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Sulfide solid electrolytes (SEs) show promise for Li metal solid-state batteries due to their high ionic conductivities and relative ease of manufacturing. However, many sulfide SEs suffer from limited electrochemical stability against Li metal electrodes. In this work, we use a suite ofoperandoanalytical techniques to investigate the dynamics of solid electrolyte interphase (SEI) formation and the associated effects on Li plating. We contrast a sulfide SE that forms an electrically insulating SEI (Li₆PS₅Cl) with an SE that forms an SEI with electrically conducting phases present (Li₁₀GeP₂S₁₂). Using anode-free cell configurations, where the Li/SE interface is formed against a current collector, we perform complimentaryoperandovideo microscopy andoperandoX-ray photoelectron spectroscopy (XPS) experiments. The combination of these techniques allows for the interpretation of electrochemical voltage traces during Li plating. The electrically insulating nature of the SEI in Li₆PS₅Cl facilitates Li metal nucleation and plating after the initial SEI formation. In contrast, in cells that form an electronically conducting SEI, the onset of Li plating is suppressed, which is attributed to a low Faradaic efficiency from continuous SE decomposition. The insights in this study reveal how interphase dynamics control the transition from SEI formation to plating in anode-free solid-state batteries.

 

Along with the increasing interest in MoS 2 as a promising electronic material, there is also an increasing demand for nanofabrication technologies that are compatible with this material and other relevant layered materials. In addition, the development of scalable nanofabrication approaches capable of directly producing MoS 2 device arrays is an imperative task to speed up the design and commercialize various functional MoS 2 -based devices. The desired fabrication methods need to meet two critical requirements. First, they should minimize the involvement of resist-based lithography and plasma etching processes, which introduce unremovable contaminations to MoS 2 structures. Second, they should be able to produce MoS 2 structures with in-plane or out-of-plane edges in a controlled way, which is key to increase the usability of MoS 2 for various device applications. Here, we introduce an inkjet-defined site-selective (IDSS) method that meets these requirements. IDSS includes two main steps: (i) inkjet printing of microscale liquid droplets that define the designated sites for MoS 2 growth, and (ii) site-selective growth of MoS 2 at droplet-defined sites. Moreover, IDSS is capable of generating MoS 2 with different structures. Specifically, an IDSS process using deionized (DI) water droplets mainly produces in-plane MoS 2 features, whereas the processes using graphene ink droplets mainly produce out-of-plane MoS 2 features rich in exposed edges. Using out-of-plane MoS 2 structures, we have demonstrated the fabrication of miniaturized on-chip lithium ion batteries, which exhibit reversible lithiation/delithiation capacity. This IDSS method could be further expanded as a scalable and reliable nanomanufacturing method for generating miniaturized on-chip energy storage devices.