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Deciphering Solid-State Battery Interface Failure: Plasma-Assisted Bulk-Interface Lithium Diffusion Kinetics Regulation
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DOI：10.1002/adfm.202521740.png)
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Abstract
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Interfacial-contact failure and void-evolution in garnet-based solid-state lithium-metal batteries (SSLMBs), caused by inadequate initial interface-bonding and limited lithium-ion diffusion at the anode, represent critical bottlenecks that need to be addressed to achieve the practical viability of SSLMBs. Here, a plasma-assisted dual-strategy is presented that integrates radio-frequency plasma-magnetron-sputtering (RF-PMS) and dielectric-barrier-discharge (DBD) plasma-treatment to construct an outstanding interface structure. Specifically, the composite-lithium-anode (CLA) doped with DBD plasma-functionalized carbon-nanotubes (D-CNT) is coated onto an AlF3-modified Li6.4La3Zr1.4Ta0.6O12 (AF-LLZTO) solid electrolyte synthesized using RF-PMS. The engineered LC10|AF-LLZTO interface (LC10: optimized CLA containing 10 wt.% D-CNT) facilitates a stable lithium-ion diffusion pathway, effectively mitigating interfacial-contact degradation. Following delithiation to 3.0 mAh cm−2, this configuration retains 85.16% interfacial-contact integrity—significantly surpassing the mere 10.49% retention observed in unmodified lithium-anodes. The enhanced interfacial-stability of this structure can be directly visualized through in situ optical-microscopy observation. The symmetric cell LC10|AF-LLZTO-AF|LC10 achieves 10000 h of stable cycling at 0.2 mA cm−2, significantly outperforming the symmetric cells Li|AF-LLZTO-AF|Li without CLA (1930 h) and LC10|LLZTO|LC10 without AlF3 (<900 h). Furthermore, a full cell LC10|AF-LLZTO-IL|NCM811 utilizing a LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode demonstrated ultra-long cycling stability, achieving a maximum of 2000 cycles at 1 C and exhibiting a single-cycle capacity degradation of ≈0.0125%.
Keywords:
composite-lithium-anode
dielectric-barrier-discharge
interface engineering
Plasma-magnetron-sputtering
solid-state Li metal battery
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19
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3.5W
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32.1W
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