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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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Stable Anode–Free All–Solid–State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector

A stable anode-free all-solid-state battery (AF-ASSB) with sulfide-based solid-electrolyte (SE) (argyrodite Li 6 PS 5 Cl) is achieved by tuning wetting of lithium metal on “empty” copper current-collector. Lithiophilic 1 µm Li 2 Te is synthesized by exposing the collector to tellurium vapor, followed by in situ Li activation during the first charge. The Li 2 Te significantly reduces the electrodeposition/electrodissolution overpotentials and improves Coulombic efficiency (CE). During continuous electrodeposition experiments using half-cells (1 mA cm –2 ), the accumulated thickness of electrodeposited Li on Li 2 Te–Cu is more than 70 µm, which is the thickness of the Li foil counter-electrode. Full AF-ASSB with NMC811 cathode delivers an initial CE of 83% at 0.2C, with a cycling CE above 99%. Additionally, cryogenic focused ion beam (Cryo-FIB) sectioning demonstrates uniform electrodeposited metal microstructure, with no signs of voids or dendrites at the collector-SE interface. Electrodissolution is uniform and complete, with Li 2 Te remaining structurally stable and adherent. By contrast, an unmodified Cu current-collector promotes inhomogeneous Li electrodeposition/electrodissolution, electrochemically inactive “dead metal,” dendrites that extend into SE, and thick non-uniform solid electrolyte interphase (SEI) interspersed with pores. Density functional theory (DFT) and mesoscale calculations provide complementary insight regarding nucleation-growth behavior. Unlike conventional liquid-electrolyte metal batteries, the role of current collector/support lithiophilicity has not been explored for emerging AF-ASSBs.

36 MATERIALS SCIENCE↗

Cathode–Sulfide Solid Electrolyte Interfacial Instability: Challenges and Solutions

All-solid-state batteries are a candidate for next-generation energy-storage devices due to potential improvements in energy density and safety compared to current battery technologies. Due to their high ionic conductivity and potential scalability through slurry processing routes, sulfide solid-state electrolytes are promising to replace traditional liquid electrolytes and enable All-solid-state batteries, but stability of cathode-sulfide solid-state electrolytes interfaces requires further improvement. Herein we review common issues encountered at cathode-sulfide SE interfaces and strategies to alleviate these issues.

25 ENERGY STORAGE↗

Fabricating Solid-State Batteries for Electric Aviation

All-solid-state lithium batteries are widely reputed as the next major step in energy storage technology on account their drastically improved safety over wet cells, as solid electrolytes lack the volatile compounds in wet electrolytes that make them combustible. This enhanced safety enables a far wider range of products and vehicles to go fully electric and aligns with future NASA missions that require high performing, reliable, and safe batteries. However, they currently face issues with implementation in consumer products due to the often-poor mechanical properties of the solid electrolyte and relative difficulty to manufacture. Typical solid-state electrolyte challenges were bypassed by incorporating a range of polymeric binders into a solid electrolyte suspension and cast onto a composite carbon-sulfide cathode to create a single bilayer film. The resulting films display superior flexibility and durability compared to solid-electrolyte films typically discussed in literature without compromising the thinness of the films. The bilayer film was then punched into 12.7 cm diameter discs and 4 cm by 5 cm sheets, pressed, and assembled into coin cells and pouch cells respectively.

Batteries↗

A Self-Healable Sulfide/Polymer Composite Electrolyte for Long-Life, Low-Lithium-Excess Lithium-Metal Batteries

Solid electrolyte-protected lithium-metal anodes promise energy-dense, safe cells. While sulfide solid electrolytes enable facile processability and fast ion transport, they suffer from complex chemo-mechanical issues, including Li plating-induced fracture and Li stripping-induced contact loss. To address these issues, a grafting approach is implemented to functionalize the sulfide solid electrolyte (Li 3,85 Sn 0.85 Sb 0.15 S 4 ) with a self-healing unit. This leads to a dynamic bonding between the solid electrolyte network and a mechanically robust polymer scaffold, which reversibly accommodates the volume changes of the lithium-metal anode. Thus, the approach improves the interfacial contact between the lithium-metal anode and the composite electrolyte, enabling stable cycling at a mild stack pressure (160 kPa). With a negative to positive capacity ratio equals to 1, pouch full cells with a high-nickel cathode (nickel content > 90%) and lithium-metal anode display 92% capacity retention for 140 cycles. Engineering the interface between solid electrolyte and the polymeric binder offers a promising pathway to address the chemo-mechanical issues.

36 MATERIALS SCIENCE↗

Pushing the Limits: Maximizing Energy Density in Silicon Sulfide Solid‐State Batteries

Here, for the first time, we demonstrate a silicon solid-state battery (SSB) architecture that achieves >400 Wh kg −1 , approaching the theoretical limit for silicon-based SSBs. This configuration features a 99.9 wt% micro-Si, a thin sulfide solid electrolyte (SSE), and a high-loading NMC811. Key to these results is strategically selecting and evaluating the processing techniques, whether wet or dry, for the negative electrode, positive electrode and thin sheet-type SSE. Excessive lithium incorporation into the silicon host, beyond the Li 3.75 +Si phase to form a LiSi composite, is essential to match the high capacity of the positive electrode. This SSB achieves over 1000 cycles for a 2 mAh cm −2 with ≈80% capacity retention and 94% capacity retention for 3 mAh cm −2 over 500 cycles at 25 °C. Post analysis identifies the primary capacity decay mechanisms as oxidation at the NMC/SSE interface and structural disruptions within NMC. Meanwhile, the Si electrode maintains a robust solid-electrolyte interphase layer, minimizing capacity decay. This study highlights the necessity for improved NMC coatings, lattice oxygen stabilization, and a durable positive electrode-electrolyte interface to improve the long-term stability of SSBs. Strategies leading to a single-layer pouch cell SSB exceeding 400 Wh kg −1 are developed.

25 ENERGY STORAGE↗

Current Status and Future Directions of All-Solid-State Batteries with Lithium Metal Anodes, Sulfide Electrolytes, and Layered Ternary Oxide Cathodes

All-solid-state batteries (ASSBs) offer great promise as a next-generation energy storage technology with higher energy density, wider operating temperature range, and improved safety for electric vehicles. ASSBs employing lithium metal anodes (Li), sulfide-based solid-state electrolytes (SSE), and Ni-rich layered transition metal oxide cathodes (LiMO 2 , M = Ni, Mn, Co, Al) are particularly promising due to its superior electrochemical performance compared to other solid-electrolyte systems. However, the battery cycle life at high cathode mass loading and high current is still limited because the failure mechanism is not fully understood. Lithium dendrite growth at the anode or inside a solid electrolyte still represents as a serious risk of cell failure. Interfacial resistance increases attributed to electrolyte decomposition and interfacial void formation at both cathode–electrolyte and anode–electrolyte interfaces lead to gradual capacity fading. In this Review, we present the fundamental challenges and recent scientific understandings of each component in ASSBs. The novel diagnostic tools for these components, especially the interfaces buried under the surface that are often hard for characterization are mainly examined. Lastly, we offer a perspective for future research directions. We hope this Review will provide a timely snapshot of state-of-the-art research progress in ASSBs to accelerate the development of ASSBs.

25 ENERGY STORAGE↗

Understanding Solid-Electrolyte Interphase Formation at the Lithium Metal Anode of Lithium-Sulfur Batteries

Lithium-sulfur (Li-S) batteries are one of the most promising chemistries for the next generation of energy storage devices. In a standard Li-S cell, the metallic lithium anode is an essential component of the battery due to its low density, extremely high theoretical specific capacity, and very low negative electrochemical potential. However, several challenges related to the use of Li metal have prevented this battery technology from becoming commercially available. For instance, Li-anodes are highly reactive, which results in the continuous decomposition of the electrolyte and the formation of the solid-electrolyte interphase (SEI) layer. This, combined with the non-uniform deposition of Liions during plating at the anode surface, can seriously affect the performance, cycling, and safety of the battery. In addition, it has been suggested that a controlled SEI formation at the metallic Li anode can yield enhanced battery performance. Hence, a comprehensive understanding of how the SEI layer is formed can help elucidate improvements in this battery technology. In this work, the formation of the SEI layer in Li-S batteries is investigated using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. The stability of liquid organic-based electrolyte components, salt concentration, electron-rich environments, and the use of inorganic solid-state electrolyte (SSE) materials are explored in order to provide molecular-level fundamental insights into how the nature and composition of the electrolyte can alter the initial stages of the SEI formation. The products of electrolyte decomposition and electro-/chemical reaction pathways of liquid electrolyte component such as solvent and salts are predicted from AIMD simulations of electrolyte-anode interfaces. Energetics of reactions from DFT ground-state optimizations are also presented to confirm the decomposition mechanisms. Some significant differences are then drawn regarding the use of low and high salt concentrations. Simulations under electron-rich environments show additional multielectron electrochemical reactions of solvent and salt decomposition taking place due to the excess of electrons and the presence of radical anions in the solution. Finally, the initial stages of formation, stability, and main constituents of interfaces between Li-metal and Sbased electrodes with sulfide-based SSEs are characterized in detail.

25 ENERGY STORAGE↗