Silicon anode solid-state batteries Research on solid-state batteries has focused on lithium metal anodes. Alloy-based anodes have received less attention in part due to their lower specific capacity even though they should be safer. Tan et al . developed a slurry-based approach to create films from micrometer-scale silicon particles that can be used in anodes with carbon binders. When incorporated into solid-state batteries, they showed good performance across a range of temperatures and excellent cycle life in full cells. —MSL

All-solid-state batteries are expected to enable batteries with high energy density with the use of lithium metal anodes. Although solid electrolytes are believed to be mechanically strong enough to prevent lithium dendrites from propagating, various reports today still show cell failure due to lithium dendritic growth at room temperature. While cell parameters such as current density, electrolyte porosity and interfacial properties have been investigated, mechanical properties of lithium metal and the role of applied stack pressure on the shorting behavior is still poorly understood. Here, we investigated failure mechanisms of lithium metal in all-solid-state batteries as a function of stack pressure, and conducted in situ characterization of the interfacial and morphological properties of the buried lithium in solid electrolytes. We found that a low stack pressure of 5 MPa allows reliable plating and stripping in a lithium symmetric cell for more than 1000 hours, and a Li | Li6PS5Cl | LiNi0.80Co0.15Al0.05O2 full cell, plating more than 4 µm of lithium per charge, is able to cycle over 200 cycles at room temperature. These results suggest the possibility of enabling the lithium metal anode in all-solid-state batteries at reasonable stack pressures.

Sulfide-based solid electrolytes are promising candidates for all solid-state batteries (ASSBs) due to their high ionic conductivity and ease of processability. However, their narrow electrochemical stability window causes undesirable electrolyte decomposition. Existing literature on Li-ion ASSBs report an irreversible nature of such decompositions, while Li–S ASSBs show evidence of some reversibility. Here, we explain these observations by investigating the redox mechanism of argyrodite Li6PS5Cl at various chemical potentials. We found that Li–In | Li6PS5Cl | Li6PS5Cl–C half-cells can be cycled reversibly, delivering capacities of 965 mAh g–1 for the electrolyte itself. During charging, Li6PS5Cl forms oxidized products of sulfur (S) and phosphorus pentasulfide (P2S5), while during discharge, these products are first reduced to a Li3PS4 intermediate before forming lithium sulfide (Li2S) and lithium phosphide (Li3P). Finally, we quantified the relative contributions of the products toward cell impedance and proposed a strategy to reduce electrolyte decomposition and increase cell Coulombic efficiency.

circumvent flammability concerns of liquid electrolytes. However, enhancing energy densities by thinning SSE layers and enabling scalable coating processes remain challenging. While previous studies have addressed thin and flexible SSEs, mainly ionic conductivity was considered for performance evaluation, and no systematic research on the effects of manufacturing conditions on the quality of SSE films was performed. Here, both uniformity and ionic conductivity are considered for evaluating the SSE films under the guidance of machine learning (ML). Three algorithms, principal component analysis, K-means clustering, and support vector machine, are employed to decipher the interdependencies between manufacturing conditions and film performance. Guided by ML, a 40 μm SSE film with high ionic conductivity and good uniformity is used to construct a LiNi 0.8 Co 0.1 Mn 0.1 O 2 || Li 6 PS 5 Cl || LiIn cell demonstrating 100 cycles. This study presents an efficient ML-assisted approach to optimize scalable production of high-quality SSE films.

All-solid-state batteries (ASSBs) are viewed as promising next-generation energy storage devices, due to their enhanced safety by replacing organic liquid electrolytes with non-flammable solid-state electrolytes (SSEs). The high ionic conductivity...

Abstract

One approach to increase the energy density of all-solid-state batteries (ASSBs) is to use high-voltage cathode materials. The spinel LiNi0.5Mn1.5O4 (LNMO) cathode is one such example, as it offers a high reaction potential (close to 5 V). Moreover, it is a Co-free cathode system, which makes it an environmentally friendly and a low-cost alternative. However, several challenges must be addressed before it can be properly adopted in ASSB technologies. Herein, we reveal that lithium argyrodite (Li6PS5Cl), a sulfide solid-state electrolyte (SSE), possesses intrinsic chemical incompatibility with the LNMO cathode. We demonstrate the necessity of using a halide SSE, Li3YCl6 (LYC), through careful analysis of the LNMO/SSE interface. Moreover, we emphasize the necessity of applying a protective coating layer to LNMO particles, even when halide SSEs are used. Furthermore, the chemical phenomena involving LYC in the oxidative environment of LNMO are analyzed, including a comparison between coated and uncoated LNMO particles.

No abstract