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DOE OSTI2023

Constructing “Li-rich Ni-rich” oxide cathodes for high-energy-density Li-ion batteries

The current exploration of high-energy-density cathode materials for Li-ion batteries is mainly concentrated on either so-called “Li-rich” or “Ni-rich” oxides. However, both are suffering from formidable practical challenges. Here, we combine these two concepts to obtain “Li-rich Ni-rich” oxides in pursuit of more practical high-energy-density cathodes. As a proof of concept, we synthesized an array of Li 1+y Ni( 3-5y)/3 Mo 2y/3 O 2 oxides, whose structures were identified to be the coexistence of LiNiO 2 -rich and Li 4 MoO 5 -rich domains with the aid of XRD, TEM, and NMR techniques. Such an intergrowth structure of 5–20 nm size enables excellent mechanical and structural reversibility for the layered rock-salt LiNiO 2 -rich domain upon cycling thanks to the robust cubic rock-salt Li 4 MoO 5 -rich domain enabling an “epitaxial stabilization” effect. As a result, we achieved high capacities (>220 mA h g -1 ) with Ni contents as low as 80%; the Li 1.09 Ni 0.85 Mo 0.06 O 2 member (y = 0.09) shows much improved cycling performances (91% capacity retention for 100 cycles at C/10) compared with pure LiNiO 2 . Further, this work validates the feasibility of constructing Li-rich Ni-rich compounds in the form of intergrowing domains and hence unlocks vast possibilities for future cathode design.

25 ENERGY STORAGE↗

DOE OSTI2021

A review of thermal physics and management inside lithium-ion batteries for high energy density and fast charging

Traditionally it has been assumed that battery thermal management systems should be designed to maintain the battery temperature around room temperature. That is not always true as lithium-ion battery (LIB) R&D is pivoting towards the development of high energy density and fast charging batteries. Therefore, it is necessary to have a comprehensive review of thermal considerations for LIBs targeted for high energy density and fast charging, i.e., the optimal thermal condition, thermal physics (heat transport and generation) inside the battery, and thermal management strategies. As the energy density and charge rate increases, the optimal battery temperature can shift to be higher than room temperature. In the first part of the review various sources of heat generation inside LIBs and various approaches to minimizing battery heat generation are summarized. The importance of heat of mixing due to ion diffusion during fast charging is also highlighted. To improve the temperature uniformity and avoid excessive internal temperature rise, heat transfer inside the battery needs to be enhanced, and reducing the thermal contact resistance between the electrodes and separator can significantly increase the effective thermal conductivity of batteries. In the second part of the review various challenges and latest developments related to thermal transport and properties of LIBs are discussed. Finally, a summary of latest advancement on smart control of internal temperature of LIBs is discussed as depending on the ambient temperature and the optimal temperature; the battery heat needs to be retained or dissipated to elevate or avoid temperature rise.

25 ENERGY STORAGE↗

DOE OSTI2022

Volumetric energy density impact on mechanical properties of additively manufactured 718 Ni alloy

The 718 Ni-based superalloy has gained enormous attention in the additive manufacturing community for its great weldability, allowing for complex geometries to be formed, and its superb mechanical strength. Here we explore the influence of a wide range of major build parameters on microstructures and mechanical properties of 718 Ni alloys. Volumetric energy density appears to be one of the major parameters that captures the relationship between energy input and measured mechanical properties and microstructures of the alloys. A threshold energy density was identified below which the properties of the additively manufactured specimen degrade substantially. Finally, the influence of energy density on the quality of the built specimen simulated using Flow3D AM correlates well with the experimental results.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Tin-graphene tubes as anodes for lithium-ion batteries with high volumetric and gravimetric energy densities

Limited by the size of microelectronics, as well as the space of electrical vehicles, there are tremendous demands for lithium-ion batteries with high volumetric energy densities. Current lithium-ion batteries, however, adopt graphite-based anodes with low tap density and gravimetric capacity, resulting in poor volumetric performance metric. Here, by encapsulating nanoparticles of metallic tin in mechanically robust graphene tubes, we show tin anodes with high volumetric and gravimetric capacities, high rate performance, and long cycling life. Pairing with a commercial cathode material LiNi0.6Mn0.2Co0.2O2, full cells exhibit a gravimetric and volumetric energy density of 590 W h Kg-1 and 1,252 W h L-1 , respectively, the latter of which doubles that of the cell based on graphite anodes. This work provides an effective route towards lithium-ion batteries with high energy density for a broad range of applications.

25 ENERGY STORAGE↗

DOE OSTI2024

Extended Fayans energy density functional: optimization and analysis

The Fayans energy density functional (EDF) has been very successful in describing global nuclear properties (binding energies, charge radii, and especially differences of radii) within nuclear density functional theory. In a recent study, supervised machine learning methods were used to calibrate the Fayans EDF. Building on this experience, in this work we explore the effect of adding isovector pairing terms, which are responsible for different proton and neutron pairing fields, by comparing a 13D model without the isovector pairing term against the extended 14D model. At the heart of the calibration is a carefully selected heterogeneous dataset of experimental observables representing ground-state properties of spherical even–even nuclei. To quantify the impact of the calibration dataset on model parameters and the importance of the new terms, we carry out advanced sensitivity and correlation analysis on both models. The extension to 14D improves the overall quality of the model by about 30%. The enhanced degrees of freedom of the 14D model reduce correlations between model parameters and enhance sensitivity.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

High energy density picoliter-scale zinc-air microbatteries for colloidal robotics

The recent interest in microscopic autonomous systems, including microrobots, colloidal state machines, and smart dust, has created a need for microscale energy storage and harvesting. However, macroscopic materials for energy storage have noted incompatibilities with microfabrication techniques, creating substantial challenges to realizing microscale energy systems. Here, we photolithographically patterned a microscale zinc/platinum/SU-8 system to generate the highest energy density microbattery at the picoliter (10 −12 liter) scale. The device scavenges ambient or solution-dissolved oxygen for a zinc oxidation reaction, achieving an energy density ranging from 760 to 1070 watt-hours per liter at scales below 100 micrometers lateral and 2 micrometers thickness in size. The parallel nature of photolithography processes allows 10,000 devices per wafer to be released into solution as colloids with energy stored on board. Within a volume of only 2 picoliters each, these primary microbatteries can deliver open circuit voltages of 1.05 ± 0.12 volts, with total energies ranging from 5.5 ± 0.3 to 7.7 ± 1.0 microjoules and a maximum power near 2.7 nanowatts. We demonstrated that such systems can reliably power a micrometer-sized memristor circuit, providing access to nonvolatile memory. We also cycled power to drive the reversible bending of microscale bimorph actuators at 0.05 hertz for mechanical functions of colloidal robots. Additional capabilities, such as powering two distinct nanosensor types and a clock circuit, were also demonstrated. The high energy density, low volume, and simple configuration promise the mass fabrication and adoption of such picoliter zinc-air batteries for micrometer-scale, colloidal robotics with autonomous functions.

Robotics↗

DOE OSTI2026

Upcycling mixed cathode materials to high-energy-density LiFe 0.75 Mn 0.25 PO 4

To address the demand for next-generation cathode materials with high energy density, upcycling LiFePO 4 into LiFe 0.75 Mn 0.25 PO 4 has attracted considerable attention. Nevertheless, existing strategies have yet to achieve both morphology and full elemental recovery under mild ambient conditions. Here, we report an upcycling route that can address this issue by combining leaching and a high-temperature treatment process. The upcycled LiFe 0.75 Mn 0.25 PO 4 exhibits enlarged lattice spacing and a high discharge plateau, and it delivers an energy density of 563.7 Wh/kg, 40.3 Wh/kg higher than recycled LiFePO 4 , which indicates the high value of the proposed upcycling strategy. At 1 C, LiFe 0.75 Mn 0.25 PO 4 also exhibits excellent cycling stability of 91% over 700 cycles. Techno-economic analysis also indicates impressive economic and environmental benefits, including 10.4% less raw materials usage and 12.2% less energy consumption and wastewater generation. This work demonstrates a scalable and economic upcycling strategy and provides a promising pathway for sustainable battery upcycling compatible with industrial conditions.

LMFP↗

DOE OSTI2023

Transport Properties of Magnetized High-Energy Density Plasma (Final Project Report)

This report summarizes results of project DE-SC0016159 "Transport Properties of Magnetized High-Energy-Density Plasma,'' which ran from 7/15/2016 - 7/14/2021. The primary objectives of the work, as stated in the original proposal, were to develop a theory that describes transport coefficients in magnetized high energy density plasmas and to test the theory with molecular dynamics (MD) simulations. The science challenge is that strong ion coupling, strong magnetization of electrons, and partial degeneracy of electrons, cause the system to be in a regime that is not well described by current theory. The particular processes that were to be investigated include: ion stopping power, diffusion, electron-ion temperature relaxation, thermal conduction and viscosity. All of the primary research objectives were accomplished during the course of this work. In addition, some unexpected results were discovered along the way that led to new and productive research directions. This work resulted in 17 publications in well-respected peer-reviewed journals (primarily Physics of Plasmas and Physical Review E), and 2 more are being prepared for publication. A few of these were selected as Editor's Picks and one was published as a Rapid Communication. Highlights of the research results include: Transport phase space: The first identification of the parameter space that defines fundamental transport regimes in terms of the Coulomb coupling and magnetization parameters. Mean force kinetic theory: Systematic derivation of a kinetic theory for strongly coupled plasmas based on a new expansion parameter of the BBGKY hierarchy. This provided the derivation of a theory that we had previously posed phenomenologically, and also revealed a new term that captures the equation of state properties at all coupling strengths. Transverse friction force: Discovery that the friction force on a test charge in a strongly magnetized plasma includes a component that is perpendicular to the motion of the test charge in the plane defined by the velocity and magnetic field vectors. Gyrofriction force: Discovery that the friction force on a test charge in a plasma that is both strongly magnetized and strongly coupled includes a component of the force in the direction of the Lorentz force. Kinetic theory for warm dense matter: Extension of the mean force kinetic theory to include partial electron degeneracy, so that it applies to warm dense matter.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

A Flexible, Redox-Active, Aqueous Electrolyte-Based Asymmetric Supercapacitor with High Energy Density Based on Keratin-Derived Renewable Carbon

This work exploits the advantage of asymmetric configuration over symmetric supercapacitor in designing high energy density flexible devices from two active electrode materials–keratin-based renewable-resource hierarchically porous carbon and hydrous ruthenium oxide (RuO 2 ). Here, the asymmetric device exhibits significantly high capacitance. Conventional estimation of energy storage parameters, however, cannot be applied for devices with a Faradaic energy storage contribution via redox charge transfer mechanism. Therefore, this work applies a precise measurement of pseudocapacitance contribution at various scan rates to correct the device data that reveals effective capacitance of 120 F g –1 with the energy density of 37 W h kg –1 at 776 W kg –1 . It also retains excellent rate capability, >74% at high current density 25 A g –1 . The charge storage activity and device stability can be further enhanced by introducing redox-active electrolytes that improve specific capacitance, but the rate capabilities deteriorate at high current densities. Further, the principle of asymmetric electrode design is applied to fabricate a bending-tolerant, flexible device by depositing active electrode material on wire-shaped current collector followed by coupling those separated with polyvinyl alcohol gel containing redox electrolyte; it yields 36.8 mF cm –1 specific capacitance at a 0.2 mA cm –1 current density.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Ultra-high energy density relativistic plasmas from nanostructures: scaling to ultra-high intensities (Final Report)

This project investigated the ultra-high energy density (UHED) regime of matter found in the center of stars, using a compact PW-class laser. These extreme conditions are typically only obtained in the laboratory in the central hot-spot of spherically imploded capsules in inertial confinement fusion experiments driven by the world’s largest lasers. We have shown that near-solid density arrays of aligned nanostructures can be volumetrically heated to multi-keV temperatures by irradiation at relativistic intensity with ultrafast laser pulses of modest energy, opening a path for the generation of UHED plasmas with compact lasers. This new UHED plasma generation approach promises to create an environment with extreme energy densities and degrees of ionization, record conversion of optical laser light into ultrafast x-ray pulses, gigantic magnetic fields and pressures, and directed beams of high energy particles . In this project we achieved record degree of ionization in volumetric heating solid density and near-solid density plasmas. Gold plasmas which spectra is characterized by L shell transition emission from ions with charge up to the Ne-like state, Au+ 72 were generated using ultrafast laser pulses of less than 10 J of energy from a compact laser focused to an intensity of ~ 3x10 21 Wcm -2 . We also conducted measurements to determine the heat penetration depth in Ni nanowire arrays as compared to Ni foil targets by monitoring the line emission of a Co buried tracer underneath a variable amount of Ni. The measurements revealed that the nanowire plasmas are roughly six times larger in depth than the solid density target plasmas. A result of this increased plasma in nanowire arrays is a greatly increased conversion of optical laser light into > 1 KeV x-rays, a record conversion efficiency of 20 %. Critical to the realization of the proposed experiments was the generation of ultrafast laser pulses with ultra-high contrast that can deposit the energy deep into the nanowire arrays before the nanowires explode to create a continuous plasma. Supporting the proposed experiments was the recent demonstration at Colorado State University of a Petawatt-class laser that emits 30 fs pulses at high repetition rates. The experiments combined this unique laser tool with a variety of tailored nanowire arrays fabricated in house and with an extensive suite of diagnostics. The experiments were accompanied by 3-dimensional particle-in-cell simulations and detailed atomic physics simulations with transient kinetics and radiation transport. The proposed research allowed us to continue training Ph.D students and post-docs with broad experience in HEDP Science.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Understanding implications of cathode architecture on energy density of solid-state batteries

Next generation solid-state batteries (SSB) will need to leverage high voltage cathodes, as well as metallic anodes to achieve the realistic performance targets necessary to replace liquid electrolyte-based batteries in cutting-edge applications including electric vehicles. However, limitations arising from mass and charge transports, kinetics and chemo-mechanical degradation at the electrode | electrolyte interface limit the performance of present day SSBs. Optimizing composite cathode architecture, which is an integral part of solid-state batteries, is vital to realize the high-energy density and high-performance goals for next-generation solid-state batteries. Additionally, cathode architecture needs to be optimized for high loadings of active material, well-percolated ion and electron transport pathways and increased resilience against electrochemical stresses. This paper provides a first report of framework for geometric modeling of composite cathode architectures and evaluates the impact of cathode architecture on cell-level energy density using hierarchical models. Packing around primary and secondary active material particles are simulated for a range of active material particle size and solid electrolyte size distributions in the composite cathode. Impact of packing architecture on processing parameters of a given cathode composition and thickness, as well as on achievable energy density is evaluated for a range of commonly used solid electrolyte and cathode materials. Overall, the proposed framework offers a facile exploratory methodology for establishing initial metrics for scalable processing of practical and competent SSBs.

25 ENERGY STORAGE↗

DOE OSTI2020

Designing a hybrid electrode toward high energy density with a staged Li + and PF 6 - deintercalation/intercalation mechanism

Existing lithium-ion battery technology is struggling to meet our increasing requirements for high energy density, long lifetime, and low-cost energy storage. Here, a hybrid electrode design is developed by a straightforward reengineering of commercial electrode materials, which has revolutionized the “rocking chair” mechanism by unlocking the role of anions in the electrolyte. Our proof-of-concept hybrid LiFePO 4 (LFP)/graphite electrode works with a staged deintercalation/intercalation mechanism of Li + cations and PF 6 - anions in a broadened voltage range, which was thoroughly studied by ex situ X-ray diffraction, ex situ Raman spectroscopy, and operando neutron powder diffraction. Introducing graphite into the hybrid electrode accelerates its conductivity, facilitating the rapid extraction/insertion of Li + from/into the LFP phase in 2.5 to 4.0 V. This charge/discharge process, in turn, triggers the in situ formation of the cathode/electrolyte interphase (CEI) layer, reinforcing the structural integrity of the whole electrode at high voltage. Consequently, this hybrid LFP/graphite-20% electrode displays a high capacity and long-term cycling stability over 3,500 cycles at 10 C, superior to LFP and graphite cathodes. Importantly, the broadened voltage range and high capacity of the hybrid electrode enhance its energy density, which is leveraged further in a full-cell configuration.

25 ENERGY STORAGE↗

DOE OSTI2021

A theoretical approach for transient shock strengthening in high-energy-density laser compression experiments

In high-energy-density shock compression experiments, the desired state of compression is typically achieved by passing shock waves through a sequence of different materials. Here, a theoretical approach for transiently strengthening such shocks passing through interfaces of experimentally relevant impedance ratios is examined. A semi-analytical method based on characteristics analysis is used to solve the problem of a shock passing from one material to another through an intermediate region of non-uniform impedance; by appropriately designing this region, a greater shock strength can be achieved in the second material for a finite duration than in the absence of this region. When a shock passes into a material of higher impedance, the shock strengthening increases to a maximum before decreasing to an asymptotic value as the strength of the incident shock is increased. For shocks passing into materials of decreasing impedance, the shock strengthening increases monotonically as the strength of the incident shock is increased when the impedance ratio is above a critical threshold. Incorporating multiple intermediate materials can further increase the strength of the transmitted shock, with an exponential discretization of intermediate material impedances being the most effective distribution for strengthening strong shocks. The results suggest that up to 25% and 9% increases in pressure behind the leading shock can be achieved for materials of increasing and decreasing impedance, respectively. The technique is applied to the design of laser-driven dynamic compression experiments, and the results of the analysis are verified via comparison to simulations performed with the HYADES hydrodynamics code.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

X-ray imaging methods for high-energy density physics applications

Large scale high-energy density science facilities continue to grow in scale and complexity worldwide. The increase in driver capabilities, including pulsed-power and lasers, continue to push the boundaries of temperature, pressure, and densities, opening up new physics regimes. X-ray imaging is one of the many diagnostic techniques that are used to probe states of matter in these extreme conditions. Improved fabrication and polishing methods have provided improved x-ray microscope performance, while improving detector and x-ray sources now enable pico-second imaging with few micron resolutions. Here this Review will cover x-ray imaging methods, primarily absorption imaging, and their improvements over the last few decades.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Predicting the Cetane Number, Sooting Tendency, and Energy Density of Terpene Fuel Additives

Abstract Discovering renewable fuels and fuel additives is paramount in reducing carbon emissions from internal combustion engines. Terpenes, a group of compounds that can be synthesized from plant matter and microorganisms, have gained significant interest in recent years as promising candidates for fuels/additives. Terpenes are a diverse class of compounds that contain rings and methyl branches, resulting in high energy densities and optimal cold weather behavior. Their variation in bond order, carbon chains, and functional groups lead to varying degrees of soot formation and performance in existing engines. The present work leverages predictive models, namely artificial neural networks, to predict the cetane number (CN), sooting tendency (quantified with yield sooting index, YSI), and energy density (quantified with lower heating value, LHV) of terpenes and hydrogenated terpenes whose sooting propensities were previously determined through experimental means. Predicted sooting propensities of these terpenes are compared with experimental values, and predicted cetane numbers and energy densities are used to comment on the compounds’ ability to act as fuels/additives. Expected prediction errors for CN, YSI, and LHV, defined by blind test set median absolute error, are within 5.56 cetane units, 3.63 yield sooting index units, and 0.77 MJ/kg respectively. Additionally, the present work investigates a variety of correlation/dependence metrics for property-property relationships, furthering our understanding of how combustion-relevant properties are related.

09 BIOMASS FUELS↗

DOE OSTI2025

Bayesian model mixing with multireference energy density functional

Reliably predicting nuclear properties across the entire chart of isotopes is important for applications ranging from nuclear astrophysics to superheavy science to nuclear technology. To this day, however, all the theoretical models that can scale at the level of the chart of isotopes remain semiphenomenological. Because they are fitted locally, their predictive power can vary significantly; different versions of the same theory provide different predictions. Bayesian model mixing takes advantage of such imperfect models to build a local mixture of a set of models to make improved predictions. Earlier attempts to use Bayesian model mixing for mass table calculations relied on models treated at single-reference energy density functional level, which fail to capture some of the correlations caused by configuration mixing or the restoration of broken symmetries. In this study we have applied Bayesian model mixing techniques within a multireference energy density functional (MR-EDF) framework. We considered predictions of two-particle separation energies from particle number projection or angular momentum projection with four different energy density functionals—a total of eight different MR-EDF models. We used a hierarchical Bayesian stacking framework with a Dirichlet prior distribution over weights together with an inverse log-ratio transform to enable positive correlations between different models. We found that Bayesian model mixing provides significantly improved predictions compared to the participating models. Published by the American Physical Society 2025

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Magnetic-Field Effects in Unstable High-Energy-Density Plasmas

The influence of magnetic fields in high-energy-density (HED) systems is a widely unexplored field of research that can play an important role in magnetized inertial confinement fusion (ICF) and in astrophysical systems. Hydrodynamic instabilities are presently believed to be the dominant degradation mechanism in ICF implosions. Therefore, understanding the influence of an imposed B-field on RT growth is important for future mitigation strategies as well as fundamental physics of ICF implosions that utilize B-fields for enhanced performance. The Crab Nebula, one of the most observed objects in our universe, contains elongated spikes of material created by hydrodynamic instabilities, however these spikes do not break-up and become turbulent as they evolve late in time. One hypothesis for this behavior is that B-fields around these spikes prevent vortex generation typical in these types of systems.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Dynamic Structure of Magnetized High Energy Density Plasmas (Final Report)

This report summarizes results of project DE-SC0022202 ``Dynamic Structure of Magnetized High Energy Density Plasmas,'' which was originally funded for the period 08/01/2021 - 7/31/2022, but was no-cost extended to 7/31/2023. The primary objectives of the work, as stated in the original proposal, were ``develop a theory to describe a novel state of magnetized high energy density plasmas, benchmark the theory using first-principles molecular dynamics simulations, and apply the results to develop a means to interpret x-ray scattering measurements in future experiments.'' These were the goals of the original project proposal, which was for a 3 year project. The project was ultimately funded for 1 year, and so the work completed focused on the goals described for only the first year of the proposed work. This included further developing a kinetic theory for strongly magnetized plasmas, applying it to compute fluid-scale (MHD) transport coefficients, and to test the predictions using molecular dynamics simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗