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DOE OSTI2024

InP- and GaAs-Based 0.6 eV GaInAs Devices for Thermophotovoltaics and Laser Power Conversion

Emerging applications such as thermal energy grid storage, waste heat recovery and portable power generation require efficient thermophotovoltaic (TPV) converters tuned to temperatures near 1000 Degrees Celsius or below. Metamorphic GaInAs with larger lattice constants than InP present a promising option for these needs. The ability to grow these devices on GaAs substrates instead of more expensive InP would enhance the scalability of these devices. In this talk, we present inverted metamorphic Ga0.3In0.7As photovoltaic converters with sub-0.60 eV bandgaps grown on InP and GaAs substrates. These devices are realized using InAsP or GaInP/InAsP compositionally graded buffers which exhibit threading dislocation densities of 1.3 +/- 0.6 x 106 cm-2 and 8.9 +/- 1.7 x 106 cm-2 on InP and GaAs, respectively. Despite this difference in defect density, the devices generate similar open-circuit voltages of 0.386 V and 0.383 V, respectively, under irradiance producing a short-circuit current density of -10 A/cm2, with bandgap-voltage offsets of 0.20 and 0.21 V. We estimate their thermophotovoltaic efficiency using these measurements coupled with broadband reflectance measurments. The InP-based cell is estimated to yield 1.09 W/cm2 at 1100 Degrees Celsius vs. 0.92 W/cm2 for the GaAs-based cell, with TPV efficiencies of 16.8 vs. 9.2%. Both devices are limited by sub-bandgap absorption, which we assess largely occurs in the graded buffers. We estimate that the 1100 Degrees Celsius thermophotovoltaic efficiencies would increase to 24.0% and 20.7% in structures with the graded buffer removed, if previously demonstrated reflectance is achieved. These devices also have application as laser power converters in the 2.0-2.3 um atmospheric window. We estimate efficiencies of 36.8% and 32.5% under 2.0 um monochromatic irradiance of 1.86 W/cm2 and 2.81 W/cm2, respectively.

ENGINEERING,MATERIALS SCIENCE,SOLAR ENERGY↗
DOE OSTI2023

FY22 Grid Modernization & Energy Storage Program: Accomplishments & Impacts

Sandia’s Grid Modernization and Energy Storage program works to advance a national vision of a secure, resilient, and sustainable electric system for all users. Our achievements reflect a strategic approach combining technology development; modeling, simulation, and data analytics; and partnered demonstrations and outreach to further the adoption of advanced grid and storage technologies. Our FY22 efforts leverage the strengths of our partnerships—spanning Sandia’s core science and technology competencies as well as external technology leaders—to develop the solutions today which enable the grid of tomorrow. Much of the material in this report comes from the separate 2022 Accomplishments Report compiled by our Energy Storage subprogram team, a cornerstone of our grid research and achievements. The Grid Energy Storage Program at Sandia is focused on making energy storage cost-effective through research and development (R&D) in new battery technologies, advanced power electronics and power conversion systems, improved safety and reliability for energy storage systems, analytical tools for the valuation of energy storage, and the validation of new energy storage technologies through demonstration projects. During the 2022 fiscal year, Sandia executed R&D work supported by the U.S. Department of Energy’s (DOE) Office of Electricity – Energy Storage Program under the leadership of Dr. Imre Gyuk. This report indicates key areas of research and engagement and summarizes the impact of Sandia’s contributions through notable accomplishments, journal publications, patents, and technical conferences and presentations. It is provided with the hope that readers discover ways we can further team to create our modern grid and apply the outcomes of our efforts. The bulk of work described herein is funded by the DOE Office of Electricity and key programs within the DOE Office of Energy Efficiency and Renewable Energy. As we indicated in our report from last year, the contributors to our successes are too numerous to name here, though our team wishes to express our deep gratitude to the numerous program and project sponsors at the US Department of Energy, who often function equally as technical collaborators; our many partners in industry, academia, utilities, and other national labs; and fellow researchers and business partners at Sandia whose leadership and creativity have enabled the accomplishments described herein.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2023

Molten salt electrochemical upcycling of CO 2 to graphite for high performance battery anodes

The efficient transformation of CO 2 into a value-added material is a potential strategy to help mitigate climate effects caused by CO 2 emissions. One potential CO 2 conversion product is graphite which is an important and versatile material extensively used in many applications including as an anode for lithium-ion batteries (LIBs). Commercial graphite, however, is traditionally synthesized via the energy intensive Acheson process (>3000 °C) and the performance of such graphite can be limited under fast charging conditions which is important for vehicle electrification. We report the electrochemical transformation of CO 2 to highly crystalline nano-graphite with a controlled microstructure in a carbonate molten salt at 780 °C. The use of a nickel foam electrode and controlled electrochemical parameters during the molten salt conversion process yielded pure graphite at a lower temperature compared to the Acheson process. Moreover, when investigated as an anode material for LIBs, the CO 2 -converted graphite exhibited high reversible capacity, long cycle life, and excellent rate capability even under fast charging conditions. This process provides a way to potentially reduce carbon emissions through the utilization of waste CO 2 by converting it into value-added graphite suitable for fast charging, high-energy-density batteries for vehicle electrification.

25 ENERGY STORAGE↗
DOE OSTI2025

Bayesian optimization of entropy-stabilized metal fluoride conversion cathodes and their synthesis

Fluoride-based conversion cathodes are promising for next-generation Li ion batteries because of their high voltage and energy densities. High entropy earth abundant fluoride cathodes are attractive for sustainable battery because of the potentially higher cycling stability. While Ni and Co containing equimolar alloys stabilized by high entropy were considered previously, Ni and Co free non-equimolar metal alloy compositions might offer new opportunities to increase materials stability and average voltage. This opportunity was pursued using Bayesian optimization of average voltage for the computational prediction of (Fe x1 Cu x2 Zn x3 Mn x4 Mg x5 )F 2 cathode chemistries. Theoretical voltage, room temperature free energy, and electronic structure of potentially high voltage compositions were computed using density functional theory calculations. Here, the experimental realization of non-equimolar quinary Co and Ni free fluorides with stable rutile single phase and improved conversion reaction voltage by up to 28 % compared to the equimolar alloy demonstrated the power of Bayesian optimization methods for the computationally guided experimental synthesis of fluoride cathodes. Finally, non-equimolar cathode chemistries were found with cycling stability superior to known multi-element fluorides.

25 ENERGY STORAGE↗
DOE OSTI2022

Multilevel Analysis, Design, and Modeling of Coupling Advanced Nuclear Reactors and Thermal Energy Storage in an Integrated Energy System

This report discusses the different options for coupling thermal energy storage (TES) systems to advanced nuclear power plants (A-NPPs) in order to enable flexible and hybrid plant operation. An advanced light-water reactor (A LWR), a high-temperature gas-cooled reactor (HTGR) and a liquid-metal fast reactor (LMFR) were selected as the initial use cases for demonstrating a thermally balanced energy storage coupling design for thermal power extraction. The models presented herein showcase several design considerations, focusing on optimal deployment methodologies for achieving steady-state and transient-state operation with minimum disruption to the nuclear power cycle. This first part of the study presents steady-state models developed using Aspen HYSYS®, with the thermal energy bypass for NPP-TES coupling being varied at up to 50%. The various components were sized using the Aspen Process Economic Analyzer (APEA) and Aspen Exchanger Design and Rating (EDR), when applicable. Cost functions from these models were developed using the latest publicly available data obtained from APEA V11. The TES-coupled A-NPP steady-state models and cost functions then provided a baseline for dynamic operation and process optimization by using Idaho National Laboratory (INL)’s Framework for Optimization of Resources and Economics (FORCE) tools. A stochastic optimization of the various energy storage systems coupled to the A-NPPs was then performed using the Risk Analysis Virtual Environment (RAVEN) and its dispatch optimization plugin, the Holistic Energy Resource Optimization Network (HERON). The signal processing and synthetic history capabilities of RAVEN were used to account for the unpredictable behavior of electricity markets. An autoregressive moving average (ARMA) model was used to analyze price signals from the Pennsylvania-New Jersey-Maryland (PJM) market and were applied to the HERON analysis in order to optimize a system with the best economics. Transient modeling evaluation was then performed using Modelica models within the HYBRID repository, which was developed at INL for the Department of Energy Integrated Energy Systems program for the characterization of dynamic integrated system behavior and feedback. This includes evaluation of the TES-coupled A-LWR systems’ impact on physical and thermal system response during imposed system demands. Additional TES-coupled reactor types, coupling approaches, markets, and TES technologies will be evaluated in future work.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2026

Mechanistic insights into CO 2 capture and electrochemical conversion in nonaqueous Na–CO 2 batteries

Developing efficient energy storage systems that capture and convert CO 2 is critical for mitigating carbon emissions. Here, we report a Na–CO 2 battery with ruthenium dioxide (RuO 2 ) cathode catalysts and propane-1,3-diamine (PDA) as an electrolyte additive to enhance CO 2 capture and conversion efficiency. The integration of CO 2 adsorption and electrochemical reduction facilitates activation of the inert CO 2 molecule and circumvents gas–solid–liquid ternary-phase reactions at the interface. We employed density functional theory (DFT) calculations to systematically unravel the reaction mechanisms and energetics governing CO 2 reduction, both with and without PDA. Our results reveal an energetically favorable pathway toward the formation of Na 2 CO 3 and C as final discharge products, rather than sodium oxalate (Na 2 C 2 O 4 ). The CO 2 –amine adduct facilitates charge transfer from PDA to CO 2 , which results in activation of CO 2 . The kinetics of CO 2 conversion and regeneration of PDA were found to be significantly enhanced on the RuO 2 surface compared to the bulk electrolyte. More importantly, pre-activation of CO 2 via the amine–CO 2 adduct lowers the total overpotential to 2.44 V, compared to 3.13 V without PDA. This study provides fundamental insights into CO 2 electroreduction in Na–CO 2 batteries and underscores the promise of electrolyte engineering for sustainable CO 2 utilization and high-performance energy storage.

25 ENERGY STORAGE↗
DOE OSTI2021

The influence of LiH and TiH 2 on hydrogen storage in MgB 2 II. XPS study of surface and near-surface phenomena

We report that Mg(BH 4 ) 2 is a promising solid-state hydrogen storage material, releasing 14.9 wt% hydrogen upon conversion to MgB 2 . The rehydrogenation of MgB 2 is particularly challenging, requiring prolonged exposure to high pressures of hydrogen at high temperature. Here we report an XPS study probing the influence of LiH and TiH 2 on the hydrogen storage properties of MgB 2 in the surface and near-surface regions, as a complementary investigation to a preceding study of the bulk properties. Surface and near-surface properties are important considerations for nanoscale and bulk hydrogen storage materials. If there are reactions occurring at the surface that modify the chemical composition in the near-surface region, species diffusion can alter the chemical composition even deep into the bulk of the material. For LiH/MgB 2 , metastable LiH–B and LiH–Mg species are produced that are more reactive than Bulk MgB 2 . With prolonged glovebox storage, the LiH/MgB 2 material shows increased reactivity towards O and C and enriched levels of Li and B in the near-surface region. In addition, Li induces the growth of Li 2 CO 3 in the surface and near surface regions. Exposing LiH/MgB 2 to hydrogen at 700 bar and 280 °C for 24 h produces borohydride at a temperature 100 °C below the threshold for bulk MgB 2 hydrogenation. In a specifically surface process with macroscopic implications, the hydrogenation conditions also cause Li 2 CO 3 to react with boron hydroxide in the sample to form a Li-deficient glassy lithium borate melt at the interfaces of the particles, bonding them together. Subsequent heating to 380 °C dehydrogenates the borohydride and eliminates the Li-deficient glassy lithium borate. The LiH/MgB 2 material is not reversible because desorption does not lead back to LiH/MgB 2 , but rather to elemental B and Mg metal in the near-surface region. In contrast to LiH, TiH 2 does not react with MgB 2 , despite the favorable thermodynamics for destabilization via TiB 2 formation. Furthermore, high pressure hydrogenation yields only unreacted TiH 2 and MgB 2 in the surface and near-surface regions. Thus, added TiH 2 provides no benefit to MgB 2 hydrogenation, in agreement with the findings of the preceding bulk study.

08 HYDROGEN↗
DOE OSTI2020

Preservation of Microalgae, Lignocellulosic Biomass Blends by Ensiling to Enable Consistent Year-Round Feedstock Supply for Thermochemical Conversion to Biofuels

Seasonal variation in microalgae productivity is a significant barrier to economical production of algae biofuels and chemicals. Summer production can be 3–5 times higher than in the winter resulting in uneven feedstock supplies at algae biorefineries. A portion of the summer production must be preserved for conversion in the winter in order to maintain a biorefinery running at capacity. Ensiling, a preservation process that utilizes lactic acid fermentation to limit microbial degradation, has been demonstrated to successfully stabilize algae biomass (20% solids) and algae-lignocellulosic blends (40% algae-60% lignocellulosic biomass, dry basis) for over 6 months, resulting in fuel production cost savings with fewer emissions. Preservation of algae as blends could be beneficial to biorefineries that utilize thermochemical approaches to fuel production as co-processing of algae and lignocellulosic biomass has been observed to enhance biocrude yield and improve oil quality. This study conducts a resource assessment of biomass residues in the southern United States to identify materials available during peak algae productivity and in sufficient quantity to meet the algae storage needs of an algae biofuel industry. Eight feedstocks met the quantity threshold but only three, distillers grains, haylage, and yard waste, were also available in season. Storage experiments utilizing both freshwater and marine strains of microalgae – Scenedesmus acutus, Chlorella vulgaris, Chlorella zofingiensis, Nannochloropsis gaditana, and Porphyridium purpureum – and yard waste were conducted for 30 days. Storage losses were less than 10% in all but one case, and the pH of all but one blend was reduced to less than 4.7, indicating that yard waste is a suitable feedstock for blending with algae prior to storage. To better understand whether the benefits to conversion realized by processing blends might be affected by storage, elemental analysis and bomb calorimetry of pre- and post-storage algae-yard waste blends were conducted to characterize changes occurring during storage. Storing algae biomass as blends with lignocellulosic biomass could be an effective method of mitigating seasonal variability in algae biomass production while retaining the synergistic effect of co-processing algae blends in thermochemical conversion.

09 BIOMASS FUELS↗
DOE OSTI2023

Plasma catalytic non-oxidative methane conversion to hydrogen and value-added hydrocarbons on zeolite 13X

Non-thermal plasma has unfolded highly efficient, safe to operate novel routes for methane conversion to hydrogen. In this work, methane conversion is performed under atmospheric dielectric barrier discharge (DBD) plasma with and without 13X zeolite-based catalysts i.e., 13X, Ga/13X, Pd/13X, and Pd-Ga/13X. Experimental results indicate that the plasma catalytic process delivered almost twofold higher product yield than the plasma only route. The binary Pd-Ga catalyst possesses highest catalytic performance with about 40 % CH 4 conversion at an input flowrate of 5 cm 3 min -1 and 2W due to the formation of the Pd-Ga alloy, which acts as catalytic active centre for activating C–H bonds. Product yield can be tailored by the catalyst design where the bimetallic Pd-Ga/13X preferably favours the hydrocarbon formation while H 2 is the dominant product obtained over the Pd/13X. The cleavage of C–H bonds of methane molecule over the plasma only route is mainly governed by energetic electrons in the gaseous phase the catalyst activity, and plasma-catalyst synergism play a significant role in the plasma catalysis process. Further, the findings from this work provide significant insights into the methane activation for subsequent optimization of the methane conversion processes operated on floating production, storage, and offloading vessels (FPSOVs). Exploiting untapped offshore natural gas reserves, where conventional pipeline systems are less economical.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Unveiling Feedstock Variability: Insights into Corn Stover Conversion - Part I: Physicochemical Properties and Self-Degradation

Transforming agricultural waste into biofuels and bioproducts is crucial to advancing a low-carbon bioeconomy. However, the inherent variability in the composition and quality introduces uncertainties in the conversion efficiency and poses challenges in process development. Through integrating a high-throughput conversion system, material characterization techniques, and advanced data analysis tools, this study investigates the variability of corn stover and its subsequent impacts on carbohydrate conversion. The findings reveal that indoor storage substantially reduces the moisture and ash content and soil contamination, while other properties remain largely unchanged. Self-degradation due to microbial activity during storage decreases the carbohydrate content of corn stover but enhances glucose and xylose yields. A negative correlation is observed between sugar yields and lignin content across samples with varying ash and moisture content. The inhibitory effect of lignin diminishes in self-degraded samples likely due to the disrupted cell wall structure. Although self-degradation slightly increases cellulose crystallinity, no strong correlation was observed between the crystallinity and sugar yield. Hot water pretreatment under mild conditions effectively mitigates inherent variability, consistently improving the sugar yield from corn stover by up to 50%. By elucidating the feedstock variability and its impact on convertibility, these findings offer valuable insights into appropriate feedstock handling and management, highlighting potential strategies to address variability challenges.

09 BIOMASS FUELS↗
DOE OSTI2021

A two-dimensional type I superionic conductor

Superionic conductors (SICs) possess liquid-like ionic diffusivity in the solid state, finding wide applicability from electrolytes in energy storage to materials for thermoelectric energy conversion. Type I SICs (e.g., AgI, Ag 2 Se, etc.) are defined by a first-order transition to the superionic state and have so far been found exclusively in three-dimensional crystal structures. Here, we reveal a two-dimensional type I SIC, α-KAg 3 Se 2 by scattering techniques and complementary simulations. Quasi-elastic neutron scattering and ab initio molecular dynamics simulations confirm that the superionic Ag + ions are confined to sub-nanometre sheets, with the simulated local structure validated by experimental X-ray powder pair-distribution-function analysis. Finally, we demonstrate that the phase transition temperature can be controlled by chemical substitution of the alkali metal ions that comprise the immobile charge-balancing layers. Our work thus extends the known classes of SICs and will facilitate the design of new materials with tailored ionic conductivities and phase transitions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Review—Development of Highly Active and Stable Catalyst Supports and Platinum–Free Catalysts for PEM Fuel Cell

Metal-free, metal-containing, and template-assisted metal-containing nitrogen-modified carbon-based catalysts carbon composite supports, and highly active and electrochemically stable hybrid cathode catalysts for oxygen reduction reaction are reviewed in this manuscript. Here, novel procedures are developed for the synthesis of (i) highly catalytically active PGM-free catalyst and stable carbon composite catalyst supports. The carbon composite catalyst supports are engineered with optimized BET surface area and pore size distribution and with a well-defined kinetic and mass transfer region during the reaction and their performance is dicussed in detail in this review. The surface activation results in increasing carbon graphitization and inclusion of non-metallic active sites on the support surface. The USC catalysts exhibit the initial performance of 0.91 V and a maximum power density of 177 mW cm –2 , with well-defined kinetic and mass-transfer regions and ~2.5% H 2 O 2 production. Activated carbon composite support (ACCS) is modified to optimize its kinetic activity and its electrochemical stability shows excellent thermal stability and support stability under simulated start-up/shut-down operating conditions. The stabilities of various supports developed in this study are compared with those of a commercial Pt/C catalyst. The active sites for the ORR identified with electrochemical and physicochemical methods are pyridinic-N and quaternary-N.

25 ENERGY STORAGE↗
DOE OSTI2021

Isolated oleaginous yeast

Some aspects provide engineered microbes for oil production. Methods for microbe engineering and for use of engineered microbes are also provided herein. Such engineered microbes exhibit greatly enhanced conversion yields and TAG synthesis and storage properties.

Stephanopoulos, Gregory↗
DOE OSTI2023

Electric charging particle heater for thermal energy storage

The disclosure relates to particle heaters for heating solid particles to store electrical energy as thermal energy. Thermal energy storage directly converts off-peak electricity into heat for thermal energy storage, which may be converted back to electricity, for example during peak-hour power generation. The particle heater is an integral part of an electro-thermal energy storage system, as it enables the conversion of electrical energy into thermal energy. As described herein, particle heater designs are described that provide efficient heating of solid particles in an efficient and compact configuration to achieve high energy density and low cost.

Ma, Zhiwen↗
DOE OSTI2021

Optimizing the lean hydrocarbon NO x trap: Sequential and dual-layer configurations

Vehicular emission control catalysts are ineffective in eliminating CO, hydrocarbons, and NO x during engine cold-start when exhaust temperatures are below 200 °C. In this study the performance of coupled low temperature NO x , n-C 12 H 26 (C 12 ), and C 3 H 6 trapping, release and conversion for a series of model Lean Hydrocarbon NO x Trap (LHCNT) catalysts are examined. Pd and Pt supported on small-pore (SSZ-13) and large-pore (BEA) zeolites are selected based on the performance during transient NO and C 12 uptake, release and conversion experiments. These catalysts are combined into sequential (Pt + Pd/BEA → Pd/SSZ-13; Pd/SSZ-13 → Pt + Pd/BEA) and dual-layer (Pt + Pd/BEA top, Pd/SSZ-13 bottom) configurations in an attempt to improve the trapping and conversion performance. While all three configurations trap between 75 and 100 μmolNO x /g-cat, the Pd/SSZ-13 → Pt + Pd/BEA sequential configuration is most effective in simultaneously trapping C 12 and NO in the presence of H 2 O, resulting in excellent NO and C 12 storage below 100 °C with release and/or conversion at or above 200 °C. For each configuration, C 12 oxidation lights-off below 300 °C and NO oxidation achieves ~35 % conversion in the absence of C 12 . Neither the presence of C 12 nor the order of the sequential configuration has a significant impact on NO uptake. C 12 significantly delays NO and NO 2 desorption to temperatures exceeding 300 °C. The more compact dual-layer catalyst is most effective in forming NO 2 as the release temperature lines up with the maximum NO conversion temperature but traps less C 12 than the sequential configurations. The addition of C 3 H 6 in the feed on the dual-layer catalyst leads to further delay in the NO x desorption as well as increased NO and C 12 conversion at high temperatures. Here, the overall findings provide guidance in the optimizing LHCNT configuration for realistic feeds.

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

Alternative Energy Carriers: Unique Interfaces for Electrochemical Hydrogenic Transformations

Abstract The shift toward renewable energy generation sources, characterized by their non‐carbon emitting but variable nature, has spurred significant innovation in energy storage technologies. Advancements in foundational understanding from investments in basic science and clever engineering solutions, coupled with increasing industrial adoption, have resulted in a notable reduction in the cost of storing electricity from variable energy generation sources. These developments have paved the way for the exploration of new and innovative forms of energy storage that deviate from traditional technologies. In this perspective, it is posited that the progress made in energy storage research over recent years has opened the door to the development of energy carriers for technologies that are yet to be realized. To illustrate this concept, examples of alternative energy carriers are provided within the context of unique electrochemical interfaces for electrochemical hydrogenic transformations. The unique properties of these interfaces and electrochemical systems can be leveraged in ways not yet imagined, creating new possibilities for energy storage. A perspective on the progress and challenges for each interface as well as a general outlook for the advancement of energy carrier systems are provided.

25 ENERGY STORAGE↗