybrid SEI, homogenizing the surface Li+ flux and suppressing lithium dendrite formation and penetration. In addition, an unexpected dynamic microdendrite scavenging is realized by virtue of the side reactions of LGPS/Li, which converts the undesirable reaction to be an advantage in our design. Benefiting from the comprehensive advantages of such design, the constructed sulfide-based solid-state batteries achieve a super low interfacial impedance of 5.1 Ω, a high critical current density (CCD) value over 5 mA/cm2, and a super long cycling stability over 8000 h. Our synergistic interlayer strategy would open an effective avenue for solving interfacial challenges for practical sulfide-based solid-state batteries.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.