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1. The interplay between solid electrolyte interface (SEI) and dendritic lithium growth

   Wu, Bingbin; Lochala, Joshua; Taverne, Tyler; Xiao, Jie (August 2017, Nano energy)

   Li dendrite formed in Li metal batteries can be categorized into two different types. One is the detrimental Li dendrite that heads towards the separator with a potential to short cell. The other is the ill-defined fibrous Li formed within bulk Li metal. The detrimental Li dendrite may cause cell short, while the other dendrites, covered by SEI, mainly increase cell impedance and terminate the cell operation, most often, before any “short” really happens. Without decoupling these two different Li dendrites, it is hard to develop any effective approach to realize both stable and safe Li metal batteries. Herein, a straightforward approach is proposed to induce the growth of detrimental dendritic Li so the cells are “shorted” frequently and consistently. Based on this new protocol, various electrolytes are revisited and the SEI derived are compared and quantified, providing new insights for addressing the challenges in rechargeable Li metal battery technologies. 

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2. The role of the solid electrolyte interphase layer in preventing Li dendrite growth in solid-state batteries

   https://doi.org/10.1039/c8ee00540k  

   Wu, Bingbin; Wang, Shanyu; Lochala, Joshua; Desrochers, David; Liu, Bo; Zhang, Wenqing; Yang, Jihui; Xiao, Jie (January 2018, Energy & Environmental Science)

   Lithium (Li) metal anodes have regained intensive interest in recent years due to the ever-increasing demand for next-generation high energy battery technologies. Li metal, unfortunately, suffers from poor cycling stability and low efficiency as well as from the formation of dangerous Li dendrites, raising safety concerns. Utilizing solid-state electrolytes (SSEs) to prevent Li dendrite growth provides a promising approach to tackle the challenge. However, recent studies indicate that Li dendrites easily form at high current densities, which calls for full investigation of the fundamental mechanisms of Li dendrite formation within SSEs. Herein, the origin and evolution of Li dendrite growth through SSEs have been studied and compared by using Li 6.1 Ga 0.3 La 3 Zr 2 O 12 (LLZO) and NASICON-type Li 2 O–Al 2 O 3 –P 2 O 5 –TiO 2 –GeO 2 (LATP) pellets as the separators. We discover that a solid electrolyte interphase (SEI)-like interfacial layer between Li and SSE plays a critical role in alleviating the growth of dendritic Li, providing new insights into the interface between SSE and Li metal to enable future all solid-state batteries. 

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3. High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

   https://doi.org/10.1073/pnas.1907507116  

   Xu, Henghui; Chien, Po-Hsiu; Shi, Jianjian; Li, Yutao; Wu, Nan; Liu, Yuanyue; Hu, Yan-Yan; Goodenough, John B. (September 2019, Proceedings of the National Academy of Sciences)

   Flexible and low-cost poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state Li-metal batteries because of their compatibility with a metallic lithium anode. However, the low room-temperature Li-ion conductivity of PEO solid electrolytes and severe lithium-dendrite growth limit their application in high-energy Li-metal batteries. Here we prepared a PEO/perovskite Li 3/8 Sr 7/16 Ta 3/4 Zr 1/4 O 3 composite electrolyte with a Li-ion conductivity of 5.4 × 10 −5 and 3.5 × 10 −4 S cm −1 at 25 and 45 °C, respectively; the strong interaction between the F − of TFSI − (bis-trifluoromethanesulfonimide) and the surface Ta 5+ of the perovskite improves the Li-ion transport at the PEO/perovskite interface. A symmetric Li/composite electrolyte/Li cell shows an excellent cyclability at a high current density up to 0.6 mA cm −2 . A solid electrolyte interphase layer formed in situ between the metallic lithium anode and the composite electrolyte suppresses lithium-dendrite formation and growth. All-solid-state Li|LiFePO 4 and high-voltage Li|LiNi 0.8 Mn 0.1 Co 0.1 O 2 batteries with the composite electrolyte have an impressive performance with high Coulombic efficiencies, small overpotentials, and good cycling stability. 

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4. The Linkage Between Electro-Chemical Mechanical Instabilities in Battery Materials

   https://doi.org/10.1007/s11837-023-06280-w  

   Wable, Minal; Marckx, Bret; Çapraz, Ömer Özgür (November 2023, JOM)

   The battery chemistry must be diversified to achieve a sustainable energy landscape by effectively utilizing renewable energy sources. Alkali metal-ion, all-solid-state, metal-air batteries, and multivalent batteries offer unique cost, safety, raw material abundance, energy, and power density solutions. However, realizing these “Beyond Li-ion batteries” must uncover their working principles and performance & property relationship. In this aspect, mitigating chemo-mechanical instabilities in the structure and surface of the electrodes plays a crucial role in their performance. Unfortunately, the coupling between electrochemical and mechanical interactions is often poorly understood due to a lack of operando characterization. This review article explains the working principles of curvature measurement and digital image correlation for measuring stress and strain generations in battery materials. We provided specific examples of how these operando mechanical measurements shed light on instabilities in alkali-metal ion electrodes, solid electrolytes, Li-O2 batteries, and aqueous Zn-ion batteries. Operando mechanical measurements offer an effective way to map changes in the physical fingerprint of the battery materials, therefore providing crucial information to elucidate instabilities in battery materials. 

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5. Modeling the chemo-mechanical behavior of all-solid-state batteries: a review.

   https://doi.org/10.1007/s11012-020-01209-y  

   Bistri, Donald; Afshar, Arman; Di Leo, Claudio V. (July 2020, Meccanica)

   Solid-state-batteries (SSBs) present a promising technology for next-generation batteries due to their superior properties including increased energy density, wider electrochemical window and safer electrolyte design. Commercialization of SSBs, however, will depend on the resolution of a number of critical chemical and mechanical stability issues. The resolution of these issues will in turn depend heavily on our ability to accurately model these systems such that appropriate material selection, microstructure design, and operational parameters may be determined. In this article we review the current state-of-the art modeling tools with a focus on chemo-mechanics. Some of the key chemo-mechanical problems in SSBs involve dendrite growth through the solid-state electrolyte (SSE), interphase formation at the anode/SSE interface, and damage/decohesion of the various phases in the solid-state composite cathode. These mechanical processes in turn lead to capacity fade, impedance increase, and short-circuit of the battery, ultimately compromising safety and reliability. The article is divided into the three natural components of an all-solid-state architecture. First, modeling efforts pertaining to Li-metal anodes and dendrite initiation and growth mechanisms are reviewed, making the transition from traditional liquid electrolyte anodes to next generation all-solid-state anodes. Second, chemo-mechanics modeling of the SSE is reviewed with a particular focus on the formation of a thermodynamically unstable interphase layer at the anode/SSE interface. Finally, we conclude with a review of chemo-mechanics modeling efforts for solid-state composite cathodes. For each of these critical areas in a SSB we conclude by highlighting the key open areas for future research as it pertains to modeling the chemo-mechanical behavior of these systems. 

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