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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Electrochemical Ammonia Compression

An electrochemical (EC) compressor is a solid-state compression device. For decades, researchers have been studying EC compressors for applications for a variety of energy systems. As the world transitions away from fossil fuel energy sources, EC compression emerges as a promising technique for energy storage, specifically energy stored in the form of pressurized ammonia. Ammonia is also a commonly used refrigerant. The present studies examine the viability of EC compression for ammonia storage and refrigeration. EC ammonia compression increases the concentration of an ammonia-hydrogen mixture via the input of electrical energy and a series of chemical reactions. A polymer electrolyte membrane separates the low-concentration side from the high-concentration side of the device. On the low-pressure (anode) side hydrogen atoms oxidize and react with ammonia molecules, forming positively charge ammonium ions. The ions traverse the membrane electrolytically. The ammonium ions are reduced and revert back to hydrogen and ammonia upon reaching the high-pressure (cathode). An external circuit provides the current needed to sustain the reactions. In this project, we studied the performance of the ammonia EC compressor under a variety of different conditions. We replicated preliminary data and using a small cell with 5 cm2 of active area. We demonstrated the operation of larger cells with 100 cm2 of active area. Further, we used a commercially available hydrogen EC compressor stack to analyze the scaled-up compressor performance. While previous experiments examined only the transient EC compressor performance, we developed test facilities that allowed the compressor to reach steady state. We analyzed the effects of pressure and current on the EC compressor performance. We measured the flow rates of gas leaving the compressors and analyzed the composition using gas chromatography. We tested methods of separating ammonia from the effluent vapor, which contained hydrogen and water vapor. We found that back diffusion adversely affected the performance, especially when we maintained high pressure lifts.

25 ENERGY STORAGE↗
DOE OSTI2021

Material Design Strategy for Halide Solid Electrolytes Li 3 MX 6 (X = Cl, Br, and I) for All-Solid-State High-Voltage Li-Ion Batteries

Although several solid electrolyte (SE) candidates have been explored, achieving the necessary combination of performance, stability, and processability has been challenging. Recently, several lithium ternary halides have attracted increasing attention for SEs because of their favorable combination of high ionic conductivity and wide electrochemical window. This study aims to provide a material design strategy for lithium halides Li 3 MX 6 (X = Cl, Br, and I) for high-voltage all-solid-state Li-ion batteries, achieved by the systematic investigation of crystal structures, phase and electrochemical stabilities, electronic and mechanical properties, and ionic conductivities. Calculation results reveal that the electronegativity difference between M and X affects structural properties and stabilities. Weak Coulomb interactions in Li 3 MX 6 result in the preference of the monoclinic phase, and the oxidation potential and chemical stability against the cathode materials of Li 3 MX 6 increase for relatively small X. Chlorides exhibit the highest oxidation potential (~4.3 V) among Li 3 MX 6 , suggesting that chlorides are appropriate SEs for high-voltage cathodes. The band gap and elastic moduli increase for relatively small X, suggesting the relatively low electronic conductivity and elastic deformability of chlorides. Chlorides with transition metals typically exhibit trigonal phases, a wider electrochemical stability window, a larger band gap, and higher elastic moduli compared to other types of halides. Additionally, chloride Li 3 MCl 6 is expected to have relatively high ionic conductivities with the aliovalent substitution of M 3+ to Zr 4+ and the anion mixing of Cl with Br. The findings of this study will provide fundamental guidelines for the development of lithium halide SEs for high-voltage all-solid-state Li-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Tutorial review on structure – dendrite growth relations in metal battery anode supports

This tutorial review explains the emerging understanding of the surface and bulk chemistry – electrochemical performance relations in anode supports (aka secondary current collectors, substrates, templates, hosts) for lithium, sodium and potassium metal batteries (LMBs, SMBs or NMBs, and KMBs or PMBs). In relation to each section, the possible future research directions that may yield both new insight and improved cycling behavior are explored. Representative case studies from Li, Na and K metal anode literature are discussed. The tutorial starts with an overview of the solid electrolyte interphase (SEI), covering both the “classic” understanding of the SEI structure and the “modern” insights obtained by site-specific cryogenic stage TEM analysis. Next, the multiple roles of supports in promoting cycling stability are detailed. Without an optimized support architecture, the metal–electrolyte interface becomes geometrically unstable at a lower current density and cycle number. Taking into consideration the available literature on LMBs, SMBs and KMBs, it is concluded that effective architectures are geometrically complex and electrochemically lithiophilic, sodiophilic or potassiophilic, so as to promote conformal electrochemical wetting of the metal during plating/stripping. One way that philicity is achieved is through support oxygen surface chemistry, which yields a reversibly reactive metal–support interface. Examples of this include the well-known oxygen–carbon moieties in reduced graphene oxide (rGO), as well as classic ion battery reversible conversion reaction oxides such as SnO 2 . Unreactive surfaces lead to dewetted island growth of the metal, which is a precursor to dendrites, and possibly to non-uniform dissolution. Surveying the literature on various Li, Na and K metal supports, it is concluded that the key bulk thermodynamic property that will predict electrochemical wetting behavior is the enthalpy of infinite solution (Δ sol H ∞ ) of the metal (solute) into the support (solvent). Large and negative Δ sol H ∞ promotes uniform metal wetting on the support surface, corresponding to relatively low plating overpotential. Positive Δ sol H ∞ promotes dewetted islands and a relatively high overpotential. This simple rule explains a broad range of studies on Li, Na and K metal – support interactions, including the previously reported correlation between mutual solubility and wetting.

25 ENERGY STORAGE↗
NASA NTRS2004

Increasing the Thermal Stability of Aluminum Titanate for Solid Oxide Fuel Cell Anodes

Solid-oxide fuel cells (SOFCs) show great potential as a power source for future space exploration missions. Because SOFCs operate at temperatures significantly higher than other types of fuel cells, they can reach overall efficiencies of up to 60% and are able to utilize fossil fuels. The SOFC team at GRC is leading NASA's effort to develop a solid oxide fuel cell with a power density high enough to be used for aeronautics and space applications, which is approximately ten times higher than ground transport targets. layers must be able to operate as a single unit at temperatures upwards of 900'C for at least 40,000 hours with less than ten percent degradation. One key challenge to meeting this goal arises from the thermal expansion mismatch between different layers. The amount a material expands upon heating is expressed by its coefficient of thermal expansion (CTE). If the CTEs of adjacent layers are substantially different, thermal stresses will arise during the cell's fabrication and operation. These stresses, accompanied by thermal cycling, can fracture and destroy the cell. While this is not an issue at the electrolyte-cathode interface, it is a major concern at the electrolyte-anode interface, especially in high power anode-supported systems. electrolyte are nearly identical. Conventionally, this has been accomplished by varying the composition of the anode to match the CTE of the yittria-stabilized zirconia (YSZ) electrolyte (approx.10.8x10(exp -6/degC). A Ni/YSZ composite is typically used as a base material for the anode due to its excellent electrochemical properties, but its CTE is about 13.4x10(exp -6/degC). One potential way to lower the CTE of this anode is to add a small percentage of polycrystalline Al2TiO5, with a CTE of 0.68x10(exp -6/degC, to the Ni/YSZ base. However, Al2TiO5 is thermally unstable and loses its effectiveness as it decomposes to Al2O3 and TiO2 between 750 C and 1280 C. be used as additives to increase the thermal stability of Al2TiO5 in SOFC operating conditions without adversely affecting the electrochemical properties of the SOFC anode. Three candidate materials were chosen through an extensive literature review: MgO, Fe2O3, and ZrTiO4. Although all three have been shown to prevent Al2TiO5 decomposition under various conditions, their effectiveness in the temperature range and atmosphere of the SOFC has not yet been evaluated. Several batches of Al2TiO5 with varying amounts of additives were prepared, exposed to reducing and oxidizing atmospheres at elevated temperatures, and the resulting decomposition of Al2TiO5 was measured. The most promising additives were further evaluated with the goal of ultimately preparing low CTE anodes that are chemically compatible to current systems. Adding minor constituents to stabilize Al2TiO5 could ultimately preserve its low CTE for the life of the fuel cell and improve the cell's long-term performance without a drop in anode conductivity. Further, these low CTE filler additions could allow the use of new sulfur tolerant anode materials, improving the viability of SOFCs for future aeronautics and space applications. Every SOFC consists of a cathode and an anode separated by an electrolyte, These three One way to avoid this problem is to design the cell such that the CTEs of the anode and The objective of this summer research project was to evaluate several materials that could

Bender, Jeffrey B.↗
DOE OSTI2026

Toward durable stacks: glass-ceramic sealants for intermediate-temperature protonic ceramic electrochemical systems

Protonic ceramic electrochemical cells (PCECs) are emerging as promising technologies for efficient energy conversion and hydrogen production because they operate at intermediate temperatures with improved efficiency and durability compared with conventional solid oxide electrochemical cells. However, the long-term reliability and commercialization of PCEC stacks remain strongly limited by the performance of sealants, which are required to maintain gas tightness, electrical insulation, and mechanical integrity under harsh thermal and chemical environments. Among various sealing approaches, glass-ceramic sealants are considered the most practical and scalable due to their excellent wettability, chemical tunability, and strong interfacial adhesion. This review provides a comprehensive overview of recent advances in glass-ceramic sealants for intermediate-temperature protonic ceramic electrochemical systems. The fundamental design principles of sealant compositions are first discussed, followed by recent developments in deposition methods, sintering strategies, surface treatments, and degradation monitoring techniques. Particular attention is given to the unique challenges associated with PCEC operating conditions, including hydrothermal degradation, interfacial reactions with barium-containing electrolytes, and thermal mismatch. Finally, future opportunities involving sustainable materials, multiscale modeling, additive manufacturing, and artificial intelligence-assisted sealant optimization are highlighted.

glass–ceramic sealants↗
DOE OSTI2022

An Investigation of the Electrochemical Activity of (Ba/Sr)FeO 3-y Anodes

FeO x , SrFeO 3-y (SF), and Ba 0.5 Sr 0.5 FeO 3–y (BSF) were studied for application as fuel oxidation catalysts in solid oxide fuel cells (SOFC) anodes. Electrodes were prepared by impregnation into porous yttria-stabilized zirconia (YSZ), with La 0.3 Sr 0.7 TiO 3–y (LST) added for electronic conductivity. The electrode impedances decreased dramatically upon addition of SF and BSF and much less when only SrO or FeO x were added. Temperature Programmed Desorption (TPD) of O 2 from oxidized BSF showed O 2 desorbing between 200 °C and 700 °C, while no O 2 desorbed from Fe 2 O 3 below 900 °C. The results, together with thermodynamic analysis, suggest that stabilization of Fe +4 in the perovskite lattice plays an important role in enhancing the catalytic activity of SF and BSF by providing access to a Fe 3+ /Fe 4+ redox couple that can accept oxygen anions from the yttria-stabilized zirconia (YSZ) electrolyte. Oxygen is weakly bound to these sites facilitating its reaction with adsorbed H 2 .

Electrochemistry↗
DOE OSTI2023

In Situ Measurement of Buried Electrolyte–Electrode Interfaces for Solid State Batteries with Nanometer Level Precision

Many technologies including high-energy solid-state batteries rely on high quality solid–solid interfaces. Solid–solid interfaces are particularly difficult to study as their nature requires the interface to be buried. Here, in this work, we demonstrate the use of a combination of neutron reflectometry and in situ electrochemistry to measure the interface between Li metal and the solid electrolyte LiPON across an 8 cm 2 area. Neutron reflectometry measurements confirm the interphase to be less than 7 nm thick. The neutron reflectometry data further emphasize that the interphase that forms is a chemical gradient consisting of a Li-rich layer that gradually decreases in Li content until it blends into pure LiPON. Experimental confirmation that we can make ideal solid–solid interphases less than 10 nm thick will help facilitate the adoption of high efficiency next generation solid state batteries. Further this combination of complementary techniques provides a more general methodology for studying buried solid–solid interfaces across applications.

25 ENERGY STORAGE↗
DOE OSTI2025

Electron Inversion and Tunneling at Silicon Thermal Oxide Interfaces for Solar-Driven Molecular Catalysis to Syngas

Semiconductor photoelectrodes are regularly coupled to solid-state heterogeneous catalysts to perform solar-driven reduction of CO 2 . Less frequently, molecular catalysts are employed to better control the reactivity toward desired products, yet the development of robust semiconductor/molecule interfaces has proven challenging. Here, we demonstrate that a 2–3 nm thermal oxide layer on Si exhibits stability in aqueous solution, high photovoltage, and a photocurrent density of ∼10 mA/cm 2 for the solar-driven photoelectrochemical reduction of a homogeneous molecular catalyst, producing syngas with an ∼2:1 H 2 to CO ratio. Because of a low defect density, the oxide interface forms an electron inversion layer with metal-like electron density at cathodic potentials. This inversion layer facilitates electron transfer to redox-active molecules via tunneling even if the molecule’s reduction potential is beyond the semiconductor’s conduction band edge. Using an electrolyte solution composed of a homogeneous cobalt bis(terpyridine) catalyst in a water/organic solvent mixture, stable photoelectrochemistry was observed under 1-sun illumination, exhibiting an ∼30% Faradaic efficiency for CO that was similar to a glassy carbon electrode under comparable conditions. Furthermore, the results demonstrate that an ultrathin thermal oxide interface is a robust platform for development of aqueous-stable, molecule-driven photoelectrocatalysis.

Catalysts↗
DOE OSTI2021

Materials design of sodium chloride solid electrolytes Na3MCl6 for all-solid-state sodium-ion batteries

All-solid-state sodium-ion batteries have attracted increasing attention owing to the low cost of sodium and the enhanced safety compared to conventional Li-ion batteries. Recently, halides have been considered as promising solid electrolytes (SEs) due to their favorable combination of high ionic conductivity and chemical stability against high-voltage cathode materials. Although a wide variety of lithium chloride SEs, Li 3 MCl 6 , have been developed for high-voltage all-solid-state batteries, only a limited number of sodium chloride SEs have been reported. This study aims to offer a material design insight for the development of sodium chloride SEs through systematic assessment of the phase stability, electrochemical stability, and transport properties of novel Na 3 MCl 6 SEs. Structural calculations indicate that Na 3 MCl 6 exhibits trigonal $P\bar{3}$1c, monoclinic P2 1 /n, and trigonal $R\bar{3}$ phases, and the stable phase of Na 3 MCl 6 is dependent on the type and ionic radius of M. Na 3 MCl 6 typically exhibits a high oxidation potential, demonstrating good electrochemical stability against cathodes. The bond-valence site energy and ab initio molecular dynamics calculations revealed that Na 3 MCl 6 with P2 1 /n and $R\bar{3}$ phases showed low ionic conductivity, while the $P\bar{3}$1c phase slightly improved the ionic conductivity of Na 3 MCl 6 . The formation of Na vacancies by aliovalent substitution considerably increased the ionic conductivity up to four orders of magnitude for pristine Na 3 MCl 6 , exhibiting ~10 –5 S cm –1 for trigonal $P\bar{3}$1c and $R\bar{3}$ phases. The formation of defects could further enhance the ionic conductivity of Na 3 MCl 6 , and the optimization of defect type and ratio can be helpful in developing superionic Na chloride SEs. The material design of Na 3 MCl 6 in this study will provide fundamental guidelines for the development of novel sodium halide SEs for all-solid-state sodium-ion batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Micro-Tubular Solid Oxide Fuel Cell Polarization and Impedance Variation With Thin Porous Samarium-Doped Ceria and Gadolinium-Doped Ceria Buffer Layer Thickness

Abstract Porous buffer layers for anode-supported solid oxide fuel cells (SOFCs) have been investigated for many years with different thicknesses of the buffer layer in each study. In this work, micro-tubular SOFCs having samarium-doped ceria (SDC) and gadolinium-doped ceria (GDC) buffer layers are compared using the current–voltage technique, electrochemical impedance spectroscopy, scanning electron microscopy, and energy-dispersive X-ray spectroscopy. The thickness of the porous SDC and GDC buffer layer is investigated systematically with the thickness varying between 0.3 and 2.0 μm. The power density varies between 212 and 1004 mW/cm2 for samples having different SDC buffer layer thickness. Comparable changes occur for the SOFCs with a GDC buffer layer, but less variation in polarization losses resulted. Variation in electrochemical performance varies due to changes in ohmic resistance, cathode activation polarization, and interfacial reactions between the cathode and electrolyte materials.

Electrochemistry↗
DOE OSTI2020

Exploring Electrocatalysis of Methane on Transition Metal Surfaces

Methane is a potent greenhouse gas because it has a heat-absorbing ability that is 20 times stronger than the better-known carbon dioxide. It is also the dominant component of nature gas (>70%). Its current greenhouse effect is only second to carbon dioxide largely because of its relatively low atmospheric concentration. Alarmingly, however, the latter has seen a 1.5-time increase since 1750, mainly due to anthropogenic livestock farming, coal and natural gas mining, and organic matter decomposing in waste landfills. Mitigating such a trend effectively and efficiently is therefore highly desirable and intensely sought for. This final technical report describes some exciting research progresses made over the last three years supported financially by the aforementioned award. The research conducted focused on exploring electrochemical direct methane to methanol (DMTM) conversion under mild conditions. The goal of research was to explore the possibility of developing potentially game-changing electrocatalysts and electrocatalysis that can convert methane directly to methanol in a most sustainable way for curbing its effect on global warming. Progress has been made in the following three directions. First, by adapting a hydrogen fuel-cell configuration that enables gaseous methane to be transported directly to the electrocatalyst surface, we have overcome the perennial difficulty in measuring activity of methane electro-oxidation at low temperature and ambient pressure that has prevented any meaningful studies of electrocatalysis of methane conversion thus far. Second, we have developed a novel and operational in situ electrochemical infrared (IR) spectral cell for studying electrocatalysis of direct methane to methanol conversion. This novel cell is also expected to alleviate the measuring difficulty caused by low solubility of methane in aqueous electrolyte and low sticking coefficient for methane adsorption onto transition metal surface. It will improve significantly the IR’s signal to noise ratio. Third, we have successfully synthesized nano-sizing copper (Cu) exchanged zeolite mordenite (Cu-ZMOR) and coated it with carbon that enabled electrochemical access to the encaged Cu ions. This opens a door to unravel the chemistry of Cu ions in catalyzing direct methane to methanol conversion under mild experimental conditions. Altogether, these progresses achieved have laid a solid foundation for further exploring electrocatalysis of direct methane to methanol conversion in general where there exists “a plenty of room” for new discoveries and developments.

03 NATURAL GAS↗
NASA NTRS2007

A Symmetrical, Planar SOFC Design for NASA's High Specific Power Density Requirements

Solid oxide fuel cell (SOFC) systems for aircraft applications require an order of magnitude increase in specific power density (1.0 kW/kg) and long life. While significant research is underway to develop anode supported cells which operate at temperatures in the range of 650-800 C, concerns about Cr-contamination from the metal interconnect may drive the operating temperature down further, to 750 C and lower. Higher temperatures, 900-1000 C, are more favorable for SOFC stacks to achieve specific power densities of 1.0 kW/kg. Since metal interconnects are not practical at these high temperatures and can account for up to 75% of the weight of the stack, NASA is pursuing a design that uses a thin, LaCrO3-based ceramic interconnect that incorporates gas channels into the electrodes. The bi-electrode supported cell (BSC) uses porous YSZ scaffolds, on either side of a 10-20 microns electrolyte. The porous support regions are fabricated with graded porosity using the freeze-tape casting process which can be tailored for fuel and air flow. Removing gas channels from the interconnect simplifies the stack design and allows the ceramic interconnect to be kept thin, on the order of 50 -100 microns. The YSZ electrode scaffolds are infiltrated with active electrode materials following the high temperature sintering step. The NASA-BSC is symmetrical and CTE matched, providing balanced stresses and favorable mechanical properties for vibration and thermal cycling.

Cable, Thomas L.↗
DOE OSTI2025

Enabling Solar Water Oxidation by BiVO 4 in Strongly Acidic Solutions

The oxygen evolution reaction (OER) is paired with various electrochemical and photoelectrochemical reduction reactions used for fuel and chemical production. As there is a strong interest in performing many of these reduction reactions in strongly acidic solutions to increase the reaction rate, efficiency, or selectivity, there is also a great interest in enabling efficient and stable OER in strongly acidic solutions. In this study, we report stable photoelectrochemical OER (POER) of a BiVO 4 photoanode in 0.1 M HNO 3 (pH 1). This was achieved by using Nb 2 O 5 as a protection layer. While Nb 2 O 5 was rarely used as a protection layer for photoelectrodes in the past, we show its excellent capability to suppress both the chemical and photoelectrochemical dissolution of BiVO 4 at pH 1. After stabilizing BiVO 4 with a Nb 2 O 5 protection layer, we added Co 2+ ions to the electrolyte as an OER catalyst to enhance the POER. We found that Co (aq) 2+ can serve as a homogeneous OER catalyst without being deposited as a CoO x solid catalyst on Nb 2 O 5 . When we performed the POER using unprotected BiVO 4 with Co (aq) 2+ under the same condition, although POER was enhanced, the enhancement could not be sustained due to the chemical dissolution of BiVO 4 . After the POER, we found that a Co 3+ -containing OER catalyst was deposited on the bare BiVO 4 surface. This result suggested that the use of Co 2+ ions as a homogeneous catalyst was possible due to the inertness of the Nb 2 O 5 surface toward the adsorption or deposition of Co ions. This study enabling stable POER of BiVO 4 in 0.1 M HNO 3 using the combination of a Nb 2 O 5 protection layer and Co (aq) 2+ as a homogeneous OER catalyst provides promising possibilities for acidic POER and OER.

Catalysts↗
DOE OSTI2025

Fast lithium ion diffusion in brownmillerite Li x Sr 2 Co 2 O 5

Transition metal oxides not only exhibits novel magnetic properties but also provides outstanding ionic transports. Ionic conductors have great potential for interesting tunable physical properties via ionic liquid gating and novel energy storage applications such as all-solid-state lithium batteries. In particular, low migration barriers and high hopping attempt frequency are the keys to achieve fast ion diffusion in solids. Taking advantage of the oxygen-vacancy channel in Li x Sr 2 Co 2 O 5 , we show that migration barriers of lithium ion are as small as 0.28–0.17 eV depending on the lithium concentration rates. Our first-principles calculation also investigated hopping attempt frequency and concluded the room temperature ionic diffusivity and ion conductivity are high as 10 −7 –10 −6 cm 2 s −1 and 10 −3 –10 −2 Scm −1 , respectively, which outperform most of perovskite-type, garnet-type, and sulfide Li-ion solid-state electrolytes. This work proves Li x Sr 2 Co 2 O 5 as a promising super-ionic conductor.

Crystallographic defects↗
DOE OSTI2023

Improved cell performance and sulphur tolerance using A-site substituted Sr2Fe1.4Ni0.1Mo0.5O6–δ anodes for solid-oxide fuel cells

Abstract Solid-oxide fuel cells (SOFCs) offer great promise for producing electricity using a wide variety of fuels such as natural gas, coal gas and gasified carbonaceous solids; however, conventional nickel-based anodes face great challenges due to contaminants in readily available fuels, especially sulphur-containing compounds. Thus, the development of new anode materials that can suppress sulphur poisoning is crucial to the realization of fuel-flexible and cost-effective SOFCs. In this work, La0.1Sr1.9Fe1.4Ni0.1Mo0.5O6–δ (LSFNM) and Pr0.1Sr1.9Fe1.4Ni0.1Mo0.5O6–δ (PSFNM) materials have been synthesized using a sol-gel method in air and investigated as anode materials for SOFCs. Metallic nanoparticle-decorated ceramic anodes were obtained by the reduction of LSFNM and PSFNM in H2 at 850°C, forming a Ruddlesden–Popper oxide with exsolved FeNi3 bimetallic nanoparticles. The electrochemical performance of the Sr2Fe1.4Ni0.1Mo0.5O6–δ ceramic anode was greatly enhanced by La doping of A-sites, resulting in a 44% decrease in the polarization resistance in reducing atmosphere. The maximum power densities of Sr- and Mg-doped LaGaO3 (LSGM) (300 μm) electrolyte-supported single cells with LSFNM as the anode reached 1.371 W cm −2 in H2 and 1.306 W cm–2 in 50 ppm H2S–H2 at 850°C. Meanwhile, PSFNM showed improved sulphur tolerance, which could be fully recovered after six cycles from H2 to 50 ppm H2S–H2 operation. This study indicates that LSFNM and PSFNM are promising high-performance anodes for SOFCs.

Li, Haixia↗
DOE OSTI2026

A Dendrite-Resistant Sodium/Porous-Carbon Anode for Solid-State Batteries – Strategies and Challenges for Low-Pressure Operation

Sodium solid-state batteries (Na-SSB) have gained interest recently due to the abundance of Na over Li, but they still tend to fail due to dendrites under practical current densities and cycling capacities. To overcome this, Na-SSBs are frequently tested with impractically high applied pressure. In this work, a porous carbon interfacial layer is utilized in conjunction with Na-ß”-Al2O3 solid electrolytes to enable Na-cycling at milder cell pressures. This sodium/porous carbon layer enables improved solid-state Na cycling in symmetric cells, up to a current density of 10 mA cm-2 at 25 °C. Cycling up to 1 mAh cm-2 is challenging with low pressure, but 1 mAh cm-2 capacity can be reliably cycled at 1 mA cm-2 at an elevated temperature of 60 °C in symmetric cells. Finally, the evolution of the interface and sodium/carbon anode is evaluated with cryogenic ion-milling and cross-sectional imaging revealing that, depending on testing temperature, pressure, current density, and capacity, void formation, Na-extraction from porous carbon, delamination of the porous carbon matrix, or a combination of these occurs at the interface between Na-metal and BASE. Despite this, excellent dendrite resistance is achieved, and a full-cell design utilizing a Na-transition metal oxide cathode is still able to achieve an areal capacity of ~ 2.7 mAh cm-2 at 0.125 mA cm-2. This work demonstrates an alternative pathway toward a Na-metal anode for Na-SSBs without the requirement of excessive stack pressure.

low-cost↗
DOE OSTI2024

Theoretical Understanding of Effects of Operating Modes on the Performance Durability of Solid Oxide Cells: A Comparison between Potentiostatic and Galvanostatic Operations

In solid oxide cells (SOCs), the choice between galvanostatic (constant current) and potentiostatic (constant voltage) modes does not significantly affect the performance of SOCs as long as the cell components remain unchanged and intact. However, the degradation of cell components, which leads to changes in electrochemical and physical properties of the cell, elevates the importance of the selected operating mode. This paper aims to investigate the effects of galvanostatic and potentiostatic operating modes on the evolving properties of SOCs and their subsequent influence on performance durability. Employing non-equilibrium thermodynamic analysis, a crucial approach for understanding the degradation phenomena within an active electrochemical system, this study aims to provide in-depth insights into how these operating modes affect the longevity and efficacy of SOCs. Key findings include: In cases where oxygen electrode (OE) degradation is accelerated by higher partial pressure of oxygen ( p O 2 ), operating under constant voltage electrolysis can mitigate the high p O 2 at the OE|electrolyte (OE|EL) interface. Conversely, if OE degradation occurs more rapidly under a lower p O 2 , constant current electrolysis is more effective in suppressing degradation by achieving a high p O 2 at the OE|EL interface. For degradation of the fuel electrode (FE) due to higher p O 2 , constant current electrolysis is beneficial for more stable performance, which helps maintain low p O 2 at the FE|EL interface. When FE degradation is accelerated by lower p O 2 , constant voltage electrolysis can avert low p O 2 at the FE|EL interface. In practical scenarios, more complex degradation mechanisms come into play, especially when p O 2 significantly deviates from initial conditions. Degradation in one electrode can influence p O 2 in the other electrode, a phenomenon more pronounced in potentiostatic than in galvanostatic electrolysis.

Electrochemistry↗