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At least 289 records · Page 16

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DOE OSTI2024

Pore-Filling Induced Solid Electrolyte Failure of Ti-Doped Na 3 Zr 2 Si 2 PO 12 Characterized by Operando Synchrotron X-Ray Tomography

Solid-state batteries (SSBs), particularly those utilizing sodium metal, are emerging as a promising technology due to their potential for enhanced safety, higher energy density, and longer cycle life. NASICON (Na superionic conductor) materials, known for their robust crystalline structure and high ionic conductivity, are pivotal in the development of efficient sodium all-solid-state batteries. These materials exhibit high room-temperature ionic conductivity and electrochemical stability, making them ideal for various applications. Research has focused on improving NASICON's ionic conductivity and stability through doping, interface regulation, and composite anode design. Recent advancements include Ti-doped Na 3 Zr 2 Si 2 PO 12 (Ti-NZSP), which demonstrates improved surface stability, higher ionic conductivity, and increased critical current density. However, challenges such as Na dendrite formation and mechanical integrity under operational conditions persist. Advanced imaging techniques like operando synchrotron X-ray tomography have provided insights into failure mechanisms, revealing that pore-filling and dendrite growth are significant issues. Understanding these processes is essential for enhancing the performance and safety of Na-based SSBs. Here, this study underscores the need for continued research to address these challenges and develop reliable, high-performance solid-state electrolytes for future energy storage solutions.

25 ENERGY STORAGE↗

DOE OSTI2025

Lithium‐Containing Hybrid SEI Layer Enabling High Mass Loading and Anode‐Less Sodium Metal Batteries

Abstract The continuous rupturing and rebuilding of unstable solid electrolyte interphase (SEI) layer during cycling would block Na + diffusion and induce Na dendrite formation, ultimately limiting the practical application of high‐energy‐density sodium metal batteries. Herein, a hybrid SEI layer containing Li‐species is dexterously constructed on the surface of sodium metal anode. Li‐containing inorganic components (Li 3 N, LiF, and Li 2 CO 3 ) are introduced to stabilize the Na/electrolyte interface and enhance the mechanical and diffusion kinetic properties of the SEI layer, which can reduce the side reactions and gas generation, regulate Na + flux during cycling and promote rapid Na + migration for uniform dendrite‐free Na deposition. As a result, the constructed Na symmetric cells achieve low overpotential and long cycle life of 5900, 1800, and 500 h at current densities of 3, 10, and 30 mA cm −2 , respectively. Furthermore, the full cells paired with the Na₃V₂(PO₄)₃ cathode demonstrate high specific capacity and excellent cycle stability, even at an ultra‐high cathode loading of 39.3 mg cm −2 and a low N/P ratio (negative/positive electrode capacity ratio of 1.21).

Xia, Li [State Key Laboratory of Physical Chemistr↗

DOE OSTI2024

Nitrogen-Doped Graphene-Like Carbon Intercalated MXene Heterostructure Electrodes for Enhanced Sodium- and Lithium-Ion Storage

MXene is investigated as an electrode material for different energy storage systems due to layered structures and metal-like electrical conductivity. Experimental results show MXenes possess excellent cycling performance as anode materials, especially at large current densities. However, the reversible capacity is relatively low, which is a significant barrier to meeting the demands of industrial applications. This work synthesizes N-doped graphene-like carbon (NGC) intercalated Ti 3 C 2 T x (NGC-Ti 3 C 2 T x ) van der Waals heterostructure by an in situ method. The as-prepared NGC-Ti 3 C 2 T x van der Waals heterostructure is employed as sodium-ion and lithium-ion battery electrodes. For sodium-ion batteries, a reversible specific capacity of 305 mAh g -1 is achieved at a specific current of 20 mA g -1 , 2.3 times higher than that of Ti 3 C 2 T x . For lithium-ion batteries, a reversible capacity of 400 mAh g -1 at a specific current of 20 mA g -1 is 1.5 times higher than that of Ti 3 C 2 T x . Both sodium-ion and lithium-ion batteries made from NGC-Ti 3 C 2 T x shows high cycling stability. The theoretical calculations also verify the remarkable improvement in battery capacity within the NGC-Ti 3 C 2 O 2 system, attributed to the additional adsorption of working ions at the edge states of NGC. This work offers an innovative way to synthesize a new van der Waals heterostructure and provides a new route to improve the electrochemical performance significantly.

25 ENERGY STORAGE↗

DOE OSTI2025

Lithium‐Containing Hybrid SEI Layer Enabling High Mass Loading and Anode‐Less Sodium Metal Batteries

The continuous rupturing and rebuilding of unstable solid electrolyte interphase (SEI) layer during cycling would block Na + diffusion and induce Na dendrite formation, ultimately limiting the practical application of high-energy-density sodium metal batteries. Herein, a hybrid SEI layer containing Li-species is dexterously constructed on the surface of sodium metal anode. Li-containing inorganic components (Li 3 N, LiF, and Li 2 CO 3 ) are introduced to stabilize the Na/electrolyte interface and enhance the mechanical and diffusion kinetic properties of the SEI layer, which can reduce the side reactions and gas generation, regulate Na + flux during cycling and promote rapid Na + migration for uniform dendrite-free Na deposition. As a result, the constructed Na symmetric cells achieve low overpotential and long cycle life of 5900, 1800, and 500 h at current densities of 3, 10, and 30 mA cm −2 , respectively. Furthermore, the full cells paired with the Na₃V₂(PO₄)₃ cathode demonstrate high specific capacity and excellent cycle stability, even at an ultra-high cathode loading of 39.3 mg cm −2 and a low N/P ratio (negative/positive electrode capacity ratio of 1.21).

Diffusion kinetic↗

DOE OSTI2026

Atomic-scale vacancy engineering unlocks basal-plane catalytic activity in metallic WSe 2 for reversible oxygen electrocatalysis

Two-dimensional metallic transition metal dichalcogenides offer high electrical conductivity and large surface areas for electrocatalysis, yet their inherent basal planes are catalytically inert. Here, we present an atomic-scale vacancy engineering strategy to activate the basal surfaces of metallic WSe 2 for reversible oxygen electrocatalysis. This approach, based on intentionally designed substitutional metal doping, promotes the spontaneous formation of selenium vacancies while preserving the metallic 1 T′ phase, thereby creating highly reactive and oxygen-affinitive sites. Density functional theory calculations reveal that these vacancy-mediated metal complexes dramatically lower the energy barriers for initial oxygen adsorption, enabling dissociative oxygen adsorption. Operando and ex-situ spectroscopic analyses confirm that vacancy-mediated metal complexes transform into dynamic Se/W-oxide intermediates under operating conditions. Se/W-oxides on the surface experimentally and theoretically prove electrocatalytic activity and reversibility. Applying this strategy in lithium–oxygen batteries, the basal-plane activated WSe 2 shows high discharge capacities (9868 mA h g −1 , corresponding to 3947 mA h g$^{-1}_{cathode}$), impressive cycle retention over 550 cycles at 1000 mA h g −1 , and outstanding rate–capability over a wide current–density range (100–3000 mA g −1 ) during 256 cycles.

2D materials↗

DOE OSTI2024

Low‐Temperature and High‐Rate Rechargeable Aluminum Batteries Enabled by Ternary Eutectic Electrolytes

Abstract Rechargeable aluminum batteries (RABs) have garnered extensive scientific attention as a promising alternative chemistry due to the inherent advantages associated with aluminum (Al) metal anodes, including their high theoretical capacities, cost‐effectiveness, environmental friendliness, and inherent non‐flammable properties. Nonetheless, the practical energy density of RABs is constrained by the electrolytes that support lower operational voltage windows. Herein, we report a ternary eutectic electrolyte composed of 1‐ethyl‐3‐methylimidazolium chloride ([C 2 C 1 im]Cl):1‐butyl‐3‐methylimidazolium chloride ([C 4 C 1 im]Cl):aluminum chloride (AlCl 3 ) for the application of RABs. The electrolyte exhibits a high operational potential window (~3 V vs. Al/Al 3+ on SS 316) and high ionic conductivity (~8.3 mS cm −1 ) while exhibiting only a low temperature glass transition at −65 °C suitable for all‐climate conditions. Al||graphene nanoplatelets cell delivers a high capacity of ~117 mAh/g, and ~43 mAh/g at a very high current densities of 1 A/g and 5 A/g, respectively. The cells render a reversible capacity of 20 mAh/g at −20 °C and 17 mAh/g at −40 °C, indicating their suitability for operation under extreme environmental conditions. We comprehensively evaluated the design and optimization of carbon paper‐based battery systems. The ternary eutectic electrolyte demonstrates exceptional electrochemical performance, thus signifying its substantial potential for utilization in high‐performance energy storage systems in all climates.

Vadthya, Raju↗

DOE OSTI2024

Upcycling Linear Low-Density Polyethylene Waste into Graphene for High Mass Loading Supercapacitors

Polyethylene is notoriously difficult to upcycle because it decomposes into light gases at approximately 350-400 °C which prevents processing it at higher temperatures to convert it into electrode materials. We address this challenge by using an air-based, thermos-oxidative process, which heats linear low-density polyethylene (LLDPE) just below the decomposition point to initiate oxidation and cross-linking of LLDPE alkyl chains. These molecular transformations allow LLDPE to be graphenized at 950 °C without decomposing. The LLDPE-derived graphene (LLDPE-G) has a BET specific surface area up to 1,800 m2/g and Raman ID/IG ratio of 0.85. When used as electrode material for a symmetric supercapacitor with the 1 M H2SO4 electrolyte, LLDPE-G possesses an specific capacitance up to 175 F/g at mass loading of 20 mg/cm2, yielding an areal capacitance of 3.5 F/cm2. The cycling stability with capacitance demonstrates a retention of 95.8% after 100,000 cycles at high current density of 4.0 A/g.

Gao, Yuan↗

DOE OSTI2026

Mitigating Hydrogen-Induced Degradation of Iridium Anodes in Proton Exchange Membrane Water Electrolyzers

One promising method for reducing precious metal usage in proton exchange membrane water electrolysis is lowering iridium (Ir) loading at the anode. However, low-loading Ir catalysts often suffer from poor stability under high current densities. In this study, hydrogen (H2) crossover from the cathode to the anode is identified as a key degradation pathway. Temperature-programmed reduction confirms the reduction of IrO2 at 80 °C in a hydrogen environment, highlighting the vulnerability of IrO2-based catalysts to H2 exposure. To mitigate this effect, palladium (Pd) is introduced as an anode additive, acting as an H2 oxidation catalyst and mitigating IrO2 reduction. This protective role is verified by inductively coupled plasma optical emission spectroscopy and in situ X-ray absorption spectroscopy, showing significantly suppressed Ir dissolution at 80 °C under H2 flow when an O-covered Pd surface is present at oxygen evolution reaction potentials. Results from the current study identify a new strategy in improving activity and durability of catalysts in electrolyzers.

58 GEOSCIENCES↗

DOE OSTI2024

Field-free deterministic switching of all–van der Waals spin-orbit torque system above room temperature

Two-dimensional van der Waals (vdW) magnetic materials hold promise for the development of high-density, energy-efficient spintronic devices for memory and computation. Recent breakthroughs in material discoveries and spin-orbit torque control of vdW ferromagnets have opened a path for integration of vdW magnets in commercial spintronic devices. However, a solution for field-free electric control of perpendicular magnetic anisotropy (PMA) vdW magnets at room temperatures, essential for building compact and thermally stable spintronic devices, is still missing. Here, we report a solution for the field-free, deterministic, and nonvolatile switching of a PMA vdW ferromagnet, Fe 3 GaTe 2 , above room temperature (up to 320 K). We use the unconventional out-of-plane anti-damping torque from an adjacent WTe 2 layer to enable such switching with a low current density of 2.23 × 10 6 A cm –2 . This study exemplifies the efficacy of low-symmetry vdW materials for spin-orbit torque control of vdW ferromagnets and provides an all-vdW solution for the next generation of scalable and energy-efficient spintronic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Lithium Dendrite-Free Li 7 N 2 I-LiOH Solid Electrolytes for High Energy Lithium Batteries

All-solid-state lithium batteries (ASSLBs) hold great potential to improve the safety and energy density of today’s lithium-ion batteries by using non-flammable inorganic solid electrolytes. Solid electrolytes (SEs) are believed to prevent Li dendrite growth because of high mechanical strength and high Li+ transference numbers. Significant advances in SE have been achieved, among which, Li7La3Zr2O12 (LLZO) and Li2S–P2S5 (LPS) are the most promising SEs for bulk-type solid-state lithium batteries because of high ionic conductivities (>10-4 S/cm2). However, in contrast to our expectations, the growth of lithium dendrites is not suppressed but is facilitated in LLZOs and LPSs regardless of dopants, porosity, and crystallinity of the electrolytes. Despite the unity Li transference number and over two-times of shear modulus than that of Li metal, the critical current densities for Li plating and stripping in these SEs are less than 1.0 mA cm-2, which is one-fourth to one-tenth of that in liquid electrolytes at room temperature. The incompatibility between LLZO and LPS with Li metal seriously limits the energy density of all-solid-state batteries. The mechanism for lithium dendrite formation and growth in SEs are still disputable. Lack of understanding of the Li dendrite formation mechanism seriously impeded the development of solid-state lithium batteries. The development of the criterion for Li dendrite suppression is essential for the success of solid electrolyte lithium batteries. In this project, a criterion for Li dendrite suppression will be developed through thermodynamics and kinetics analysis of lithium dendrite nucleation/growth, which will guide the solid-state electrolyte design. Li7N2I-LiOH, Li5NI2-LiOH and Li3YCl6 solid electrolyte with high ionic conductivity and low electronic conductivity were used to validate the criterion for lithium dendrite suppression. Different surface modifications were also explored to enhance the dendrite suppression capability of SSEs.

25 ENERGY STORAGE↗

DOE OSTI2026

Theory Guided Fine‐Tune of Strain Effects in Pt Ternary Alloy via Rare Earth Templating: Achieving High Performance PEMFCs Catalysts

The sluggish kinetics and insufficient durability of platinum-based catalysts remain crucial barriers limiting proton-exchange-membrane fuel cells (PEMFCs) deployment. Here, we report a theory-guided synthesis combined with rare-earth templating to realize a previously inaccessible Pt 5 Co-like phase with tailored atomic-scale strain. Guided by density functional theory (DFT) calculations, we identified that a Pt 5 Co-like sublayer can induce a unique mild compressive strain (−1.24%) to the Pt(111) shell and an optimal *OH binding energy shift (ΔE ≈ 0.11 eV). This shift positions the alloy catalyst near the apex of the oxygen reduction reaction activity volcano. This prediction guided the synthesis of ternary alloy Pt 5 (Ce)Co@Pt multilayer nanoparticles, featuring a Ce-stabilized core, a Pt 5 Co-like sublayer, and a Pt-rich shell. This catalyst demonstrates both exceptionally high activity and durability, achieving a mass activity of 2.6 A∙mg Pt −1 in rotating disk electrode testing. In fuel cell membrane electrode assembly tests, Pt 5 (Ce)Co@Pt achieves a current density of 1.9 A∙cm −2 at 0.7 V under heavy-duty vehicle conditions. Remarkably, it maintains 1.2 A∙cm −2 after 1 80 000 AST cycles, doubling the U.S. DOE 2025 target. This work demonstrates a rational design strategy that DFT-guided strain engineering integrates with rare-earth templating to advance Pt-based catalysts for fuel cell applications.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2025

A Universal Design of Lithium Anode via Dynamic Stability Strategy for Practical All‐Solid‐State Batteries

Abstract All‐solid‐state Li‐metal battery (ASSLB) chemistry with thin solid‐state electrolyte (SSE) membranes features high energy density and intrinsic safety but suffers from severe dendrite formation and poor interface contact during cycling, which hampers the practical application of rechargeable ASSLB. Here, we propose a universal design of thin Li‐metal anode (LMA) via a dynamic stability strategy to address these issues. The ultra‐thin LMA (20 μm) is in situ constructed with uniform highly Li‐ion conductive solid‐electrolyte interphase and composite‐polymer interphase (CPI) via electroplating process. As a result, the passivation layer with poor Li‐ion conduction on Li anode can be dissolved and small surface resistance can be achieved due to the good compatibility of CPI to SSEs. The cycling of Li symmetric cell with Li 6 PS 5 Cl thin film electrolyte (<100 μm) shows a high critical current density of >2.0 mA cm −2 with excellent cycling stability at 1.0 mA cm −2 . The ASSLBs paring with Ni‐rich LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode demonstrated the feasibility of engineered LMA design by presenting good rate capability from 0.1 C to 1.0 C at room temperature, as well as long‐term cycling stability (81 % retention after 100 cycles). This work represents a general pathway to make thin dendrite‐free LMA available for high‐energy‐density ASSLBs.

Deng, Tao [Department of Chemical and Biomolecular↗

DOE OSTI2025

A Universal Design of Lithium Anode via Dynamic Stability Strategy for Practical All‐Solid‐State Batteries

Deng, Tao [Department of Chemical and Biomolecular↗

DOE OSTI2024

Upcycling Low Linear Density Polyethylene Waste into Turbostratic Graphene for High Mass Loading Supercapacitors

In this work, LLDPE was upcycled into a high quality turbostratic graphene using a pre-treatment step to oxidatively crosslink the polymer with the assistance of solid additives (KCl and K2CO3) that improve crosslinking by increasing the effective surface area of the polymer melt during processing. After this pretreatment step, the crosslinked polymer could then be carbonized and catalytically graphenized between 400-950 °C without complete decomposition of the material. The LLDPE derived graphene (LLDPE-G) obtained from this process has a Brunauer–Emmett–Teller (BET) specific surface area, up to 1800 m2g-1 and average Raman ID/IG and I2D/IG ratios of 0.85 and 0.57, respectively, indicating high quality graphene. When used as an electrode material in symmetric supercapacitors, LLDPE-G possesses an outstanding specific capacitance up to 175 Fg-1 at a mass loading of 20 mgcm-2, which is two times the commercial requirement, yielding an excellent areal capacitance of 3.5 Fcm-2. Moreover, LLDPE-G exhibits exceptional cycling stability with a capacitance retention of 95.8% after 100,000 cycles at a current density of 4.0 Ag-1. Additionally, the KCl and K2CO3 were recycled and reused over 3 complete cycles to make new LLDPE-G with the material quality and electrocapacitive performance retained and verified after each cycle. Our approach creates new opportunities for upcycling not only waste LLDPE but also other varieties of PE to high value graphene materials.

Gao, Yuan [NETL Site Support Contractor, National ↗

DOE OSTI2024

Wall heating by subcritical energetic electrons generated by the runaway electron avalanche source *

Abstract Subcritical energetic electrons (SEEs) produced by the runaway electron (RE) avalanche source at energies below the runaway threshold are found to be the primary contributor to surface heating of plasma-facing components (PFCs) during final loss events. This finding is supported by theoretical analysis, computational modeling with the Kinetic Orbit Runaway electrons Code (KORC), and qualitative agreement with DIII-D experimental observations. The avalanche source generates significantly more secondary electrons below the runaway threshold, which thermalize rapidly when well-confined. However, during a final loss event, the RE beam impacts the first wall, and SEEs are deconfined before they can thermalize. Additionally, because the energy deposition length decreases faster than energy, the deposited energy density, and thus the maximum PFC surface temperature change, is larger for SEEs than REs. KORC simulations employ an analytic first wall to model particle deconfinement onto a non-axisymmetric wall composed of individual tiles. PFC surface heating is calculated using a 1D model extended to include an energy-dependent deposition length scale. Simulations of DIII-D qualitatively agree with infrared (IR) imaging only when SEEs from the avalanche source are included. These results demonstrate that SEEs are the dominant contributor to PFC surface heating and indicate that the avalanche source plays a critical role in the PFC damage caused during final loss events. The prominence of SEEs also has important implications for interpreting IR imaging, one of the primary diagnostics for RE-wall interaction diagnosis, despite REs dominating the energy and current density. This result improves predictions of wall damage due to post-disruption REs to estimate material lifetime and design RE mitigation systems for ITER and future reactors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Fast oxygen redox enabled by flexible Al–O bonds in P2-type layered oxides for sodium batteries

Sodium-ion batteries (SIBs) exhibit significant potential for large-scale energy storage systems due to the abundance and low cost of sodium resources. Triggering lattice oxygen redox (LOR) in P2-type transition metal oxides is considered a promising approach to enhance energy density in SIB cathodes, providing high operating potential and substantial capacity. However, irreversible phase transitions associated with LOR, particularly from prisms (P-type stacking) to octahedrons (O-type stacking), lead to severe structural distortions and sluggish Na + diffusion kinetics. In this work, an Al-substitution strategy is proposed to suppress the formation of O-type stacking and instead promote the formation of a beneficial Z phase. Furthermore, the flexible Al-O bonds accommodate asymmetric variations in their occupied states during the sodiation process, mitigating local structural distortions through Al-O bond contraction. Stabilization of the local structure ensures the maintenance of a robust Na + diffusion pathway. As a result, the Al-substituted cathode achieves a low Na + diffusion barrier of 0.47 eV and delivers a capacity of 86 mAh/g even at a high current density of 1 A/g within 1.5–4.5 V, maintaining 62.5% capacity retention over 100 cycles.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Zn 2+ -mediated catalysis for fast-charging aqueous Zn-ion batteries

Rechargeable aqueous zinc-ion batteries (AZIBs), renowned for their safety, high energy density and rapid charging, are prime choices for grid-scale energy storage. Historically, ion-shuttling models centring on ion-migration behaviour have dominated explanations for charge/discharge processes in aqueous batteries, like classical ion insertion/extraction and pseudocapacitance mechanisms. However, these models struggle to account for the exceptional performance of AZIBs compared to other aqueous metal-ion batteries. Here, in this study, we present a catalysis model elucidating the Zn 2+ anomaly in aqueous batteries, explaining it through the concept of adsorption in catalysis. Such behaviour can serve the charge/discharge role, predominantly dictated by solvated metal cations and cathode materials. First-principles calculations suggest optimal adsorption/desorption behaviour (water dissociation process) with the Zn 2+ -vanadium nitride (VN) combination. Experimentally, AZIBs implementing VN cathodes demonstrate fast-charging kinetics, showing a capacity of 577.1 mAh g -1 at a current density of 300,000 mA g -1 . The grasp of catalysis steps within AZIBs can drive solutions beyond state-of-the-art fast-charging batteries.

25 ENERGY STORAGE↗

DOE OSTI2025

Minimization of Cathode|Solid-Electrolyte Interfacial Delamination through the Application of Interphase Layers

Next-generation lithium-ion batteries are expected to use solid electrolytes (SEs) to enable higher energy density and extreme fast-charge capabilities. One major mode of degradation at the cathode|SE interface is delamination between the cathode active materials and SEs, which leads to performance decay. Experimental observations indicate that implementation of interphase layers can minimize the cathode|SE delamination induced capacity fade. A multiscale computational methodology is developed here to investigate the applicability of boron substituted lithium carbonate (Li 2+x B x C 1–x O 3 , x = 0.5, or LBCO) to minimize the delamination at the cathode|SE interface. Atomistic simulations indicate that the fracture energies at both the cathode|LBCO and LBCO|SE interfaces are higher than those at the cathode|SE interface, which reduces the extent of delamination. Mesoscale simulations indicate that, apart from increasing the fracture energy, decreasing the evolution of strain energy by lowering the elastic modulus of the interphase layer can also minimize the extent of delamination at the cathode|SE interface. However, the adoption of an interphase layer with high ionic conductivity is necessary to minimize the ohmic losses during operation at higher current densities. This study provides guidance on selecting interphase layers with specific properties and thicknesses to minimize both interfacial delamination and impedance growth.

LBCO↗