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DOE OSTI2023

The effect of metals on zeolite crystallization kinetics with relevance to nuclear waste glass corrosion

Abstract Geologic disposal of vitrified radioactive material is planned in several countries, but there are remaining uncertainties related to the long-term stability of glass exposed to groundwater. Specifically, the crystallization of aluminosilicate zeolite minerals can accelerate the rate at which glass corrodes and radioactive material is released into the biosphere. In this study, we identify elemental species that may accelerate or suppress zeolite formation using a protocol to examine their effects on zeolite synthesis over a three-day duration. Our results are consistent with previous works demonstrating glass corrosion acceleration in the presence of calcium. Furthermore, we identify two elements—tin and lithium—as inhibitors of zeolite P2 (gismondine, or GIS type) nucleation and, thus, promising components for promoting the long-term durability of glass waste forms.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Spherical tokamak physics research in preparation for the operation of NSTX-U

The National Spherical Torus Experiment Upgrade (NSTX-U) is preparing to resume operation, representing a crucial step toward realizing compact, cost-effective fusion pilot plants. In advance of this, extensive modeling and data analysis have been conducted to advance the physics basis for low-aspect-ratio, high-performance plasma regimes, focusing on three core objectives: confinement and stability, power and particle handling, and steady-state operation. Significant progress has been made in understanding the electron temperature flattening in high-β plasmas, which is shown to be driven by a complex interplay of magnetohydrodynamic instabilities (e.g. non-resonant infernal modes), fast-ion-driven Alfvén eigenmodes, and electron and ion-scale micro-instabilities, particularly Kinetic Ballooning Modes (KBMs), whose destabilization is strongly dependent on parallel magnetic field fluctuations (δB ∥ ). Furthermore, a new gyrokinetic critical pedestal model was developed, accurately predicting pedestal structure by identifying KBMs as the primary stability limit, offering a critical constraint for future high-confinement scenarios. To address the challenge of high heat flux, novel liquid lithium plasma-facing components were modeled. The analysis confirmed that lithium vapor shielding is a self-regulating mechanism for heat mitigation, while also emphasizing that strong main ion parallel flow is essential to minimize core lithium contamination. Finally, progress toward steady-state operation was anchored by developing the required physics basis and control tools. This includes predictive modeling for reversed magnetic shear sustainment, demonstrating that magnetic island-induced bootstrap current reduction is negligible in STs, and advancing real-time control and disruption avoidance capabilities. The development of high-speed surrogate models (e.g. MMMNet) provides computationally efficient tools vital for non-inductive scenario optimization and integrated, low-disruptivity operations planned for NSTX-U.

NSTX-U↗

DOE OSTI2020

Long-range Doppler lidar measurements of wind turbine wakes and their interaction with turbulent atmospheric boundary-layer flow at Perdigao 2017

As part of the Perdigão 2017 campaign, vertical RHI (range-height indicator) scans with long-range pulsed Doppler wind lidars were performed aligned with the main wind direction and a wind turbine (WT) located on a mountain ridge. The measurements are used to not only retrieve flow velocities, but also their variance and - by using the turbulent broadening of the Doppler spectrum - also turbulent kinetic energy (TKE) dissipation rate. The study shows that turbulence in the WT wake is dependent on the turbulence of the inflow, but also on atmospheric stability. In stable atmospheric conditions, wakes could be analyzed up to five rotor diameters downstream (D) and showed the maximum turbulence in the wake at 2-3 D, whereas in unstable conditions, the maximum was found at 2 D and the wake could not be detected further than 3 D. A clear dependency of wake turbulence enhancement on inflow turbulence intensity is found, which levels out to no further enhancement at turbulence intensities of 30%.

17 WIND ENERGY↗

DOE OSTI2021

Enhancing Paraoxon Binding to Organophosphorus Hydrolase Active Site

Organophosphorus hydrolase (OPH) is a metalloenzyme that can hydrolyze organophosphorus agents resulting in products that are generally of reduced toxicity. The best OPH substrate found to date is diethyl p-nitrophenyl phosphate (paraoxon). Most structural and kinetic studies assume that the binding orientation of paraoxon is identical to that of diethyl 4-methylbenzylphosphonate, which is the only substrate analog co-crystallized with OPH. In the current work, we used a combined docking and molecular dynamics (MD) approach to predict the likely binding mode of paraoxon. Then, we used the predicted binding mode to run MD simulations on the wild type (WT) OPH complexed with paraoxon, and OPH mutants complexed with paraoxon. Additionally, we identified three hot-spot residues (D253, H254, and I255) involved in the stability of the OPH active site. We then experimentally assayed single and double mutants involving these residues for paraoxon binding affinity. The binding free energy calculations and the experimental kinetics of the reactions between each OPH mutant and paraoxon show that mutated forms D253E, D253E-H254R, and D253E-I255G exhibit enhanced substrate binding affinity over WT OPH. Interestingly, our experimental results show that the substrate binding affinity of the double mutant D253E-H254R increased by 19-fold compared to WT OPH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Data‐driven variational method for discrepancy modeling: Dynamics with small‐strain nonlinear elasticity and viscoelasticity

Abstract The effective inclusion of a priori knowledge when embedding known data in physics‐based models of dynamical systems can ensure that the reconstructed model respects physical principles, while simultaneously improving the accuracy of the solution in the previously unseen regions of state space. This paper presents a physics‐constrained data‐driven discrepancy modeling method that variationally embeds known data in the modeling framework. The hierarchical structure of the method yields fine scale variational equations that facilitate the derivation of residuals which are comprised of the first‐principles theory and sensor‐based data from the dynamical system. The embedding of the sensor data via residual terms leads to discrepancy‐informed closure models that yield a method which is driven not only by boundary and initial conditions, but also by measurements that are taken at only a few observation points in the target system. Specifically, the data‐embedding term serves as residual‐based least‐squares loss function, thus retaining variational consistency. Another important relation arises from the interpretation of the stabilization tensor as a kernel function, thereby incorporating a priori knowledge of the problem and adding computational intelligence to the modeling framework. Numerical test cases show that when known data is taken into account, the data driven variational (DDV) method can correctly predict the system response in the presence of several types of discrepancies. Specifically, the damped solution and correct energy time histories are recovered by including known data in the undamped situation. Morlet wavelet analyses reveal that the surrogate problem with embedded data recovers the fundamental frequency band of the target system. The enhanced stability and accuracy of the DDV method is manifested via reconstructed displacement and velocity fields that yield time histories of strain and kinetic energies which match the target systems. The proposed DDV method also serves as a procedure for restoring eigenvalues and eigenvectors of a deficient dynamical system when known data is taken into account, as shown in the numerical test cases presented here.

Masud, Arif↗

DOE OSTI2026

Observations of the Marine Atmospheric Boundary Layer’s Response to a Solar Eclipse

The atmospheric response to the solar eclipse of 8 April 2024 in North America is investigated with a specific focus on the marine atmospheric boundary layer (MABL). We leverage measurements collected during the Third Wind Forecast Improvement Project (WFIP3), including Doppler lidars, sonic anemometers, and thermodynamic profiler data to investigate the atmospheric response across sites that experienced partial eclipse conditions with nearly 90% obscuration. Using these measurements, we examine eclipse-induced changes in key meteorological parameters, such as temperature, wind speed, and turbulent fluxes. Most previous eclipse studies have been conducted over land, whereas this study provides new observations for both coastal and marine environments, offering additional insight into eclipse-driven variability in the MABL. The findings confirm a notable decrease in downwelling shortwave radiation during the eclipse, which results in rapid cooling of surface air. The temperature reduction ranges from $1.2^\circ \text {C}$ to $1.4^\circ \text {C}$ in coastal regions and from $0.3^\circ \text {C}$ to $0.5^\circ \text {C}$ over the ocean. This analysis suggests that the MABL’s higher thermal inertia compared to coastal regions moderates the temperature decrease during the eclipse. Wind speed exhibits a more complex behavior, as it is influenced by both the MABL and preexisting synoptic conditions. Although a reduction in wind speed is observable up to approximately 140 m above ground level (AGL) at more inland sites, at other locations closer to the coast, this reduction is constrained to the lowest 100 m AGL. Turbulence parameters retrieved from sonic anemometers, such as turbulence kinetic energy, turbulent heat flux, and friction velocity, decrease during the eclipse at coastal sites, accompanied by a brief transition of atmospheric stability from unstable to neutral or weakly stable conditions. For the open-ocean sites, the variability in turbulence statistics and atmospheric stability is minimal during the occurrence of the eclipse.

16 TIDAL AND WAVE POWER↗

DOE OSTI2021

All-Solid-State Lithium–Sulfur Batteries Enhanced by Redox Mediators

We report redox mediators (RMs) play a vital role in some liquid electrolyte-based electrochemical energy storage systems. However, the concept of redox mediator in solid-state batteries remains unexplored. Here, we selected a group of RM candidates and investigated their behaviors and roles in all-solid-state lithium-sulfur batteries (ASSLSBs). The soluble-type quinone-based RM (AQT) shows the most favorable redox potential and the best redox reversibility that functions well for lithium sulfide (Li 2 S) oxidation in solid polymer electrolytes. Accordingly, Li 2 S cathodes with AQT RMs present a significantly reduced energy barrier (average oxidation potential of 2.4 V) during initial charging at 0.1 C at 60 °C and the following discharge capacity of 1133 mAh g s -1 . Using operando sulfur K-edge X-ray absorption spectroscopy, we directly tracked the sulfur speciation in ASSLSBs and proved that the solid-polysulfide-solid reaction of Li 2 S cathodes with RMs facilitated Li 2 S oxidation. In contrast, for bare Li 2 S cathodes, the solid-solid Li 2 S-sulfur direct conversion in the first charge cycle results in a high energy barrier for activation (charge to ~4 V) and low sulfur utilization. The Li 2 S@AQT cell demonstrates superior cycling stability (average Coulombic efficiency 98.9% for 150 cycles) and rate capability owing to the effective AQT-enhanced Li-S reaction kinetics. This work reveals the evolution of sulfur species in ASSLSBs and realizes the fast Li-S reaction kinetics by designing an effective sulfur speciation pathway

25 ENERGY STORAGE↗

DOE OSTI2025

Structure Sensitivity and Catalyst Restructuring for CO2 Electro-reduction on Copper

Abstract Cu is the most promising metal catalyst for CO 2 electroreduction (CO 2 RR) to multi-carbon products, yet the structure sensitivity of the reaction and the stability versus restructuring of the catalyst surface under reaction conditions remain controversial. Here, atomic scale simulations of surface energies and reaction pathway kinetics supported by experimental evidence unveil that CO 2 RR does not take place on perfect planar Cu(111) and Cu(100) surfaces but rather on steps or kinks. These planar surfaces tend to restructure in reaction conditions to the active stepped surfaces, with the strong binding of CO on defective sites acting as a thermodynamic driving force. Notably, we identify that the square motifs adjacent to defects, not the defects themselves, as the active sites for CO 2 RR via synergistic effect. We evaluate these mechanisms against experiments of CO 2 RR on ultra-high vacuum-prepared ultraclean Cu surfaces, uncovering the crucial role of step-edge orientation in steering selectivity. Overall, our study refines the structural sensitivity of CO 2 RR on Cu at the atomic level, highlights the self-activation mechanism and elucidates the origin of in situ restructuring of Cu surfaces during the reaction.

Science & Technology - Other Topics↗

DOE OSTI2025

Adsorptive behavior of poly (vinylidene fluoride) membranes for the recovery of lignin-derived hydrophobic deep eutectic solvents

Abstract Recently, membrane technology has gained significant traction as an energy-efficient alternative to traditional thermal processes for solvent recovery. Deep eutectic solvents (DESs) have emerged as sustainable alternatives to conventional organic solvents, yet a systematic methodology for selecting compatible membrane materials for their recovery remains underdeveloped. This study established a predictive framework for membrane material selection in hydrophobic DES applications using Hansen Solubility Parameters (HSP) with inverted criteria targeting materials with relative energy difference (RED) values greater than 1.0. Flat sheet membranes were fabricated via the non-solvent induced phase separation (NIPS) technique. Four NIPS fabricated polymer membranes were evaluated: polysulfone, cellulose acetate, polyvinylidene fluoride (PVDF) fabricated with polyethylene glycol (PEG) as a pore-forming agent, and polybenzimidazole (PBI). The HSP approach successfully predicted membrane-solvent compatibility, with polysulfone (RED = 0.6) and cellulose acetate (RED = 0.9) dissolving completely within 24 h, while PVDF (RED = 1.9) and PBI (RED = 1.1) maintained structural integrity throughout a 7-day exposure period. Furthermore, PVDF demonstrated superior performance with minimal weight gain (3.0%), hydrophobic surface characteristics (122° water contact angle), and enhanced mechanical properties following DES exposure. Comprehensive chemical and morphological characterization confirmed PVDF’s chemical stability and revealed a surface-selective interaction mechanism involving simultaneous PEG (pore-forming agent) extraction and DES component adsorption. Adsorption kinetics followed pseudo-first-order behavior with reversible characteristics, best described by the Temkin isotherm model (R² = 0.9987). PVDF membranes-maintained separation functionality with average lignin rejection (75.2 ± 7.69%) and demonstrated filtration permeability of 2.0 ± 0.34 LMH/bar. This methodology provides a rational approach for membrane selection in emerging solvent systems, contributing to the advancement of sustainable separation technologies for DES-based biomass processing applications.

Science & Technology - Other Topics↗

DOE OSTI2021

Aqueous-soluble bipyridine cobalt($\tiny{II}$/$\tiny{III}$) complexes act as direct redox mediators in photosystem I-based biophotovoltaic devices

Sustainable energy production is critical for meeting growing worldwide energy demands. Due to its stability and reduction potential, photosystem I (PSI) is attractive as the photosensitizer in biophotovoltaic devices. Herein, we characterize aqueous and organic solvent soluble synthetic bipyridine-based cobalt complexes as redox mediators for PSI-based biophotovoltaics applications. Cobalt-based complexes are not destructive to protein and have appropriate midpoint potentials for electron donation to PSI. We report on PSI stability in organic solvents commonly used in biophotovoltaics. We also show the effects of a mixed organic solvent phase on PSI reduction kinetics, slowing reduction rates approximately 8–38 fold as compared to fully aqueous systems, with implications for dye regeneration rates in PSI-based biophotovoltaics. Further, we show evidence of direct electron transfer from cobalt complexes to PSI. Finally, we report on photocurrent generation from Co mediator-PSI biophotovoltaic devices. Taken together, we discuss the development of novel Co complexes and our ability to fine-tune their characteristics via functional groups and counteranion choice to drive interaction with a biological electron acceptor on multiple levels from redox midpoints, spectral overlap, and solvent requirements, among others. This work suggests that fine-tuning of redox active species for interaction with a biological partner is possible for the creation and improvement of low cost, carbon-neutral energy production in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Fast ion relaxation in ITER mediated by Alfvén instabilities

Abstract We address the critical issue for future burning plasmas of whether high-energy fusion products or auxiliary heating-beam ions will be confined for a sufficiently long time to compensate for thermal plasma energy losses. This issue can be mitigated by one of the most deleterious collective phenomena—the instability of low, sub-cyclotron frequency Alfvén eigenmodes (AEs), such as toroidicity-induced AEs and reversed-shear AEs in the ITER steady-state scenario. Using a revised quasi-linear (QL) theory applied to energetic particle (EP) relaxation in the presence of AEs, we find that the AE instabilities can affect both neutral beam ions and alpha particles, although the resulting fast ion transport is expected to be modest if classical particle slowing down is assumed. On the other hand, the QL theory predicts that the AE amplitudes will be enhanced by the background microturbulence, although this topic remains outside our scope due to the significant numerical effort required to evaluate these effects. We report our results for EP relaxation dynamics obtained utilizing several tools: (i) a comprehensive linear stability study of the sub-cyclotron Alfvénic spectrum as computed by ideal magnetohydrodynamic NOVA simulations for the AE eigenproblem, (ii) drift kinetic NOVA-C calculations for wave–particle interaction and AE growth/damping rates, and (iii) predictive QL modeling coupled with the global transport code TRANSP to assess the EP relaxation on the equilibrium timescale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1987

Vertical temperature gradients on Uranus - Implications for layered convection

Analyses of Voyager IR spectroscopy and radio occultation measurements confirm ground-based observations that the deep lapse rate of Uranus exceeds that for an adiabat of H2 in thermodynamic equilibrium. However, in approximately the same region of the atmosphere, Voyager IR and ground-based observations also indicate that the ratio of ortho to para hydrogen is near the equilibrium value. These two sets of observations can be reconciled by postulating the existence of rapid convective overturning within layers which are thin in comparison to a pressure scale height. Two forms of layered convection are examined. In one case, deposition of kinetic energy results in thin, rapidly overturning layers. Possible kinetic energy sources include braking waves and local instabilities. In the second case considered, molecular-weight discontinuities due to CH4 stratification stabilize the interfaces of thin layers. It is argued that both forms may be important in the convective portion of the Uranus atmosphere.

Gierasch, Peter J.↗

NASA NTRS1999

Ocean Turbulence: Two-Point Closure Model Momentum, Heat and Salt Vertical Diffusivities in the Presence of Shear - Paper 3

In papers 1 and 2 we have presented the results of the most updated 1-point closure model for the turbulent vertical diffusivities of momentum, heat and salt, K(sub m,h,s). In this paper, we derive the analytic expressions for K(sub m,h,s) using a new 2-point closure model that has recently been developed and successfully tested against some approx. 80 turbulence statistics for different flows. The new model has no free parameters. The expressions for K(sub m, h. s) are analytical functions of two stability parameters: the Turner number R(sub rho) (salinity gradient/temperature gradient) and the Richardson number R(sub i) (temperature gradient/shear). The turbulent kinetic energy K and its rate of dissipation may be taken local or non-local (K-epsilon model). Contrary to all previous models that to describe turbulent mixing below the mixed layer (ML) have adopted three adjustable "background diffusivities" for momentum. heat and salt, we propose a model that avoids such adjustable diffusivities. We assume that below the ML, K(sub m,h,s) have the same functional dependence on R(sub i) and R(sub rho) derived from the turbulence model. However, in order to compute R(sub i) below the ML, we use data of vertical shear due to wave-breaking measured by Gargett et al. (1981). The procedure frees the model from adjustable background diffusivities and indeed we use the same model throughout the entire vertical extent of the ocean. Using the new K(sub m,h, s), we run an O-GCM and present a variety of results that we compare with Levitus and the KPP model. Since the traditional 1-point (used in papers 1 and 2) and the new 2-point closure models used here represent different modeling philosophies and procedures, testing them in an O-GCM is indispensable. The basic motivation is to show that the new 2-point closure model gives results that are overall superior to the 1-point closure in spite of the fact that the latter rely on several adjustable parameters while the new 2-point closure has none. After the extensive comparisons presented in papers 1 and 2, we conclude that the new model presented here is overall superior for it not only is parameter free but also 2 because is part of a more general turbulence model that has been previously successfully tested on a wide variety of other types of turbulent flows.

Canuto, V. M.↗

NASA NTRS2005

In-Situ Heating Decrease Kinetics of Aliphatic Hydrocarbons in Tagish Lake Meteorite by Micro-FTIR

Carbonaceous chondrites are known to contain up to 3wt.% C, the major part of which corresponds to a macromolecular organic fraction. Chondritic organic matter is based on small aromatic units, cross-linked by short aliphatic chains rather than large clusters of polyaromatic structures. Two main characteristic features of those organics measured by FTIR are: (1) an equivalent intensity of the asymmetric stretching mode absorptions for CH3 (2960/cm) and CH2 (2920/cm) and (2) a lack of aromatic CH-stretching mode (3040/cm). Tagish Lake is a new type of water- and carbon-rich type 2 carbonaceous chondrite. Its total carbon content is approx. 5 wt%, of which the organic carbon content reaches approx. 1.3 wt%. Tagish Lake may have never experienced temperatures higher than 120 C after formation of organics based on the disappearance of infrared (IR) organic peaks in step heating experiments. Here we report in-situ kinetic heating experiments of organics in Tagish Lake by micro-FTIR to characterize the nature of aliphatic hydrocarbons and their thermal stabilities.

Kebukawa, Y.↗

NASA NTRS2019

Nonmodal Growth of TravelingWaves on Blunt Cones at Hypersonic Speeds

The existing database of transition measurements in hypersonic ground facilities has established that, as the nosetip bluntness is increased, the onset of boundary layer transition over a circular cone at zero angle of attack shifts downstream. However, this trend is reversed at sufficiently large values of the nose Reynolds number, so that the transition onset location eventually moves upstream with a further increase in nose-tip bluntness. Because modal amplification is too weak to initiate transition at moderate-to-large bluntness values, nonmodal growth has been investigated as the potential basis for a physics-based model for the frustum transition. The present analysis investigates the nonmodal growth of traveling disturbances initiated within the nose-tip vicinity that peak within the entropy layer. Results show that, with increasing nose bluntness, both planar and oblique traveling disturbances experience appreciable energy amplification up to successively higher frequencies. For moderately blunt cones, the initial nonmmodal growth is followed by a partial decay that is more than overcome by an eventual, modal growth as Mack-mode waves. For larger bluntness values, the Mack-mode waves are not amplified anywhere upstream of the experimentally measured transition location, but the traveling modes still undergo a significant amount of nonmodal growth. This finding does not provide a definitive link between optimal growth and the onset of transition, but it is qualitatively consistent with the experimental observations that frustum transition in the absence of sufficient Mack-mode amplification implies a double peak in disturbance amplification and the appearance of transitional events above the boundary-layer edge.

Hypersonic speed↗

DOE OSTI2021

Analytic quasi-steady evolution of marginally unstable kinetic plasma instabilities in the presence of drag and scattering

The 1D bump-on-tail problem is studied in order to determine the influence of drag on quasi-steady solutions near marginal stability (1-γ d /γ L << 1) when effective collisions are much larger than the instability growth rate (ν>>γ). In this common tokamak regime, it is rigorously shown that the paradigmatic Berk–Breizman cubic equation for the nonlinear mode evolution reduces to a much simpler differential equation, dubbed the time-local cubic equation, which can be solved directly. It is found that in addition to increasing the saturation amplitude, drag introduces a shift in the apparent oscillation frequency by modulating the saturated wave envelope. Furthermore, excellent agreement is found between the analytic solution for the mode evolution and both the numerically integrated Berk–Breizman cubic equation and fully nonlinear 1D Vlasov simulations. Experimentally isolating the contribution of drag to the saturated mode amplitude for verification purposes is explored but complicated by the reality that the amount of drag cannot be varied independently of other key parameters in realistic scenarios. While the influence of drag is modest when the ratio of effective drag to effective scattering α/ν is very small, it can become substantial when α/ν ≳ 0.5, suggesting that drag should be accounted for in quantitative models of fast-ion-driven instabilities in fusion plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Fundamental Science for Enhancing the Durability of Photoelectrodes for Solar Fuels Production

During the award period, we performed a series of investigations to address a key bottleneck in solar-driven fuel production, which is materials stability. Regardless of the activity of electrocatalysts or selectivity of products, or efficiency of the light absorbers, if the systems are not stable then there is no ultimate technological relevance for solar fuels production. Degradation of semiconductor photoelectrodes is a well-known, long-recognized impediment to implementation of practical stable solar fuels systems. Thus, we aimed to define the thermodynamics and kinetics of the (electro)chemical processes that underpin corrosion of semiconductor photoelectrodes. We also sought to develop protective coatings and kinetic control strategies to extend durability of semiconductor photoelectrodes.

14 SOLAR ENERGY↗

DOE OSTI2025

Interlayer Design for Halide Electrolytes in All‐Solid‐State Lithium Metal Batteries

Abstract All‐solid‐state lithium‐metal batteries (ASSLMBs) are promising for transportation electrification due to their superior safety and high energy density. Lithium halide electrolytes provide excellent processing flexibility, high ionic conductivity, and anodic stability (>4.1 V), making them highly compatible with high‐voltage cathodes, surpassing sulfide electrolytes (<2.1 V). Nevertheless, halide electrolytes suffer from low cathodic stability and form an electronically conductive interphase with lithium, resulting in a critical current density (CCD) of nearly zero. Herein, Li 3 YbCl 6 electrolytes are synthesized that are kinetically stable with lithium by forming an electronic insulating solid electrolyte interphase. Guided by critical overpotential criteria, a PI 3 interlayer is designed that transforms into Li 6 PI 3 upon contact with lithium, substantially reducing the interfacial resistance of Li 3 YbCl 6 against lithium to 34 Ω and achieving a high critical overpotential of 114 mV. By substituting Yb with Lu, Li 3 LuCl 6 electrolytes with Li 6 PI 3 interlayers reach a CCD of 1.0 mA cm −2 at a capacity of 1.0 mAh cm −2 , comparable to sulfide electrolytes but with higher oxidation stability. Additionally, Li 6 PI 3 enables stable cycling of Li//Li cells with Li 3 LuCl 6 electrolytes at 0.5 mA cm −2 for 400 cycles and maintains 86.5% capacity in Li//LiCoO 2 cells after 220 cycles at 30 °C, paving the way for high‐performance ASSLMBs.

Chemistry↗