Integration Plasma Strategy Controlled Interfacial Chemistry Regulation Enabling Planar Lithium Growth in Solid‐State Lithium Metal Batteries

Abstract

Solid‐state lithium metal batteries (SSLMBs) are identified as a highly promising candidate for next‐generation energy storage devices, yet they still face uncontrollable dendritic lithium (Li) growth originating from interfacial incompatibility. To address this issue, an “integration plasma (IP)” strategy for interlayer construction is proposed that integrates metal reduction and vapor deposition functions, featuring the ability to give a manipulable and quantifiable chemical regulation for controlling the surface concentration (Csurface) and the atomic ratio of the introduced metal element and electronegative element (ARE/M) on solid‐state electrolyte (SSE). This IP‐formed interlayer can in situ react with Li anode to synchronously produce metal‐Li alloy, Li salt and amorphous carbon, thus offering an “integrated function” to promote a spherical and hexagonal Li growth, preventing the dendrite propagation from SSE. When Csurface of metal elements and corresponding ARE/M is regulated as ≈1.13 nmol cm‐2 and ≈2.6, the IP‐modified SSE prolongs the lifespan of SSLMBs with LiNi0.8Co0.1Mn0.1O2 cathode to over 1000 cycles with a low‐capacity attenuation of 0.03% per cycle, highlighting the multiply functions of IP to accelerate the practical application of SSLMBs.

A Review on Engineering Design for Enhancing Interfacial Contact in Solid-State Lithium–Sulfur Batteries

“…Sun et al [38] reported an "integration plasma (IP)" strategy for constructing an interlayer layer between Li anode and SSE (Fig. 4a).…”

“…Moreover, the high mechanical stiffness of inorganic SSEs can significantly increase the stress/strain at the electrode/electrolyte interface and is inadequate to accommodate the volumetric expansion during cycling, thereby leading to high interfacial resistance [37]. Introducing a buffer/protective layer between the electrodes and the electrolytes is one of the effective strategies to enhance the physical contact and to regulate the Li/SSE interface [31,[38][39][40][41]. For instance, the deposition of ZnO layer on the surface of garnet-like Ta-doped LLZO via atomic layer deposition significantly improved the wettability of the garnet SSE to Li anode, resulting in a conformal contact without interfacial void space [42].…”

Development of plasma technology for the preparation and modification of energy storage materials

“…Shiyi Sun et al 88 proposed an “integration plasma (IP)“ strategy that combines the functionalities of metal reduction and gas-phase deposition. This strategy offers an operable and quantifiable chemical control to regulate the surface concentration and atomic ratio of metal and electronegative elements introduced onto the solid electrolyte.…”

Stabilizing the LAGP/Li interface and in situ visualizing the interfacial structure evolution for high-performance solid-state lithium metal batteries

“…1a), which hampers Li + transportation and fails to block the electron transfer. 19 The continuous growth of the SEI layer leads to uneven Li + /e − flux, resulting in increased interfacial resistance and local current density (hotpots). 20 The presence of hotspots and volume changes further exacerbates the interfacial chemistry, promoting the growth of lithium dendrites and ultimately causing cell short-circuiting.…”