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DOE OSTI2020

Development of an Optimized Gasoline Surrogate Formulation for PACE Experiments and Simulations

New powertrain solutions are needed to address societal challenges stemming in part from a transportation sector which relies heavily on combustion of conventional hydrocarbon fuels like gasoline. One way to advance new solutions is through predictive simulations. Predictive simulations can potentially limit the extent of experimental validations, reduce time spent in engineering design cycles, unlock new strategies for high efficiency combustion with power density, and minimize tailpipe emissions. However, the simulation tools currently available are either too computationally expensive, inadequate in their accuracy, or a combination of the two. A DOE-funded consortium of national laboratories called the Partnership to Advance Combustion Engines (PACE) seeks to address this gap by rapidly delivering new knowledge and tools which enable market-competitive powertrain solutions for light-duty vehicles. Approaches to modeling combustion in powertrain systems typically incorporate computational fluid dynamics (CFD) simulations with chemical kinetic models. These CFD simulations generally use surrogate fuels featuring a limited number of existing components in a reduced kinetic model to limit computational costs. Such surrogate fuels often sacrifice matching several or more combustion and physical properties of the target gasoline fuel. Validation of surrogate fuels is also often only pursued for a small subset of standard metrics such as research or motor octane number (RON, MON). The purpose of this project is to develop an optimal E10 gasoline surrogate fuel suitable for tasks across PACE to facilitate rapid common analysis and progression toward consortium goals. This project received contributions from tasks led by eight PACE principal investigators. The project funding here reflects all tasks under Pitz, whose tasks also contributed to additional PACE projects. Based on the optimal gasoline surrogate fuel composition, a reduced chemical kinetic model will be shared with PACE researchers, industry, and the broader combustion community.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2024

The effect of remnant CdSe layers on the performance of CdSeTe/CdTe photovoltaic devices

Thin film CdTe-based photovoltaic devices have achieved high efficiency above 22 %. The recent improvement in efficiency is due to Se alloying in the CdTe absorbers to form a CdSeTe/CdTe structure. The subsequent band gap grading increases the short circuit current density. The Se can be introduced by depositing a precursor thin film of either CdSe or a CdSeTe alloy and then diffusing the Se into the CdTe during the high temperature cadmium chloride activation process. Using CdSe is preferred because it is easier to control the Se concentration. However, during fabrication of the CdSeTe/CdTe devices, the CdSe thickness needs to be precisely controlled to prevent the retention of a CdSe remnant layer after the activation treatment. Retention of a remnant CdSe layer causes a dramatic reduction in device efficiency. In this work, we show that the reduction in efficiency is caused by a number of factors. The remnant CdSe layer is n-type which moves the position of the p-n junction. Also, it is widely thought that the CdSe remnants are photo-inactive. In this work, we clarify that the individual CdSe grains are actually highly photo-active. However, the grain sizes in the CdSe remnant and the adjacent CdSeTe layer are very small resulting in a high grain boundary area. Although the grain boundaries are passivated with chlorine, cathodoluminescence imaging and electrical measurements show that this is only partially effective. Also, EQE measurements show that the remnant CdSe causes parasitic absorption. Overall, the remnant CdSe layer causes a reduction in short circuit current density and device efficiency. The thickness of the CdSe precursor layer and the cadmium chloride activation process conditions must be precisely optimised to ensure that all the CdSe is consumed and inter-diffused to form the CdSeTe alloy for highest efficiency devices.

CdSe remnant↗

DOE OSTI2024

Fast ion studies in the extended high-performance high β P plasma on EAST

Comprehending and optimizing fast ion behaviors is critical for the enhancement of performance in Experimental Advanced Superconducting Tokamak (EAST). This study explores the potential benefits of several factors that can improve the fast ion confinement. First, experiments show the change in the direction of the NBI2 from counter-I p to co-I p leads to a significant reduction in fast ion losses. TRANSP/NUBEAM simulation and tomography results based on fast-ion D-alpha measurements reveal that after the neutral beam injection (NBI) upgrade, the beam ion prompt loss is reduced by approximately 50%. Second, the upgraded ion cyclotron resonant frequency (ICRF) antenna at the N-port features twice the coupling resistance of the original antennas at EAST. This improved ICRF power coupling has enhanced the synergistic heating effect of NBI + ICRF, where the ICRF wave field accelerates beam ions at the harmonics. Experiments demonstrate that NBI + ICRF synergistic not only enhances plasma neutron yield and β P , but also accelerates beam ions to hundreds of keV. Further, the electron density and the neutral beam voltage have been optimized to reduce the fast ion slowing-down time and beam ion losses. Experimental and simulation results indicate that increasing the electron density reduces beam ion losses and enhances the bootstrap current fraction. While higher beam voltage results in a slight decrease in beam power absorption, it can increase the fraction of bootstrap current. With the understanding of these optimization of fast ion confinement, experiments have demonstrated fully non-inductive operation at high density (n e /n G ∼ 0.67, β P ∼ 3.1, β N ∼ 2.1, H 98,y2 ∼ 1.2) even without the support of co-I p beam NBI2. This investigation presents a potential regime to enhance fast ion confinement and extend performance in the high β P plasma for future experiments.

EAST tokamak↗

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

Regulating crystallization to maintain balanced carrier mobility via ternary strategy in blade-coated flexible organic solar cells

Regulating the crystallization of donor and acceptor to maintain balanced carrier mobility is of great importance to fabricate efficient organic solar cells (OSCs). Herein, the balanced crystallinity between donor and acceptor was finely controlled in blade-coated OSCs. By adding high crystalline FOIC into PBDB-T:ITIC system, a balanced carrier mobility was achieved, resulting in the much improved fill factor. The optimized ternary device exhibits an increased current density, due to the enhanced light-harvesting efficiency with complementary absorption and the morphology change. Morphology characterization demonstrated that the ternary film exhibits a highly balanced crystallinity between the donor and acceptor on account of the formation of acceptor alloy. Moreover, the ternary film not only possesses a small domain size, but also exhibits a high domain purity as compared to both binary films. Encouragingly, a highest power conversion efficiency (PCE) of 10.68% was obtained for the blade-coated ternary OSCs. In addition, the blade-coated flexible large-area (105 mm 2 ) OSC based on PBDB-T:ITIC:FOIC ternary system also exhibits a high PCE of 9.81%, showing great potential in the high-throughput fabrication of OSCs.

14 SOLAR ENERGY↗

DOE OSTI2020

Dual-atom Ag 2 /graphene catalyst for efficient electroreduction of CO 2 to CO

Electrochemical reduction of CO 2 into value-added carbon compounds offers a promising strategy to mitigate global warming, but present challenges for chemistry due to the poor selectivity and stability of electrocatalysts. In this work, we report a dual-atom Ag 2 /graphene catalyst featuring well-defined AgN 3 -AgN 3 active site for CO 2 electrochemical reduction. This dual-atom catalyst can drive CO 2 reduction reaction at a potential as high as -0.25 V, and exhibit excellent CO Faradic efficiency up to 93.4 % with a current density of 11.87 mA cm -2 at -0.7 V and long-term stability, far surpassing the single-atom Ag 1 /graphene and the traditional silver nanoparticle catalysts. Finally, DFT calculations reveal that the dual-atom Ag site lowers the barrier for the formation of *COOH by stabilizing the *CO 2 through the concomitant interactions with the C and an O atom of CO 2 , resulting in excellent catalytic performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Large Spin-Orbit-Torque Efficiency and Room-Temperature Magnetization Switching in Sr Ir O 3 / Co-Fe-B Heterostructures

Spin-orbit-torque (SOT) switching is a potentially energy-efficient mechanism by which electrical current can control magnetization. We demonstrate room-temperature SOT switching in nanometer-thick Co⁢Fe⁢B/Sr⁢Ir⁢O 3 bilayers despite the amorphous nature of CoFeB and the interface. This behavior is attributed to the large spin Hall angle in Sr⁢Ir⁢O 3 as well as high spin transmission at the interface that contribute to the SOT efficiency ξ SOT . Our bilayers exhibit large ξ SOT of up to 1.4 and effective spin Hall conductivity of 0.9 ×10 5 (ℏ/2e)Ω –1 ⁢m –1 . In our bilayers, we observe unidirectional magnetoresistance and current-induced magnetization switching with a low critical current density of 1.38 ×10 10 A/m 2 at room temperature. Finally, our results are promising for heterostructures combining technologically relevant CoFeB with high spin-orbit-coupling oxides.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Modeling the electrochemical behavior and interfacial junction profiles of bipolar membranes at solar flux relevant operating current densities

A 1-dimensional, multi-physics model that accounts for the migration and diffusion of solution species, electrostatics, and chemical reactions, in particular water dissociation (WD), at bipolar membrane (BPM) interfaces was developed to study the electrochemical behavior of bipolar membranes (BPMs) at solar flux relevant operating current densities (tens of mA cm -2 ). Significant partial current densities for WD were observed at BPM voltages much less than the equilibrium voltage, e.g., 59 mV × ΔpH from both experiments and modeling. The co-ion leakage across the BPM at pH differentials accounted for the early presence of the partial current density for WD. Two distinctive electric field dependent WD pathways, the un-catalyzed pathway and the catalyzed pathway, were quantitatively and parametrically studied to improve the turn-on potential of the BPM. The catalyzed pathway accounted for the majority of the partial current density for WD at low voltages, while the un-catalyzed pathway dominated the WD at relatively high voltages. Significant WD was observed only within the interfacial CL (<5 nm), in which a large electric field was present. To improve the electrochemical behavior and the turn-on potential of BPMs, the impacts of the pKa of the immobilized WD catalysts, the electric-field dependent rate constant, the thickness of the catalyst layer and fixed charge density in BPMs on the partial current densities for WD were studied systematically. In addition, the electrochemical behavior and concentration profiles of BPMs in a buffered electrolyte were studied and contrasted with those in an un-buffered electrolyte from both modeling and experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Electron Redistributed S-Doped Nickel Iron Phosphides Derived from One-Step Phosphatization of MOFs for Significantly Boosting Electrochemical Water Splitting

Nonprecious transition metal-organic frameworks (MOFs) are one of the most promising precursors for developing electrocatalysts with high porosity and structural rigidity. This study reports the synthesis of high efficiency electrocatalysts based on S-doped NiFeP. MOF-derived S-doped NiFeP structure is synthesized by a one-step phosphorization process with using S-doped MOFs as the precursor, which is more convenient and environment friendly, and also helps retain the samples’ framework. The oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance of the NiFeP catalysts can be improved after partially replacing P by S due to the tunable electronic structure. The optimized CCS-NiFeP-10 reaches a current density of 10 mA cm –2 for OER with an overpotential of 201 mV and outperforms most NiFe-based catalysts. The S doping plays an important role in tuning the ΔG values for intermediates formation in Ni atoms to a suitable value and exhibits a pronouncedly improved the OER performance. CCS-NiFeP-20 sample presents excellent HER performance due to the d-band center downshifting from the Fermi level. When the voltage of the electrolytic cell is 1.50 V, a current density of 10 mA cm –2 can be obtained. This strategy paves the way for designing highly active none-noble metal catalysts.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Targeted synthesis and reaction mechanism discussion of Mo 2 C based insertion-type electrodes for advanced pseudocapacitors

Mo 2 C is one of the few compounds that possess good electronic conductivity. Meanwhile, it possesses a natural 1D zigzag tunnel structure that is ideally suited for fast ion diffusion. Here, an effective approach is demonstrated for fabrication of structurally stable N-doped Mo 2 C/C nanobelts. They demonstrate high and fast energy storage ability with initial capacitances of 1139 C g -1 at 1 mV s-1, 151 C g -1 at an extremely high scan rate of 2000 mV s -1 and 208 C g -1 at a discharge current density of 200 A g -1 . After electrochemical activation of cycling, the capacity is continuously enhanced and much higher capacitances of 2523 C g -1 at 1 mV s -1 and 1403 C g -1 at 50 A g -1 are achieved after 15,000 cycles at 50 mV s -1 . Using the power law, it is evaluated that a surface-controlled capacitive process makes the main contribution to the capacity, which is over 90% when the scan rates are higher than 10 mV s -1 and still high as 73% at 1 mV s -1 . From in situ synchrotron XRD, it is found that there is a negligible change in the crystal structure and volume during charging/discharging, reflecting an insertion-type charge storage mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Investigating the Impact of Thickness, Calendering and Channel Structures of Printed Electrodes on the Energy Density of LIBs - 3D Simulation and Validation

Current lithium ion batteries (LIBs) are expensive and bulky, limited by relatively low charging rates. To increase the rate of charging and reduce weight, thin electrodes with high energy density are required. The increase in energy density can be achieved by several techniques including boosting electrolyte transport, high loading/utilization of active material, employing high conductive electrolytes and electrodes with advanced architectures, and increasing cell temperature. In this paper, a 3D physics-based electrochemical model of LIBs is developed in COMSOL simulation software for different thickness, calendering steps as well as channel structures (conical, cylindrical) to optimize the electrode design and in turn maximize volumetric energy density. The simulation results demonstrated that calendering the electrodes with high initial porosity increases the volumetric energy density of the cell. In addition, cylindrical channel structures with relatively lower edge-to-edge distance also results in increased volumetric energy density. The simulation results of the 3D model was validated by comparing it with experimental results.

improving volumetric energy density↗

DOE OSTI2022

Cold-Starting All-Solid-State Batteries from Room Temperature by Thermally Modulated Current Collector in Sub-Minute

All-solid-state batteries (ASSBs) show great potential as high-energy and high-power energy storage devices but their attainable energy/power density at room temperature is severely reduced because of the sluggish kinetics of lithium-ion transport. Here we first reported a thermally modulated current collector (TMCC), which can rapidly cold-start ASSBs from room temperature to operating temperatures (70–90 °C) in less than one minute, and simultaneously enhance the transient peak power density by 15-fold compared to one without heating. This TMCC is prepared by integrating a uniform, ultrathin (~200 nm) nickel layer as a thermal modulator within an ultralight polymer-based current collector. By isolating the thermal modulator from the ion/electron pathway of ASSBs, it can provide fast, stable heat control yet does not interfere with regular battery operation. Moreover, this ultrathin (13.2 μm) TMCC effectively shortens the heat transfer pathway, minimizes heat losses, and mitigates the formation of local hot spots. The simulated heating energy consumption can be as low as ~3.94% of total battery energy. This TMCC design with good tunability opens new frontiers towards smart energy storage devices in the future from the current collector perspective.

25 ENERGY STORAGE↗

DOE OSTI2021

An Active and Robust Air Electrode for Reversible Protonic Ceramic Electrochemical Cells

Reversible protonic ceramic electrochemical cells (RPCECs) are a promising option for efficient and low-cost generation of electricity and hydrogen. Commercialization of R-PCECs, however, hinges on the development of highly active and robust air electrodes. Here, we report an air electrode consisting of PrBa 0.8 Ca 0.2 Co 2 O 5+δ and in situ exsolved BaCoO 3–δ nanoparticles (PBCC–BCO) that shows minimal polarization resistance (~0.24 Ω cm 2 at 600 °C) and high stability when exposed to humidified air with 3–50% H 2 O. An R-PCEC utilizing PBCC-BCO demonstrates remarkable performances at 600 °C: achieving a peak power density of 1.06 W cm –2 in the fuel cell mode and a current density of 1.51 A cm –2 at 1.3 V in an electrolysis mode. More importantly, the RPCECs demonstrate an exceptionally high durability over 1833 h of continuous operation in the electrolysis mode. Furthermore, this work offers an efficient approach to design of high-performance and durable electrodes for R-PCECs.

25 ENERGY STORAGE↗

DOE OSTI2020

Probing Mg Intercalation in the Tetragonal Tungsten Bronze Framework V 4 Nb 18 O 55

While commercial Li-ion batteries offer the highest energy densities of current rechargeable battery technologies, their energy storage limit has almost been achieved. Therefore, there is considerable interest in Mg batteries, which could offer increased energy densities in comparison to Li-ion batteries if a high-voltage electrode material, such as a transition-metal oxide, can be developed. However, there are currently very few oxide materials which have demonstrated reversible and efficient Mg 2+ insertion and extraction at high voltages; this is thought to be due to poor Mg 2+ diffusion kinetics within the oxide structural framework. Here, in this paper, the authors provide conclusive evidence of electrochemical insertion of Mg 2+ into the tetragonal tungsten bronze V 4 Nb 18 O 55 , with a maximum reversible electrochemical capacity of 75 mA h g –1 , which corresponds to a magnesiated composition of Mg 4 V 4 Nb 18 O 55 . Experimental electrochemical magnesiation/demagnesiation revealed a large voltage hysteresis with charge/discharge (1.12 V vs Mg/Mg 2+ ); when magnesiation is limited to a composition of Mg 2 V 4 Nb 18 O 55 , this hysteresis can be reduced to only 0.5 V. Hybrid-exchange density functional theory (DFT) calculations suggest that a limited number of Mg sites are accessible via low-energy diffusion pathways, but that larger kinetic barriers need to be overcome to access the entire structure. The reversible Mg 2+ intercalation involved concurrent V and Nb redox activity and changes in crystal structure, as confirmed by an array of complementary methods, including powder X-ray diffraction, X-ray absorption spectroscopy, and energy-dispersive X-ray spectroscopy. Consequently, it can be concluded that the tetragonal tungsten bronzes show promise as intercalation electrode materials for Mg batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Thermochemical reduction modeling in a high-temperature moving-bed reactor for energy storage: 1D model

The design of robust and efficient high-temperature thermochemical reactors and determination of operating conditions are critical steps toward enabling high-efficiency long-duration solar energy storage. This work presents a computational model for the thermal reduction of a metal oxide material (Mg-Mn-O) up to 1450 °C and the coupled complex transport phenomena in a novel tubular thermal reactor design that features the capability for a high extent-of-reduction (high energy storage density) and inherent heat recuperation. A one-dimensional model coupling counter-current gas–solid flow, two-phase heat transfer, thermochemical redox reactions, and species transport in a moving-bed reactor is developed. Simplified versions of the model are validated with published results in the literature for packed beds with both inert and reactive particles; the fully coupled model is also validated with experimental measurements of a moving-bed reactor in terms of local temperatures and oxygen release at the exit. Detailed comparisons on the effects of different boundary conditions in the reaction zone (prescribed wall temperature vs. heat flux conditions) and formulations based on a simple uniform flow assumption vs. plug flow using Ergun equation for gas flow are investigated. The results are compared with experimental measurements, and for all cases, the energy flow components in the reactor system and the thermal to chemical conversion efficiency and overall system efficiency are computed. Finally, the predicted high thermal-to-chemical efficiency ~95% and system efficiency ~30% agree with experimental measurements.

25 ENERGY STORAGE↗

DOE OSTI2020

Fast Organic Vapor Phase Deposition of Thin Films in Light-Emitting Diodes

Fast deposition of thin films is essential for achieving low-cost, high throughput phosphorescent organic light emitting diode (PHOLED) production. In this work, we demonstrate rapid and uniform growth of semiconductor thin films by organic vapor phase deposition (OVPD). A green PHOLED comprising an emission layer (EML) grown at 50 Å/s with bis[2-(2-pyridinyl-N)phenyl-C](acetylacetonato)iridium(III) (Ir(ppy)2(acac)) doped into 4,4 bis(N-carbazolyl)-1,1zolylld (CBP) exhibits a maximum external quantum efficiency of 20 ± 1%. The morphology, charge transport properties, and radiative efficiency under optical and electrical excitation of the PHOLED EML are investigated as functions of the deposition rate via both experimental and theoretical approaches. The EML shows no evidence for gas phase nucleation of the organic molecules at deposition rates as high as 50 Å/s. However, the roll-off in quantum efficiency at high current progressively increases with deposition rate due to enhanced triplet-polaron annihilation. The roll-off results from accumulation of stress within the PHOLED EML that generates a high density of defect states. Here, the defects, in turn, act as recombination sites for triplets and hole polarons, leading to enhanced triplet-polaron annihilation at high current. We introduce a void nucleation model to describe the film morphology evolution that is observed using electron microscopy.

42 ENGINEERING↗

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↗

DOE OSTI2025

VoroClust

SAND2025-11465O VoroClust, also known as Voronoi Clustering, is a fast, density-based unsupervised clustering algorithm applicable to high-resolution and high-dimensional data. It operates as quickly as distance-based clustering methods while effectively capturing complex regional geometries, matching the performance of current density-based methods. VoroClust employs a data-centered sphere cover to reduce computational demands while preserving data topology. It propagates clusters outward from local density peaks. Although supervised machine learning is powerful for applications like image classification and segmentation, it requires comprehensive, consistent datasets, which many applications lack. Unsupervised clustering algorithms analyze the structure of each dataset rather than relying on similarities with other examples, making them well-suited for practical applications with insufficient or inappropriate data for supervised learning. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Ebeida, Mohamed [Sandia National Lab. (SNL-CA), Li↗