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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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At least 1,189 records · Page 66
All sourcesNASA NTRSDOE OSTI
NASA NTRS1975

Plasma-sprayed, self-lubricating coatings for use from cryogenic temperatures to 870 deg C (1600 deg F)

A plasma-sprayed coating is described with good lubricating properties over a wide temperature range. The coating, designated NASA LUBE PS101, contains silver, nichrome, calcium fluoride, and an oxidation protective glass. Oscillating tests were conducted of self-aligning, plain cylindrical bearings, in which the bore was lined with 0.025 cm (0.010 in.) thick coatings of PS101; these were conducted at a radial load of 3.5 x 10 to the 7th power N/sq m (5000 psi) in nitrogen gas at -107 C (-160 F), in vacuum at room temperature, and in air from room temperature to 870 C (1600 F). Friction coefficients were less than 0.25 in all cases and wear rates were low. The coating is not brittle, and it has adequate oxidation resistance in air to at least 870 C.

Sliney, H. E.↗
NASA NTRS2002

Strength and Fracture Toughness of Solid Oxide Fuel Cell Electrolyte Material Improved

Solid oxide fuel cells (SOFC) are being developed for various applications in the automobile, power-generation, and aeronautics industries. Recently, the NASA Glenn Research Center has been exploring the possibility of using SOFC's for aeropropulsion under its Zero Carbon Dioxide Emission Technology (ZCET) Program. 10-mol% yttriastabilized zirconia (10YSZ) is a very good anionic conductor at high temperatures and is, therefore, used as an oxygen solid electrolyte in SOFC. However, it has a high thermal expansion coefficient, low thermal shock resistance, low fracture toughness, and poor mechanical strength. For aeronautic applications, the thin ceramic electrolyte membrane of the SOFC needs to be strong and tough. Therefore, we have been investigating the possibility of enhancing the strength and fracture toughness of the 10YSZ electrolyte without degrading its electrical conductivity to an appreciable extent. We recently demonstrated that the addition of alumina to zirconia electrolyte increases its strength as well as its fracture toughness. Zirconia-alumina composites containing 0 to 30 mol% of alumina were fabricated by hot pressing. The hot pressing procedure was developed and various hot pressing parameters were optimized, resulting in dense, crackfree panels of composite materials. Cubic zirconia and a-alumina were the only phases detected, indicating that there was no chemical reaction between the constituents during hot pressing at elevated temperatures. Flexure strength sf and fracture toughness K(sub IC) of the various zirconia-alumina composites were measured at room temperature as well as at 1000 C in air. Both properties showed systematic improvement with increased alumina addition at room temperature and at 1000 C. Use of these modified electrolytes with improved strength and fracture toughness should prolong the life and enhance the performance of SOFC in aeronautics and other applications.

Bansal, Narottam P.↗
DOE OSTI2022

Molecular Vibrational Polaritons Towards Quantum Technologies

In this paper molecular vibrational polaritons (MVPs)—a hybrid molecular-photon quasiparticle—and the development of a proof-of-principle quantum technology platform are discussed to simulate coherence transfer, for use at room temperature. It is shown that MVPs can form qubits, coherence, and have nonlinear interactions, all at room temperature. Some new insights, such as polaritonic nonlinearity dependence on macroscopic properties including cavity thickness and molecular concentrations are also uncovered. It is hoped that these advances can stimulate more research in developing this system into a quantum technology platform free from the constraints imposed by the requirement of cryogenic conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

OH Roaming during the Ozonolysis of α-Pinene: A New Route to Highly Oxygenated Molecules?

The formation of low-volatility organic compounds in the ozonolysis of α-pinene, the dominant atmospheric monoterpene, provides an important route to aerosol formation. Here, in this work, we consider a previously unexplored set of pathways for the formation of highly oxygenated molecules in α-pinene ozonolysis. Pioneering, direct experimental observations of Lester and co-workers have demonstrated a significant production of hydroxycarbonyl products in the dissociation of Criegee intermediates. Theoretical analyses indicate that this production arises from OH roaming-induced pathways during the OO fission of the vinylhydroperoxides (VHPs), which in turn come from internal H transfers in the Criegee intermediates. Ab initio kinetics computations are used here to explore the OH roaming-induced channels that arise from the ozonolysis of α-pinene. For computational reasons, the calculations consider a surrogate for α-pinene, where two spectator methyl groups are replaced with H atoms. Multireference electronic structure calculations are used to illustrate a variety of energetically accessible OH roaming pathways for the four VHPs arising from the ozonolysis of this α-pinene surrogate. Ab initio transition-state theory-based master equation calculations indicate that for the dissociation of stabilized VHPs, these OH roaming pathways are kinetically significant with a branching that generally increases from ~20% at room temperature up to ~70% at lower temperatures representative of the troposphere. For one of the VHPs, this branching already exceeds 60% at room temperature. For the overall ozonolysis process, these branching ratios would be greatly reduced by a limited branching to the stabilized VHP, although there would also be some modest roaming fraction for the nonthermal VHP dissociation process. The strong exothermicities of the roaming-induced isomerizations/additions and abstractions suggest new routes to fission of the cyclobutane rings. Such ring fissions would facilitate further autoxidation reactions, thereby providing a new route for producing highly oxygenated nonvolatile precursors to aerosol formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

High-volume tunable resonator for axion searches above 7 GHz

In this research, we present results from an experimental demonstration of a tunable thin-shell axion haloscope whose geometry decouples its overall volume from its resonant frequency, thereby evading the steep sensitivity degradation at high frequencies. An aluminum 2.6-l (41⁢λ 3 ) prototype, which tunes from 7.1 to 8.0 GHz, was fabricated and characterized at room temperature. An axion-sensitive, straightforwardly tunable TM 010 mode is clearly identified with a room-temperature quality factor, Q, of approximately 5000. The on-resonance E-field distribution is mapped and found to agree with numerical calculations. Anticipating future cryogenic operation, we develop an alignment protocol relying only on rf measurements of the cavity, maintaining a form factor of 0.57 across the full tuning range. These measurements demonstrate the feasibility of cavity-based haloscopes with operating volume V $\gg$ λ 3 . We discuss plans for future development and the parameters required for a thin-shell haloscope exploring the postinflationary axion parameter space (approximately 4 to 30 GHz) at Dine-Fischler-Srednicki-Zhitnitsky sensitivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Structure-property relationships and mobility optimization in sputtered La-doped BaSn O 3 films: Toward 100cm 2 V -1 s -1

he wide band gap semiconducting perovskite BaSnO 3 is of high current interest due to outstanding room temperature mobility at high electron density, fueled by potential applications in oxide, transparent, and power electronics. Due in part to a lack of lattice-matched substrates, BaSnO 3 thin films suffer from high defect densities, however, limiting electron mobility. Additionally, the vast majority of BaSnO 3 thin film research has focused on pulsed laser deposition or molecular beam epitaxy. In this work, we present an exhaustive optimization of the mobility of Ba 0.98 La 0.02 SnO 3 films grown by a scalable, high-throughput method: high-pressure-oxygen sputter deposition. Considering target synthesis conditions, substrate selection, buffer layer structure, deposition temperature, deposition rate, thickness, and postdeposition annealing conditions, and by combining high-resolution x-ray diffraction, reciprocal space mapping, rocking curve analysis, scanning transmission electron microscopy, atomic force microscopy, and temperature-dependent electronic transport measurements, detailed understanding of synthesis-structure-property relationships is attained. Optimized room temperature mobility of 96 cm 2 V –1 s –1 is achieved in vacuum-annealed GdScO 3 (110)/BaSnO 3 (120 nm)/Ba 0.98 La 0.02 SnO 3 (200 nm) heterostructures, as well as 92 cm 2 V –1 s –1 on unbuffered substrates and 87 2 V –1 s –1 without postdeposition annealing. These results, including important trends in defect densities and a surprising dependence of mobility on lattice mismatch, substantially expand the understanding of the interplay between deposition conditions, microstructure, and transport in doped BaSnO 3 films, establishing competitive mobilities in films fabricated via a scalable, high-throughput, industry-standard technique.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Field-free switching of perpendicular magnetization in a ferrimagnetic insulator with spin reorientation transition

Writing magnetic bits through spin-orbit torque (SOT) switching is promising for fast and efficient magnetic random-access memory devices. While SOT switching of out-of-plane (OOP) magnetized states requires lateral symmetry breaking, in-plane (IP) magnetized states suffer from low storage density. Here, we demonstrate a field-free switching scheme using a 5-nanometer europium iron garnet film grown with a (110) orientation that shows a spin reorientation transition from OOP to IP above room temperature. This scheme combines the benefits of high-density storage in the OOP states at room temperature and the efficient field-free SOT switching in the IP states at elevated temperatures. While conventional switching of OOP bits faces the dilemma that high OOP anisotropy is required to improve bit stability and low OOP anisotropy is required to lower switching current density, this scheme disentangles this interdependence, allowing for low switching currents to be possible without sacrificing the bit stability, offering opportunities for future memory devices.

Science & Technology - Other Topics↗
DOE OSTI2021

Study of the Segmental Dynamics and Ion Transport of Solid Polymer Electrolytes in the Semi-crystalline State

Solid polymer electrolytes are promising in fulfilling the requirements for a stable lithium metal anode toward higher energy and power densities. In this work, we investigate the segmental dynamics, ionic conductivity, and crystallinity of a polymer electrolyte consisting of poly(ethylene oxide) (PEO) and lithium triflate salt, in the semi-crystalline state. Using quasi-elastic neutron scattering, the segmental dynamics of PEO chains confined between the crystalline lamellae is quantified, using Cole–Cole analysis. We show that the structural relaxation time, τ 0 , of PEO equilibrated near room temperature is six-fold longer than the same sample that had just cooled down to room temperature. This corresponds to a three-fold smaller ionic conductivity in the equilibrated condition. This work reveals that the segmental dynamics of semi-crystalline polymer electrolytes is very sensitive to thermal history. We demonstrate that quasi-elastic neutron scattering can be used to characterize the ion transport and segmental dynamics in the semi-crystalline state.

36 MATERIALS SCIENCE↗
NASA NTRS1996

Properties of Single Crystalline Semiconducting CoSb3

A study of the thermoelectric properties of the skutterudite compound CoSb3 was carried out on single crystals grown by the Bridgman gradient freeze technique. p- and n-type samples were obtained over a wide range of carrier concentration. Undoped As-grown crystals show p-type conductivity while n-type samples were obtained by addition of Te or Pd. Samples were characterized by x-ray diffractometry, electron microprobe analysis, and density measurements. The physical properties of CoSb3 such as linear thermal expansion coefficient, sound velocity, and Debye temperature were also determined and are presented. Seebeck coefficient, electrical resistivity, thermal conductivity, and Hall effect measurements were performed between room temperature and about 900 K. Exceptionally high Hall mobilities were obtained on p-type samples with a maximum room-temperature Hall mobility of 3300 sq cm/V.s at a carrier concentration of 1 x 10(exp 17)/cc. The results of the transport property measurements are discussed and are in agreement with some recent predictions based on band structure calculations. The potential of CoSb3 for thermoelectric applications is evaluated.

Caillat, T.↗
DOE OSTI2021

Understanding the Reactions Between Fe and Se Binary Diffusion Couples

Spurred by recent discoveries of high-temperature superconductivity in Fe-Se based materials, the magnetic, electronic, and catalytic properties of iron-chalcogenides have drawn significant attention. Furthermore, much remains to be understood about the sequence of phase formation in these systems. In this work, we shed light on this issue by preparing a series of binary Fe-Se ultrathin diffusion couples via designed thin film precursors and investigating their structural evolution as a function of composition and annealing temperature. Two previously unreported Fe-Se phases crystallized during the deposition process on a nominally room-temperature Si substrate in the 27-33% and 37-47% Fe (atomic percent) composition regimes. Both phases completely decompose after annealing to 200°C in a nitrogen glovebox. At higher temperatures, the sequence of phase formation is governed by Se loss in the annealing process, consistent with what would be expected from the phase diagram. Films rich in Fe (53-59% Fe) crystalized during deposition as β-FeSe (P4/nmm) with preferred c-axis orientation to the amorphous SiO 2 substrate surface, providing a means to non-epitaxial self-assembly of crystallographically aligned, iron-rich β-FeSe for future research. Our findings suggest the crystallization of binary Fe-Se compounds at room temperature via near diffusionless transformations should be a significant consideration in future attempts to prepare metastable ternary and higher order compounds containing Fe and Se.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Experimental thermal equation of state of B 2–KCl

The alkali halides are often used as optically-transparent pressure-transmitting media and thermal insulators in laser-heated diamond anvil cell experiments. High P-T equations of state for these materials would allow them to be used simultaneously as sensitive in situ pressure markers, making sample preparation and data analysis simpler. KCl is especially useful for this application because its high melting point, crystallographic simplicity, and low electron density are ideal for use in high-temperature X-ray diffraction experiments. However, the high-temperature static equation of state data for this material is limited in pressure to 8 GPa. As experiments routinely exceed 100 GPa in pressure and thousands of Kelvin, it is necessary for the equation of state of KCl to be determined experimentally at these conditions if it is to be used as an equation of state calibrant in the future. This work combines new high-pressure, high-temperature data of the B2 phase of KCl (up to 167 GPa and 2400 K) with the previously published room-temperature data of Dewaele et al. (2012) to produce a Mie-Gruneisen-Debye thermal equation of state for this material. The room temperature equation of state parameters are similar to those reported previously: V 0 = 32.0(3) cm 3 /mole, K 0 = 24(1) GPa and $K$$^{'}_{0}$ = 4.56(5). The thermal parameters, 0 and q, are 2.9(4) and 1.0(1), respectively. While a q of 1 is expected, the 0 is higher than expected from previous calculations, lower pressure experimental data, and the available shockwave data. Here, previously-reported equations of state underestimate the pressure of KCl at high temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1984

Propane absorption band intensities and band model parameters from 680 to 1580/cm at 296 and 200 K

Band intensities and profiles have been measured for the propane absorption bands from 680 to 1580/cm at 296 and 200 K. This work was stimulated by the discovery of several propane bands in the spectrum of Titan by the Voyager 1 spacecraft. The low temperature laboratory data show that the bands become narrower and the Q branches of the bands somewhat stronger than they are at room temperature. Random band model parameters were determined over the entire region from the 42 spectra obtained at room temperature.

Giver, L. P.↗
NASA NTRS2008

MEMS Microshutter Array System for James Webb Space Telescope

A complex MEMS microshutter array system has been developed at NASA Goddard Space Flight Center (GSFC) for use as a multi-object aperture array for a Near-Infrared Spectrometer (NIRSpec). The NIRSpec is one of the four major instruments carried by the James Webb Space Telescope (JWST), the next generation of space telescope after the Hubble Space Telescope retires. The microshutter arrays (MSAs) are designed for the selective transmission of light with high efficiency and high contrast. It is demonstrated in Figure 1 how a MSA is used as a multiple object selector in deep space. The MSAs empower the NIRSpec instrument simultaneously collect spectra from more than 100 targets therefore increases the instrument efficiency 100 times or more. The MSA assembly is one of three major innovations on JWST and the first major MEMS devices serving observation missions in space. The MSA system developed at NASA GSFC is assembled with four quadrant fully addressable 365x171 shutter arrays that are actuated magnetically, latched and addressed electrostatically. As shown in Figure 2, each MSA is fabricated out of a 4' silicon-on-insulator (SOI) wafer using MEMS bulk-micromachining technology. Individual shutters are close-packed silicon nitride membranes with a pixel size close to 100x200 pm (Figure 3). Shutters are patterned with a torsion flexure permitting shutters to open 90 degrees with a minimized mechanical stress concentration. In order to prevent light leak, light shields are made on to the surrounding frame of each shutter to cover the gaps between the shutters and the Game (Figure 4). Micro-ribs and sub-micron bumps are tailored on hack walls and light shields, respectively, to prevent sticktion, shown in Figures 4 and 5. JWST instruments are required to operate at cryogenic temperatures as low as 35K, though they are to be subjected to various levels of ground tests at room temperature. The shutters should therefore maintain nearly flat in the entire temperature range between 35K and 300K. Through intensive numerical simulations and experimental studies, an optically opaque and electrically conductive metal-nitride thin film was selected as a coating material deposited on the shutters with the best thermal-expansion match to silicon nitride - the shutter blade thin film material. A shutter image shown in Figure 6 was taken at room temperature, presenting shutters slightly bowing down as expected. Shutters become flat when the temperature decreases to 35K. The MSAs are then bonded to silicon substrates that are fabricated out of 6" single-silicon wafers in the thickness of 2mm. The bonding is conducted using a novel single-sided indium flip-chip bonding technology. Indium bumps fabricated on a substrate are shown in Figure 7. There are 180,000 indium bumps for bonding a flight format MSA array to its substrate. Besides a MSA, each substrate houses five customer-designed ASIC (Application Specific Integrated Circuit) multiplexer/address chips for 2-dimensional addressing, twenty capacitors, two temperature sensors, numbers of resistors and all necessary interconnects, as shown in Figure 8. Complete MSA quadrant assemblies have been successfully manufactured and fully functionally tested. The assemblies have passed a series of critical reviews required by JWST in satisfying all the design specifications. The qualification tests cover programmable 2-D addressing, life tests, optical contrast tests, and environmental tests including radiation, vibration, and acoustic tests. A 2-D addressing pattern with 'ESA' letters programmed in a MSA is shown in Figure 9. The MSAs passed 1 million cycle life tests and achieved high optical contrast over 10,000. MSA teams are now making progress in final fabrication, testing and assembly (Figure 10). The delivery of flight-format MSA system is scheduled at the end of 2008 for being integrated to the focal plane of the NIRSpec detectors.

Li, Mary J.↗
DOE OSTI2020

Characterization of the pressure coefficient of manganin and temperature evolution of pressure in piston-cylinder cells

Here, we report measurements of the temperature- and pressure-dependent resistance, R ( T , p ), of a manganin manometer in a 4 He-gas pressure setup from room temperature down to the solidification temperature of 4 He ( T solid ~ 50 K at 0.8 GPa) for pressures, p , between 0 GPa and ~0.8 GPa. The same manganin wire manometer was also measured in a piston-cylinder cell (PCC) from 300 K down to 1.8 K and for pressures between 0 GPa and ~2 GPa. From these data, we infer the temperature and pressure dependence of the pressure coefficient of manganin, α ( T , p ), defined by the equation R p = (1 + αp ) R 0 , where R 0 and R p are the resistances of manganin at ambient pressure and finite pressure, respectively. Our results indicate that upon cooling, α first decreases, then goes through a broad minimum at ~120 K, and increases again toward lower temperatures. In addition, we find that α is almost pressure-independent at T ≳ 60 K up to p ~ 2 GPa, but shows a pronounced p dependence at T ≲ 60 K. Using this manganin manometer, we demonstrate that p overall decreases with decreasing temperature in the PCC for the full pressure range and that the size of the pressure difference between room temperature and low temperatures ( T = 1.8 K), Δ p , decreases with increasing pressure. We also compare the pressure values inferred from the manganin manometer with the low-temperature pressure, determined from the superconducting transition temperature of elemental lead (Pb). As a result of these data and analysis, we propose a practical algorithm to infer the evolution of pressure with temperature in a PCC.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Theoretical and experimental quantification of Suzuki segregation enthalpy and strengthening mechanisms in a binary alloy

Solute segregation to planar defects in metallic alloys has been shown to drastically alter mechanical properties. While various works using first-principles and thermodynamic calculations have studied the fundamental driving forces for solute segregation via the Suzuki criterion, planar defect energy, or a comparison of energies of the HCP-like phase and FCC matrix, a quantitative experimental and computational comparison of equilibrium composition and segregation enthalpies has not yet been reported. In this work, we predict the equilibrium composition and segregation enthalpy to intrinsic stacking faults in a Ni-60Co (at.%) alloy and compare the results to two independent experimental methods. We observed that Co segregates to the innermost two planes of the intrinsic stacking fault, and we found that the experimental segregation enrichment, measured from transmission electron microscopy energy dispersive X-ray spectroscopy, of the faults is 6.8 at.% Co, which is 2.2 at.% less than the predicted value at the same temperature. We also find that the segregation enthalpy measured from the composition profile is −21.1 ± 6.4 meV/atom and separately from differential scanning calorimetry segregation enthalpy is −33.2 meV/atom, whereas the predicted enthalpy is −31 ± 1 meV/atom. Based on these results, we determine that segregation occurs very rapidly, within 8 min at temperatures as low as 36% of the homologous solidus temperature. Furthermore, this analysis provides an overview of the possible dislocation mechanisms responsible for strengthening effects due to solute segregation, and concludes that changes in room temperature hardness from local phase transformation is likely tied to post-segregation room temperature equilibrium partial separation distance.

Ab initio calculation↗
DOE OSTI2022

Role of chemical disorder on radiation-induced defect production and damage evolution in NiFeCoCr

Understanding chemical disorder in many concentrated solid solution alloys (CSAs) at the levels of electrons and atoms has attracted increasing attention as a path forward to reveal and identify underlying mechanisms for extraordinary mechanical properties and improved radiation tolerance. Single-phase NiFeCoCr CSA is a common base for many high-entropy alloys (HEAs) that have shown improved mechanical strength and radiation tolerance. In this study, defect production and damage evolution in NiFeCoCr under ion irradiation at room temperature to dose over 20 dpa are determined using ion channeling technique along both <100> and <110> directions utilizing multiple probing beam energies. The results obtained from the multi-axial and multi-energy channeling analysis are compared with those previously obtained for Ni crystals irradiated under similar conditions. The influence of chemical complexity on defect production and clustering at early-stage under room temperature irradiation up to dose of 1 dpa is discussed based on positron annihilation spectroscopy results. Defect structure evaluation in Ni and NiFeCoCr is also discussed based on transmission electron microscopy results over a prolonged irradiation at both room and elevated temperatures. Compared with chemically complex NiFeCoCr, larger dislocation loops thus less lattice strain are expected to form in pure Ni. Moreover, the role of chemical disorder in this CSA is also investigated based on ab initio calculations using large supercells. Finally, to understand the impact of chemical complexity effect on defect structure evolution, this integrated research effort attempts to link the relatively large charge redistribution due to difference in valence electron counts resulting from alloying different 3d transition metal elements, moderate lattice distortion arising from similar adaptable atomic size, and notable suppressed or delayed damage evolution in NiFeCoCr.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Crystal and Electronic Structures of A 2 NaIO 6 Periodate Double Perovskites (A = Sr, Ca, Ba): Candidate Wasteforms for I-129 Immobilization

The synthesis, structure, and thermal stability of the periodate double perovskites A 2 NaIO 6 (A= Ba, Sr, Ca) were investigated in the context of potential application for the immobilization of radioiodine. A combination of X-ray diffraction and neutron diffraction, Raman spectroscopy, and DFT simulations were applied to determine accurate crystal structures of these compounds and understand their relative stability. The compounds were found to exhibit rock-salt ordering of Na and I on the perovskite B-site; Ba 2 NaIO 6 was found to adopt the Fm- 3 m aristotype structure, whereas Sr 2 NaIO 6 and Ca 2 NaIO 6 adopt the P 2 1 / n hettotype structure, characterized by cooperative octahedral tilting. DFT simulations determined the Fm- 3 m and P 2 1 / n structures of Ba 2 NaIO 6 to be energetically degenerate at room temperature, whereas diffraction and spectroscopy data evidence only the presence of the Fm- 3 m phase at room temperature, which may imply an incipient phase transition for this compound. The periodate double perovskites were found to exhibit remarkable thermal stability, with Ba 2 NaIO 6 only decomposing above 1050 °C in air, which is apparently the highest recorded decomposition temperature so far recorded for any iodine bearing compound. As such, these compounds offer some potential for application in the immobilization of iodine-129, from nuclear fuel reprocessing, with an iodine incorporation rate of 25–40 wt%. The synthesis of these compounds, elaborated here, is also compatible with both current conventional and future advanced processes for iodine recovery from the dissolver off-gas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Kinetic Effects of Anion Clusters on the Interfacial Stability between Solid-State Electrolyte and Metal Anode

The success of all-solid-state batteries (ASSBs) depends on the solid-state electrolyte (SSE) exhibiting high interfacial stability and room-temperature ionic conductivity. However, the current SSEs, especially those with practical ionic conductivities (≥10 –3 S/cm) at room temperature, often develop unstable interfaces at the metal anode, in some cases with even greater severity than with liquid organic electrolytes. Despite persistent efforts, achieving interfacial stability and sufficient ionic conductivity simultaneously represents one of the greatest challenges in ASSBs. The current approaches focus on stabilizing the interface by incorporating secondary interlayers or introducing coatings by surface engineering. The method is often material-specific, and the added interlayers often deteriorate during cycling. In this work, using phase analysis and explicit interface modeling, we demonstrate a strategy to kinetically stabilize the interface between the SSE and metal anode by incorporating selected monoanion clusters in the SSE; they can effectively lower or even halt the reduction kinetics at the interface by promoting on-site formation of interphases that are highly electron insulating. The study provides insight into the kinetic effects to achieve SSEs with superior properties in bulk and at the interface.

25 ENERGY STORAGE↗