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DOE OSTI2026

Deciphering the Conflict Between Ion and Electron Percolating Networks in Solid-State Battery Cathodes

High-energy- and power-density solid state batteries require an optimal cathode composition and microstructural arrangement of cathode active material, solid-state electrolyte, conductive carbon, and binder to simultaneously support lithium-ion transport, electron conduction, and storage capacity. The ion and electron conducting phases in solid-state cathodes counteract each other's percolating networks as their mass ratios increase or decrease relative to each other. Here, we investigate targeted mass ratio variations of argyrodite solid electrolyte and two different types of conductive carbon (particles and fibers) in composite LiNi0.8Mn0.1Co0.1O2 (NMC811) solid-state cathodes to ascertain the ionic-electronic tradeoffs in cathode performance. Through ionic and electronic conductivity measurements on composite cathodes, as well as rate-testing and cycling performance in full cells, it is shown that the conductive carbon fibers form a percolative electronic network within the composite at a lower mass ratio (3-5 wt%) than particulate carbon (>5 wt%). The threshold to achieve electronic percolation coincides with higher accessible capacity in the cathode as the active material particles become electronically connected. However, carbon loadings beyond this percolation threshold lead to increased ion transport resistance, arising from disruptions to ionic conduction pathways and degraded contact at the interface between the electrolyte and active materials. Imaging, spectroscopy, and physics-based models quantitatively describe the relationship between carbon and electrolyte compositions and the cell's capacity and rate performance through percolation theory. This work demonstrates the importance of quantitatively understanding percolating networks in solid-state cells and that strategic engineering of conductive carbon morphologies can further increase the energy- and power-density of solid-state cells.

25 ENERGY STORAGE↗

DOE OSTI2021

Metal alloy layers on substrates, methods of making same, and uses thereof

Metal alloy layers on substrates. The metal-alloy layers (e.g., lithium-metal layers, sodium-metal layers, and magnesium-metal layers) can be disposed on, for example, a solid-state electrolyte material. The metal-alloy layers can be used in, for example, solid-state batteries. A metal alloy layer can be an anode or part of an anode of a solid state battery.

Hu, Liangbing↗

NASA NTRSDate not supplied

Solid-state Architecture Batteries for Enhanced Rechargeability and Safety for Electric Aircraft

All electric vertical take-off and landing vehicles (eVTOL) for urban air mobility (UAM) concepts face numerous challenging technical barriers before their introduction into the consumer marketplace. The most challenging of these technical barriers to overcome is developing an energy storage system capable of meeting the rigorous aerospace safety and performance criteria. The performance metrics for eVTOL craft are at least 2 times greater than those of electric automobiles. Furthermore, safety is essential for operation of commercial electric aerovehicles. Preliminary systems level analysis has indicated that there are five key properties which must be optimized for successful implementation of battery systems. Those five key criteria are: safety, energy density, power, packaging design and scalability. Current state-of-the-art (SOA) lithium-ion batteries meet or exceed the requirements for electric aviation in the areas of power and scalability, yet are insufficient in the key performance criteria of energy, safety and packaging design. The SABERS concept proposes a battery that meets all five key performance criteria through development of a solid-state architecture battery utilizing high energy density and power density sulfur-selenium cathode with a lithium metal anode. The combination of sulfur and selenium offers a balanced energy-to-power density ratio, which can be tailored to the specific application by altering the stoichiometric ratios of sulfur to selenium. This cathode will be developed by implementing NASA patented holey graphene technology as a highly conductive, ultra-lightweight electrode scaffold. A solid-state electrolyte will be used as a safe, non-flammable replacement to the highly flammable liquid organic electrolytes currently used in SOA lithium-ion batteries. This solid-state lithium-sulfur-selenium cell will be designed into a serial stacking configuration to enable dense packaging of the battery cells. The serial stacking configuration is termed a bipolar stack, which has the advantages of reducing overall cell weight, reducing the amount of interfaced connections for the cell, and minimizing the cooling requirements for the cell. Lastly, optimization of battery components will occur through a robust and rigorous combination of various computational modeling techniques covering multiple length scales. The expected result will be a fully solid-state battery with operational temperatures from 0 °C to 150 °C which provides the required energy density, discharge rates, and inherent safety to meet the strict aerospace performance criteria. This presentation will show initial results that demonstrate the SABERS Team has developed a composite carbon-sulfur cathode which exceeds 1100 Wh/kg at a discharge rate of 0.4C, and 804 Wh/kg at a discharge rate of 1C. Additionally, this presentation will show the SABERS Team multiscale computational modeling approach and has produced a novel particle dynamics method called Solid Electrolyte Sphere Approximation Model (SESAM). SESAM is on the 1-10 µm scale and provides electromechanical and grain interactions for predictive design guidelines for the experimental team to follow.

Urban Air Mobility (UAM) Vehicles↗

NASA NTRSDate not supplied

Computational Modeling Development of Solid-state Architecture Batteries for Enhanced Rechargeability and Safety for Electric Aircraft

Urban Air Mobility (UAM) Vehicles↗

DOE OSTI2022

Solid Electrolytes in the Spotlight

This virtual issue is targeted to students and researchers, and highlights 32 research articles published over the past 5 years (from July 2016 to July 2021) in Chemistry of Materials (CM). Here, the compilation of papers summarizes the latest advances in the field of solid-state electrolytes for lithium (Li)-, sodium (Na)-, and multivalent-ion (not among the 32 articles discussed) all-solid-state batteries (ASSBs), with a focus on inorganic materials and excluding hybrid systems, e.g., polymer/ceramic composites or systems including liquid media. A total of 125 articles reporting exciting experimental and/or theoretical findings on solid electrolytes were considered for this issue. During 2017–2019, there were about 25–30 papers published per year on this topic, but 2020 and 2021 saw a significant increase, with 26 publications in the first half of 2021 alone. Submissions came from many countries around the world, as shown in Figure 1. While most papers were led by research groups located in the United States, Germany and Japan follow closely, and Austria, the United Kingdom, Canada, and China are also well represented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

The Key Role of Grain Boundary Dynamics in Revolutionizing the Potential of Solid Electrolytes

Solid electrolytes (SEs) have the potential to enhance the safety and performance of Li-metal batteries. However, the existence of grain boundaries in polycrystalline SEs presents a significant challenge for both ionic and electronic migration, promoting the propagation of detrimental lithium dendrites. This study compares the roles of grain boundaries in electrical properties of three distinct SEs including garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZO), argyrodite-type Li 6 PS 5 Cl (LPSC), and NASICON-type Li 1+x+y Al x (Ti,Ge) 2-x Si y P 3-y O 12 (LATP). Results demonstrate that the electronic and ionic conductivities of solid-state electrolytes are affected differently by grain boundaries, depending on the specific type of electrolyte. For instance, LLZO and LATP experience dielectric breakdown at 3.7 and 5.3 V, respectively, while LPSC does not exhibit such behavior. Here, a new chemical modification is proposed that simultaneously alters the composition of both the surface and grain boundaries of SEs, ultimately reducing electronic conductivity for the LLZO SEs. Consequently, the proposed LLZO exhibits unprecedented dendrite-free cycling stability, achieving a remarkable 12 000-h lifetime at room temperature, surpassing conventional strategies such as surface coatings in dendrite mitigation. This study highlights the significance of modifying grain boundaries to design safe and durable Li-metal batteries. It provides new insights for developing SEs that are highly resistant to dendrite formation.

36 MATERIALS SCIENCE↗

NASA NTRSDate not supplied

Design Considerations for Practical Li-S Battery Components for Electric Aviaiton

The development of high-energy, high-safety, and high-power batteries beyond electric automobile requirements is vital for future electric aviation applications. The transition to non-volatile solid-state electrolytes (SSE) promises many advantages over traditional flammable liquid electrolytes, and may also be an enabling technology for next generation chemistries. However, significant manufacturing challenges must be overcome before the adoption of such technology. Electrolytes developed in this study were produced as sulfide-polymer composites with densified thicknesses between 20-30 microns using a tape-casting technique and elastomer binder [1]. The composites were determined to retain reasonable ionic conductivity with improved flexibility and scalability critical for practical manufacturing of such cells. Films were produced 10-15 times thinner than comparable bulk powder electrolytes and within the range of commercial polyolefin separators (25 micron) used in commercial liquid containing lithium-ion cells. Composite conductivities were maintained above 0.2mS/cm, which holds promise for future electric aviation applications. Processing techniques are investigated to further improve electrochemical performance.

battery↗

NASA NTRSDate not supplied

Solid-state Architecture Batteries for Enhanced Rechargeability and Safety (SABERS) for Extended Deep Space Applications

Extended duration deep space missions as well as permanent space habitats face numerous technical challenges, key among them is energy generation and energy storage. There are considerable monetary and technical barriers to the generation of power in space. Therefore, it is important to store and be able to access power in an efficient and safe manner over a large number of cycles. Energy storage and in particular, batteries, are vital to the operation of next-generation extraterrestrial shuttles, rovers, habitats and extravehicular activity (EVA) space suits. The performance metrics for extended duration space missions are at least 2 times greater than those set for terrestrial applications such as electric automobiles. Furthermore, safety is essential for operation of space missions particularly involving astronauts such as shuttles, habitats and EVA space suits. Preliminary systems level analysis has indicated that there are five key properties which must be optimized for successful implementation of battery systems. Those five key criteria are: safety, energy density, power, packaging design and scalability. Current state-of-the-art (SOA) lithium-ion batteries can meet or exceed the requirements for certain space applications in the areas of power and scalability, yet are insufficient in the key performance criteria of energy, safety and packaging design. The SABERS concept proposes a battery that meets all five key performance criteria through development of a solid-state architecture battery utilizing high capacity sulfur-selenium cathode and lithium metal anode. The combination of sulfur and selenium offers a balanced energy-to-power density ratio, which can be tailored to the specific application by altering the stoichiometric ratios of sulfur to selenium. This hybrid cathode will be developed by implementing NASA patented holey graphene technology as a highly conductive, ultra-lightweight electrode scaffold. A solid-state electrolyte will be used as a safe, non-flammable replacement to the highly flammable liquid organic electrolytes currently used in SOA lithium-ion batteries. This solid-state lithium-sulfur/selenium cell will be designed into a serial stacking configuration to enable dense packaging of the battery cells. The serial stacking configuration is termed a bipolar stack, which has the advantages of reducing overall cell weight, simplifying the interfaced connections for the cell, and minimizing the cooling requirements for the cell. Lastly, optimization of battery components will occur through a robust and rigorous combination of various computational modeling techniques covering multiple length scales. The expected result will be a fully solid-state battery with operational temperatures up to 150 °C which provides the required energy density, discharge rates, and inherent safety to meet the strict space mission performance criteria. In particular, the wide operational temperature window is required for the large temperature ranges which are experienced across a broad range of potential space missions. This presentation will show initial results that demonstrate the SABERS team has developed a composite carbon-sulfur cathode which exceeds 1100 Wh/kg at a discharge rate of 0.4C, and 804 Wh/kg at a discharge rate of 1C. Additionally, this presentation will show the SABERS team multiscale computational modeling approach and has produced a novel particle dynamics method called Solid Electrolyte Sphere Approximation Model (SESAM). SESAM is on the 1-10 µm scale and provides electromechanical and grain interactions for predictive design guidelines for the experimental team to follow.

Urban Air Mobility (UAM) Vehicles↗

DOE OSTI2025

Tetrahedral Tilting and Lithium‐Ion Transport in Halide Argyrodites Prepared by Rapid, Microwave‐Assisted Synthesis

Abstract This study demonstrates a rapid, dry, microwave‐assisted (MW) synthesis method that enables preparation of halide argyrodites ( , , ) in less than 20 min. The structures and ion transport properties of the resulting materials are compared with those synthesized by conventional solid‐state synthesis methods. The microwave‐assisted method leads to increased site disorder and elevated Arrhenius prefactors (), which lead to an order of magnitude improvement in the 30 ionic conductivity of MW‐. X‐ray pair distribution function analysis (XPDF) reveals significant rotational disorder of the units, which is impacted by the synthesis method, choice of halide, and presence of / site disorder. These rotational displacements are strongly correlated with ion transport, specifically and entropy of migration (). Overall, this study demonstrates a rapid synthesis route for preparing high‐quality halide argyrodite solid‐state electrolytes in less than 20 min, and further unravels atomistic insights into the interplay of structural disorder, rotational dynamics, and ion transport mechanisms.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Enabling High-Performance NASICON-Based Solid-State Lithium Metal Batteries Towards Practical Conditions

Solid-state lithium metal batteries (SSLMBs) are promising next-generation high-energy rechargeable batteries. However, the practical energy densities of the reported SSLMBs have been significantly overstated due to the use of thick solid-state electrolytes, thick lithium (Li) anodes, and thin cathodes. Here, a high-performance NASICON-based SSLMB using a thin (60 µm) Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) electrolyte, ultrathin (36 µm) Li metal, and high-loading (8 mg cm -2 ) LiFePO 4 (LFP) cathode is reported. The thin and dense LAGP electrolyte prepared by hot-pressing exhibits a high Li ionic conductivity of 1 × 10 -3 S cm -1 at 80 °C. The assembled SSLMB can thus deliver an increased areal capacity of ≈1 mAh cm -2 at C/5 with a high capacity retention of ≈96% after 50 cycles under 80 °C. Furthermore, it is revealed by synchrotron X-ray absorption spectroscopy and in situ high-energy X-ray diffraction that the side reactions between LAGP electrolyte and LFP cathode are significantly suppressed, while rational surface protection is required for Ni-rich layered cathodes. This study provides valuable insights and guidelines for the development of high-energy SSLMBs towards practical conditions.

25 ENERGY STORAGE↗

DOE OSTI2023

Unveiling the Mechanical and Electrochemical Evolution of Nanosilicon Composite Anodes in Sulfide-Based All-Solid-State Batteries

The utilization of silicon anodes in all-solid-state lithium batteries provides good prospects for facilitating high energy density. However, the compatibility of sulfide solid-state electrolytes (SEs) with Si and carbon is often questioned due to potential decomposition. Here, in this paper, operando X-ray absorption near-edge structure (XANES) spectroscopy, ex situ scanning electron microscopy (SEM), and ex situ X-ray nanotomography (XnT) are utilized to investigate the chemistry and structure evolution of nano-Si composite anodes. Results from XANES demonstrate a partial decomposition of SEs during the first lithiation stage, which is intensified by the presence of carbon. Nevertheless, the performances of first three cycles in Si–SE–C are stable, which proves that the generated media is ionically conductive. XnT and SEM results show that the addition of SEs and carbon improves the structural stability of the anode, with fewer pores and voids. A chemo-elasto-plastic model reveals that SEs and carbon buffer the volume expansion of Si, thus enhancing mechanical stability. The balance between the pros and cons of SEs and carbon in enhancing reaction kinetics and structural stability enables the Si composite anode to demonstrate the highest Si utilization with higher specific capacities and a better rate than pure Si and Si composite anodes with only SEs.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Operando EDXRD Study of All;#8208;Solid;#8208;State Lithium Batteries Coupling Thioantimonate Superi

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Sun, Xiao↗

DOE OSTI2024

Surface Engineering Strategy to Synthesize Bicomponent Carbons for Rechargeable Zinc-Air Batteries

Atomic Fe-N x moieties and nanosized FeCo species anchored on carbons have each been demonstrated to be among the most effective active components for oxygen reduction and evolution reactions (ORR/OER), respectively in rechargeable zinc -air batteries (ZABs). However, incorporating both of these components in a single catalyst presents a great challenge due to the trade-off in formation between them during hightemperature preparation. Herein, we integrate them into a bicomponent carbon through a surface engineering strategy. In this process, K 3 [Fe(CN) 6 ] is engineered on the surface of a precursor mixture consisting of polyaniline-coated graphene oxide and ZIF-67. This is followed by pyrolysis to produce the bicomponent carbon catalyst of FeCo nanoparticles modified carbon polyhedron (for accelerating the OER), supported on atomically dispersed Fe -N -doped carbon nanosheet (for boosting the ORR). The catalyst exhibits a small potential gap of 0.69 V for OER/ORR. In situ Raman spectroscopy demonstrates that spinel FeCo oxides may be responsible for OER. The use of this catalyst in ZABs achieves high power densities of 225 mW cm -2 in aqueous electrolyte and 164 mW cm -2 in solid-state electrolyte. Additionally, a small and stable voltage gap of 0.712 V at 10 mA cm -2 is maintained after 1035 discharge -charge cycles demonstrating the great application potential in energy devices.

An, Jia-Xing↗

DOE OSTI2024

Suppressing Atmospheric Degradation of Sulfide-Based Solid Electrolytes via Ultrathin Metal Oxide Layers

Sulfide-based solid-state electrolytes (SSEs) are promising materials with superior Li-ion conductivity; however, their poor atmospheric stability limits commercial manufacturing at scale. Here, we investigate the impact of ultrathin metal oxide layers deposited via atomic layer deposition (ALD) on the stability of Li 6 PS 5 Cl (LPSCl). Al 2 O 3 layers grown directly on LPSCl particles significantly stabilize the surface chemistry and Li-ion transport properties relative to uncoated material upon exposure to both an ambient atmosphere (22% relative humidity, RH) and humidified O 2 (100% RH). Detailed investigations indicate that coatings impede the surface and bulk degradation kinetics of exposed materials, even for coatings as thin as ∼1 Å. Furthermore, this suggests that stabilization is due to more than just a physical barrier. Shifts in valence band edge positions of coated LPSCl indicate that ALD coatings alter the surface electronic structure and resulting oxidation tendency of underlying LPSCl, suggesting new avenues to improving the environmental stability of sulfide SSEs.

Atmospheric chemistry↗

DOE OSTI2024

Solid-state polymer-particle hybrid electrolytes: Structure and electrochemical properties

Solid-state electrolytes (SSEs) are challenged by complex interfacial chemistry and poor ion transport through the interfaces they form with battery electrodes. Here, we investigate a class of SSE composed of micrometer-sized lithium oxide (Li 2 O) particles dispersed in a polymerizable 1,3-dioxolane (DOL) liquid. Ring-opening polymerization (ROP) of the DOL by Lewis acid salts inside a battery cell produces polymer-inorganic hybrid electrolytes with gradient properties on both the particle and battery cell length scales. These electrolytes sustain stable charge-discharge behavior in Li||NCM811 and anode-free Cu||NCM811 electrochemical cells. On the particle length scale, Li 2 O retards ROP, facilitating efficient ion transport in a fluid-like region near the particle surface. On battery cell length scales, gravity-assisted settling creates physical and electrochemical gradients in the hybrid electrolytes. By means of electrochemical and spectroscopic analyses, we find that Li 2 O particles participate in a reversible redox reaction that increases the effective CE in anode-free cells to values approaching 100%, enhancing battery cycle life.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2020

Solid-state Architecture Batteries for Enhanced Rechargeability and Safety (SABERS)

All-electric vertical take-off and landing vehicles (eVTOL) for urban air mobility (UAM) concepts face numerous challenging technical barriers before their introduction into the consumer marketplace. The most challenging of these technical barriers to overcome is developing an energy storage system capable of meeting the rigorous aerospace safety and performance criteria. The performance metrics for eVTOL craft, such as specific energy and cycle life, are at least 2 times greater than those of electric automobiles. Furthermore, safety is essential for operation of commercial electric aerovehicles. Preliminary systems level analysis studies have indicated that there are five key properties which must be optimized for successful implementation of battery systems. Those five key criteria are safety, energy density, power, packaging design and scalability. Current state-of-the-art (SOA) lithium-ion batteries meet or exceed the requirements for electric aviation in the areas of power and scalability, yet are insufficient in the key performance criteria of energy, safety and packaging design. The SABERS concept proposes a battery that meets all five key performance criteria through the development of a solid-state architecture cell design utilizing high energy density and power density sulfur-selenium cathode with a lithium metal anode. Data will be presented demonstrating high performing sulfur - selenium cathode that offers a balanced energy to power density ratio, which can be tailored to the specific application by altering the stoichiometric ratios of sulfur to selenium. This cathode is being developed by implementing NASA patented holey graphene technology as a highly conductive, ultra-lightweight electrode scaffold. Novel processing methods allow developing solid-state electrolyte that is a safe, non-flammable replacement to the highly flammable liquid organic electrolytes currently used in SOA lithium-ion batteries. The all solid-state lithium-sulfur-selenium cell design enables the implementation of a bipolar stack configuration, which has the advantages of reducing overall cell weight, reducing the amount of interfaced connections for the cell, and minimizing cooling requirements for the battery. In particular, the solid-state design allows for a serial stacking configuration to enable dense packaging of the cells within the bipolar stack. Lastly, optimization of battery components occurs through a robust and rigorous combination of various computational modeling techniques covering multiple length scales. The expected result will be a solid-state battery with operational temperatures from 0 °C to 150 °C which provides the required energy density, discharge rate, and inherent safety to meet strict aerospace performance criteria.

solid state batteries↗

DOE OSTI2025

Understanding the Cathode Electrochemistry of Humidified Solid‐State Lithium‐Oxygen Batteries

Lithium-oxygen batteries (LOBs) possess a high theoretical energy density, making them potential candidates for next-generation energy storage. However, challenges such as reactive oxygen species-induced component degradation hinder their practical use. Inorganic solid-state electrolytes offer an alternative to degradation-prone aprotic electrolytes, while also protecting lithium anodes from potential atmospheric reactants. Here, this study explores the cathode electrochemistry of solid-state LOBs using humidified oxygen, which forms an aqueous catholyte during initial cycling, thereby improving cathode-electrolyte contact. To quantitatively analyze the cathode electrochemistry, a ‘Humidity-Incorporated’ Differential Electrochemical Gas Monitoring System (HiDEMS) is developed to control humidity and monitor gas consumption and evolution in real time. When studying a Li-O 2 cell that employs a NASICON-type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) solid electrolyte and a porous carbon cathode, a shift in discharge products from Li 2 O 2 to LiOH is observed over repeated cycles. While Li 2 O 2 evolves O 2 during charging, LiOH oxidation leads to minimal O 2 release and increased CO 2 production, originating from oxidation of carbon electrodes. Further, dissolution of Al and P from LATP is observed, likely driven by the formation of the alkaline catholyte. The findings highlight the need for carbon-free cathode materials and more stable solid-state conductors to minimize side reactions and improve rechargeability in humidified solid-state Li-O 2 batteries.

LATP degradation↗

DOE OSTI2020

Towards a high-performance garnet-based solid-state Li metal battery: A perspective on recent advances

Garnet-based solid-state Li metal batteries have been widely considered one of the most promising next-generation energy storage systems. However, the performance of these batteries is plagued by various limitations caused by the solid-state electrolyte (SSE). The poor wetting of lithium on the garnet surface diminishes the contact between the anode and electrolyte, leading to extremely high anode interfacial resistance. Similarly, the point-to-point contact between the cathode and electrolyte leads to high impedance on the cathode side. Moreover, although the SSE serves a firm barrier separating the anode and cathode, lithium dendrites can still grow through, causing a short circuit. Lastly, the solid/solid interface cannot be well maintained under cycling at high current density and capacity. Recently, remarkable progress has been achieved in garnet electrolyte to resolve these problems towards the aim of a high-performance solid-state Li metal battery. In this perspective, we highlight various recent advances in the field of garnet-based solid-state battery, including improving the anode/electrolyte interface, lithium dendrite detection, reducing cathode impedance, and electrolyte architecture design.

25 ENERGY STORAGE↗