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DOE OSTI2026

Impact of Porous Transport Layer Morphology on the Performance of Proton Exchange Membrane Water Electrolyzers with Ultra-Low Iridium Loadings

Reducing Ir loadings in proton exchange membrane water electrolyzer anodes is critical for lowering capital expenses. Loading reduction could be achieved by improving the Ir activity via doping/alloying and/or the development of advanced microstructures. However, the anode porous transport layer (PTL) is a comparatively simple component whose properties also impact Ir utilization. Therefore, well-designed PTLs may also enable reduced Ir loadings. In this work, we survey eight PTLs from various manufacturers to observe their impact on cell performance at low (0.4 mg Ir cm -2 ) and ultralow (0.1 mg Ir cm -2 ) Ir loadings. The PTLs were characterized by their microstructural properties, including porosity, particle size distribution, and pore size distribution. Electrochemical cell performance was correlated to PTL morphology, and it was found that PTLs with lower porosities and smaller particle and pore radii enabled good performance even at ultralow Ir loadings. 1000-h durability testing indicated that using lower porosity PTLs can significantly improve durability behavior. A runaway voltage phenomenon was observed during durability testing of cells with ultralow Ir loadings, which was caused by increases in both anode and cathode overpotentials. Furthermore, we observed that the beginning of test performance of 0.1 mg Ir cm -2 cells correlates to the 1000-h degradation rates of 0.4 mg Ir cm -2 cells, suggesting that for the Ir catalyst used in this work, short-term testing at ultralow loadings can be used as an indicator of long-term degradation at higher loadings.

08 HYDROGEN↗

DOE OSTI2022

Highly Efficient Organosulfur and Lithium-Metal Hosts Enabled by C@Fe 3 N Sponge

Lithium-organosulfur (Li-OS) batteries, despite possessing high theoretical specific capacity, encounter a few practical challenges, including unsatisfactory lifespan and low active material utilization under realistic conditions. Here, diisoropyl xanthogen polysulfide (DIXPS) has been selected as a model organosulfur compound to investigate the practical feasibility of Li-OS batteries under realistic conditions. A well-designed freestanding carbon sponge decorated with Fe 3 N nanoparticles (C@Fe 3 N) is introduced into the Li-OS cells as a scaffold for both Li and DIXPS. The lithiophilic property of the C@Fe 3 N host guides uniform lithium deposition at the anode, and the catalysis of the DIXPS conversion reaction promotes the kinetics at the cathode. Impressively, the synergistic effect of C@Fe 3 N leads to an extremely stable cycling performance over 1000 cycles in a Li-OS full cell under realistic conditions.

25 ENERGY STORAGE↗

NASA NTRS1991

Coproduction of volatiles and metals from extraterrestrial materials

Two main efforts in support of the general goals of SERC/culpr are presented. Investigations of processes for the coproduction of metals from extra-terrestrial materials in conjunction with plausible schemes for oxygen extraction continue. The principal emphasis was on the extraction and purification of iron from the ilmenite reduction process for oxygen, from the cathode metal deposits made in the magma electrolysis process for oxygen, and from native ferrous metal alloys on the moon and asteroids. All work on the separation and purification of ferrous metals was focussed upon the gaseous carbonyl process, a scheme that involves only temperatures attainable by passive thermal control. The exploration of a variety of schemes was initiated, involving the use of several different propulsion options and both propulsive and aerobraking capture at earth, for return of extraterrestrial resources to earth orbits. In addition, the search for new opportunities in space resource utilization continues. Examples include the continuation of work underway on: (1) the feasibility of locating solar power satellites in highly eccentric earth orbit; (2) the energetics of extracting the potential clean fusion fuel He-3 from the atmosphere for return to earth; and (3) the utility of a nuclear steam rocket (using non-terrestrial water as the working fluid) for transportation in the inner solar system.

Lewis, John S.↗

NASA NTRSDate not supplied

Ground Test Stand Development for One-step Electrochemical Production of High-Pressure Oxygen

NASA designed a test rig, High-Pressure Oxygen Generation Assembly (HPOGA) to test a novel method of electrolysis as an alternative technology to the state-of-the-art Oxygen Generation Assembly (OGA) currently on the International Space Station (ISS). This approach involves utilizing a specialized electrolysis cell stack designed to both generate and compress high-pressure oxygen up to 3600 PSIG. The design eliminates the need for an external compressor and hydrogen separator, streamlining the oxygen generation process. HPOGA tests the viability of an electrolysis cell stack for extended life usage. Within the system, there are several key subsystems: nitrogen, high/low pressure oxygen, hydrogen, water recirculation, and water injection. The water injection subsystem supplies deionized (DI) water to a centralized reservoir for consumption. Subsequently, a water recirculation loop transfers the DI water across the cathode side of the electrolysis cell stack with constant flow rate. The result is a supply of hydrogen in the water loop and oxygen accumulation on the anode side of the cell stack. Hydrogen is evaporated out as part of the hydrogen sub-system which also measures hydrogen/oxygen concentration for safety. The oxygen subsystem is responsible for managing high pressure oxygen, O2 exhaust, and conducting hydrogen/oxygen concentration measurements. The nitrogen subsystem serves dual functions, purging the hydrogen/oxygen subsystems, and regulating pressure in both high/low-pressure O2 sections via pneumatic back pressure regulators. Various sensors monitor pressure, temperature, humidity, gas concentration and flow rate in each subsystem. This paper presents the design and testing of a comprehensive test stand, which serves to operate and functionally verify the performance of the electrolysis cell while offering valuable lessons learned.

electrolysis↗

DOE OSTI2025

Cost analysis of alternative large-scale high-temperature solid oxide electrolysis hydrogen production facilities

We extend our past cost analysis of gigawatt-scale solid oxide electrolysis (SOE) facilities that produce high purity hydrogen gas from water by estimating construction and operating costs for three new alternative design cases: (1) offsite feed steam generation; (2) near-atmospheric pressure (NAP) stack; and (3) onsite electric boiler feed steam generation. Pressure effects on hydrogen electrode-(cathode-)supported SOE cell (SOEC) stack performance are estimated for the same assumed cell and stack construction and used to determine facility-wide stack capital costs for achieving a fixed H2 production at different pressures. Modular balance of plant (BOP) process equipment capital costs are estimated for each new alternative design case using our past equipment sizing, design, and cost data and scaling relationships. Furthermore, we update BOP equipment sizing and design for the NAP case using Aspen®. Vendor quotes for electric boilers are used to estimate costs for the electric boiler design case. Factory and onsite assembly and installation costs for SOEC stacks and BOP equipment are calculated using our past simplified first-principles approach. First-of-a-kind (FOAK) and N th -of-a-kind (NOAK) production maturity cost estimates are included for all results. The case with NAP stacks offers the lowest facility total capital cost (TCC, ~23% lower than base) while use of small electric boilers requires the highest TCC (~3% higher than base). H 2 production prices decrease from the base of ~$\$2.17$ /kgH 2 to ~$\$1.92$/kgH 2 for 1 GW e DC SIP facilities utilizing NAP stacks supplied by offsites steam situated in large modules and blocks for $\$0.030$/kWh e and $0.009/kWh t prices for electricity and thermal energy, respectively. We report all costs in 2021 US dollars.

Balance of plant (BOP) process equipment↗

DOE OSTI2023

Modular Solar-to-Fuel Electrolysis at Low Cell Potentials Enabled by Glycerol Electrooxidation and a Bipolar Membrane Separator

Solar fuel generation through water electrolysis or electrochemical CO 2 reduction is thermodynamically limited when paired with the oxygen evolution reaction (OER). The glycerol electrooxidation reaction (GEOR) is an alternative anodic reaction with lower anodic electrochemical potential that utilizes a renewable coproduct produced during biodiesel synthesis. We show that GEOR on a Au-Pt-Bi ternary metal electrocatalyst in a model alkaline crude glycerol solution can provide significant cell potential reductions even when paired to reduction reactions in seawater and acidic catholytes via a bipolar membrane (BPM). We showed that the combination of GEOR electrooxidation and a BPM separator lowers the total cell potential by 1 V at an electrolysis current of 10.0 mA cm -2 versus to an anode performing OER when paired with hydrogen evolution and CO 2 reduction cathodes. The observed voltage reduction was steady for periods of up to 80 hours, with minimal glycerol crossover observed through the membrane. Furthermore, these results motivate new, high-performance cell designs for photoelectrochemical solar fuels integrated systems based on glycerol electrooxidation.

25 ENERGY STORAGE↗

DOE OSTI2021

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

In this study, we loaded Pd catalysts onto a reduced graphene oxide (rGO) support in an atomically dispersed fashion [i.e., Pd single-atom catalysts (SACs) on rGO or Pd 1 /rGO] via a facile and scalable synthesis based on anchor-site and photoreduction techniques. The as-synthesized Pd 1 /rGO significantly outperformed the Pd nanoparticle (Pdnano) counterparts in the electrocatalytic hydrodechlorination of chlorinated phenols. Downsizing Pd nano to Pd 1 leads to a substantially higher Pd atomic efficiency (14 times that of Pdnano), remarkably reducing the cost for practical applications. The unique single-atom architecture of Pd 1 additionally affects the desorption energy of the intermediate, suppressing the catalyst poisoning by Cl – , which is a prevalent challenge with Pdnano. Characterization and experimental results demonstrate that the superior performance of Pd 1 /rGO originates from (1) enhanced interfacial electron transfer through Pd–O bonds due to the electronic metal–support interaction and (2) increased atomic H (H*) utilization efficiency by inhibiting H 2 evolution on Pd 1 . Furthermore, this work presents an important example of how the unique geometric and electronic structure of SACs can tune their catalytic performance toward beneficial use in environmental remediation applications.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Direct Ink Writing of 3D Zn Structures as High‐Capacity Anodes for Rechargeable Alkaline Batteries

The relationship between structure and performance in alkaline Zn batteries is undeniable, where anode utilization, dendrite formation, shape change, and passivation issues are all addressable through anode morphology. While tailoring 3D hosts can improve the electrode performance, these practices are inherently limited by scaffolds that increase the mass or volume. Herein, a direct write strategy for producing template‐free metallic 3D Zn electrode architectures is discussed. Concentrated inks are customized to build designs with low electrical resistivity (5 × 10 −4 Ω cm), submillimeter sizes (200 μm filaments), and high mechanical stability (Young's modulus of 0.1–0.5 GPa at relative densities of 0.28–0.46). A printed Zn lattice anode versus NiOOH cathode with an alkaline polymer gel electrolyte is then demonstrated. This Zn||NiOOH cell operates for over 650 cycles at high rates of 25 mA cm −2 with an average areal capacity of 11.89 mAh cm −2 , a cumulative capacity of 7.8 Ah cm −2 , and a volumetric capacity of 23.78 mAh cm −3 . A thicker Zn anode achieves an ultrahigh areal capacity of 85.45 mAh cm −2 and a volumetric capacity of 81.45 mAh cm −3 without significant microstructural changes after 50 cycles.

25 ENERGY STORAGE↗

DOE OSTI2017

First-Principles-Based Computational Study on Nucleation and Growth Mechanisms of U on Mo(110) Surface Solvated in an Eutectic LiCl-KCl Molten Salt

In nuclear engineering and industry electrochemical methods have been intensively employed in pyro-processing technology to recycle used nuclear fuels for substantial alleviation of the concern with the safe treatment of high-level radioactive nuclear wastes. Pyro-processing is based on sequential electrochemical reactions at high temperature (typically above 700 K at ambient pressure) to enhance the efficiency for decoupling nuclear fuels from unfavorable fission fragments. Using a molten salt in electrorefining process, at which actinides can be selectively deposited in solid cathode from ionic states, gives several advantages over an aqueous solution: higher thermal conductivity (it is liquid phase at high temperature, molten salt plays a role as medium at high temperature over 773 K in electrochemical reaction, lower kinetic barrier in ionic diffusion mobility and better stability against undesired side reactions with radioactive materials. Therefore, the volume of high-level nuclear wastes to be, otherwise, disposed into secured sites is dramatically reduced. Most of all it conforms to nuclear non-proliferation treaty. Electrochemical reactions in a molten salt medium are, however, much more complicated than in aqueous solution rendering the accurate understanding of thermodynamic and kinetic properties formidably challenging. It is represented by extensive researches in experiments and computations to identify underlying mechanisms on how U and other fission fragments behave in the electrorefining system. Regardless of the researches there is a general agreement that the initial stage of the nucleation and growth process of the U deposit is critical for determining the properties of final product and the electrorefining efficiency. In spite of the focused studies it still remains unclear. Theoretical and computational researches have been often carried out with various empirical parameter for interatomic potential energy, which are unknown variables until numerical fits to experimental measurements or just assumption is made. Thus, empirical simulations sometimes predicted outcomes are inconsistent depending on materials of interest with experimental measurements. This may be largely because the accuracy of an empirical interatomic potential energy models critically depends on the input parameters and thus, can be limited in transferability of the results. Furthermore, it may be devoid of fundamental physics or chemistry. This situation requires special caution when an electrorefining system is studied to recycle spent nuclear fuels because of the extreme difficulty in reliable acquisition of thermodynamic and kinetic data from direct experimental measurements. In this presentation, we extensively utilized first principles density functional theory (DFT) calculations and ab-initio molecular dynamic (AIMD) simulations to figure out underlying mechanisms of the initial stage of nucleation and growth behaviors of U on Mo(110) surface in a eutectic LiCl-KCl molten salt at T = 773 K. To rigorously investigate the effect of the molten salt electrolyte we compared the results with those calculated under vacuum condition.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Carbon dioxide reduction in solid oxide electrolyzer cells using transition metals infiltrated into Gd 0.1 Ce 0.9 O 1.95 (GDC10) scaffolds

Here, this study reports the catalytic activity of transition metal electrocatalysts (Co, Ni, and Cu) incorporated into Gd 0.1 Ce 0.9 O 1.95 (GDC10) cathodes for the electroreduction of CO 2 in solid oxide electrolyzer cells (SOECs). CO 2 electroreduction performance of cells having porous and non-infiltrated GDC10 cathodes was compared with the performance of cells containing transition metal electrocatalysts infiltrated into porous GDC10 cathodes at 750, 800, and 850°C. Results showed that cells with Co infiltrated cathodes had the best catalytic activity towards CO 2 electroreduction. Furthermore, these cells displayed good stability towards CO electroreduction, having a faradaic efficiency value close to 100% with insignificant voltage increase when tested for 48h at 750 and 850°C under the current densities of 0.2, and 0.4Acm -2 , respectively.

25 ENERGY STORAGE↗

DOE OSTI2025

Finite element modeling of electropolishing of radio frequency dipole Nb crab cavity in hydrofluoric-sulfuric acid electrolyte

The superior performance of niobium superconducting radio frequency (SRF) cavities is achieved through meticulous surface treatment, notably via chemical electropolishing, ensuring exceptionally smooth surfaces. While this technique has been extensively employed for cylindrically symmetric structures, addressing more intricate geometries poses significant challenges in achieving uniform polishing and controlled material removal, especially when moving away from retractable cathodes. This presents a multifaceted electrochemical, thermal, and fluid dynamics conundrum. A prime example is the 197 MHz radio frequency dipole (RFD) crabbing cavity proposed for the Electron Ion Collider (EIC) project, exemplifying such complex structures. Our groundbreaking work integrates the localized oxide thickness variation, considering its impact on current distribution and Joule heating, within the framework of multi-physics modeling using the COMSOL® simulation suite. This approach was applied to a comprehensive model of the RFD cavity, allowing us to investigate optimal external cooling water flow conditions necessary for achieving desirable outcomes. In conclusion, this illustrates the increasing utility of such multi-physics codes to greatly aid in designing solutions to challenging processing requirements for increasingly complex accelerator cavities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

Chemisorption of polysulfides through redox reactions with organic molecules for lithium–sulfur batteries

Lithium-sulfur battery possesses high energy density but suffers from severe capacity fading due to the dissolution of lithium polysulfides. Novel design and mechanisms to encapsulate lithium polysulfides are greatly desired by high-performance lithium-sulfur batteries towards practical applications. Herein, we report a strategy of utilizing anthraquinone, a natural abundant organic molecule, to suppress dissolution and diffusion of polysulfides species through redox reactions during cycling. The keto groups of anthraquinone play a critical role in forming strong Lewis acid-based chemical bonding. This mechanism leads to a long cycling stability of sulfur-based electrodes. With a high sulfur content of ~73%, a low capacity decay of 0.019% per cycle for 300 cycles and retention of 81.7% over 500 cycles at 0.5 C rate can be achieved. Here, this finding and understanding paves an alternative avenue for the future design of sulfur-based cathodes toward the practical application of lithium-sulfur batteries.

25 ENERGY STORAGE↗

DOE OSTI2019

Quantification of Heterogeneous Degradation in Li-Ion Batteries

The multiscale chemomechanical interplay in lithium-ion batteries builds up mechanical stress, provokes morphological breakdown, and leads to state of charge heterogeneity. Quantifying the interplay in complex composite electrodes with multiscale resolution constitutes a frontier challenge in precisely diagnosing the fading mechanism of batteries. In this work, hard X-ray phase contrast tomography, capable of nanoprobing thousands of active particles at once, enables an unprecedented statistical analysis of the chemomechanical transformation of composite electrodes under fast charging conditions. The damage heterogeneity is demonstrated to prevail at all length scales, which stems from the unbalanced electron conduction and ionic diffusion, and collectively leads to the nonuniform utilization of active particles spatially and temporally. This research highlights that the statistical mapping of the chemomechanical transformation offers a diagnostic method for the particles utilization and fading, hence could improve electrode formulation for fast-charging batteries.

25 ENERGY STORAGE↗

DOE OSTI2023

Designing High‐Donicity Anions for Rechargeable Potassium Superoxide/Peroxide Batteries

Abstract A battery cathode based on the superoxide/peroxide redox not only inherits the advantage of oxygen (O 2 ) batteries in high capacities and low costs but also overcomes the disadvantages in O 2 storage, electrolyte evaporation, and anode deactivation due to O 2 crossover. Herein, we report an enhanced potassium superoxide (KO 2 )/peroxide (K 2 O 2 ) conversion by adopting a high‐donicity anion additive in the ether‐based electrolyte. Such an anion was synthesized via a “Solvent‐in‐Anion” strategy and validated to enhance the electron donicity of the electrolyte. The use of high‐donicity anion could lead to enhanced KO 2 utilization (≈90.2 %) by retarding electrode passivation and allow the full charging back of K 2 O 2 through the solution‐mediated pathway without electrocatalysts. No apparent cell degradation is observed during the first 120 cycles by controlling the reversible depth‐of‐discharge capacity at 292 mAh g −1 within an O 2 ‐free region. The K−KO 2 cell delivers a high energy efficiency (>84.4 %) and a lifespan of over 1440 hours.

Qin, Lei↗

DOE OSTI2023

Designing High‐Donicity Anions for Rechargeable Potassium Superoxide/Peroxide Batteries

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

A Full-Cell Model for Direct Toluene Electro-Hydrogenation Electrolysis

Liquid organic hydrogen carriers (LOHCs) are organic molecules that undergo a hydrogenation/dehydrogenation cycle to enable storage and transportation of hydrogen fuel under ambient conditions. One promising LOHC candidate is toluene, which can be converted to methylcyclohexane (MCH) electrochemically, enabling a decarbonized process when green electricity is used. In this study, we developed a full-cell model for the direct electro-hydrogenation of toluene to MCH, utilizing a zero-gap membrane electrode assembly architecture. The model incorporates electrochemical kinetics, ionic transport, water transport across the membrane, and mass transport effects. Electrochemical kinetics are characterized using Tafel analysis on Pt/Ru catalyst. The model is validated against experimental data, including polarization curves, Faradaic efficiencies, and water crossover. A voltage breakdown analysis shows that the performance is dominated by kinetic losses, and the model is used to carry out a comparison of different toluene electro-hydrogenation reaction catalysts. Finally, a sensitivity analysis is conducted on key design parameters illustrating which can be modified to maximize electrolyzer performance. The cathode specific surface area and cathode porous transport layer thickness (PTL) have the largest impact on the current density, while the PTL thickness and Pt loading in the PTL have the largest impact on Faradaic efficiency.

Ehlinger, Victoria M. [Lawrence Livermore National↗

DOE OSTI2021

High Performance Air Breathing Flexible Lithium–Air Battery

Lithium–oxygen (Li–O 2 ) batteries possess the highest theoretical energy density (3500 Wh kg –1 ), which makes them attractive candidates for modern electronics and transportation applications. In this work, an inexpensive, flexible, and wearable Li–O 2 battery based on the bifunctional redox mediator of InBr 3 , MoS 2 cathode catalyst, and Fomblin-based oxygen permeable membrane that enable long-cycle-life operation of the battery in pure oxygen, dry air, and ambient air is designed, fabricated, and tested. The battery operates in ambient air with an open system air-breathing architecture and exhibits excellent cycling up to 240 at the high current density of 1 A g –1 with a relative humidity of 75%. The electrochemical performance of the battery including deep-discharge capacity, and rate capability remains almost identical after 1000 cycle in a bending fatigue test. Furthermore, this finding opens a new direction for utilizing high performance Li–O 2 batteries for applications in the field of flexible and wearable electronics.

25 ENERGY STORAGE↗

DOE OSTI2017

High Energy, Long Cycle Life Lithium-ion Batteries for PHEV Application

High-loading and high quality PSU Si anode has been optimized and fabricated. The electrochemical performance has been utilized. The PSU Si-graphite anode exhibits the mass loading of 5.8 mg/cm2, charge capacity of 850 mAh/ g and good cycling performance. This optimized electrode has been used for full-cell fabrication. The performance enhancement of Ni-rich materials can be achieved by a diversity of strategies. Higher Mn content and a small amount of Al doping can improve the electrochemical performance by suppressing interfacial side reactions with electrolytes, thus greatly benefiting the cyclability of the samples. Also, surface coatings of Li-rich materials and AlF 3 are able to improve the performance stability of Ni-rich cathodes. One kilogram of optimized concentration-gradient LiNi 0.76 Co 0.10 Mn 0.14 O 2 (CG) with careful control of composition, morphology and electrochemical performance was delivered to our collaborators. The sample achieved an initial specific capacity close to 190 mA h g -1 at C/10 rate and 180 mA h g -1 at C/3 rate as well as good cyclability in pouch full cells with a 4.4 V upper cut-off voltage at room temperature. Electrolyte additive with Si-N skeleton forms a less resistant SEI on the surface of silicon anode (from PSU) as evidenced by the evolution of the impedance at various lithiation/de-lithiation stages and the cycling data The prelithiation result demonstrates a solution processing method to achieve large area, uniform SLMP coating on well-made anode surface for the prelithiation of lithium-ion batteries. The prelithiation effect with this method is applied both in graphite half cells, graphite/NMC full cells, SiO half cells, SiO/NMC full cells, Si-Graphite half cells and Si-Graphite/NMC full cells with improvements in cycle performance and higher first cycle coulombic efficiency than their corresponding cells without SLMP prelithiation. As to the full cell fabrication and test, full pouch cells with high capacity of 2.2 Ah and 1.2 Ah have been fabricated and delivered. The cells show great uniformity and good cycling performance. The prelithiation method effectively compensate the loss in the first cycle. The cell with high energy density and long-cycle life has been achieved.

25 ENERGY STORAGE↗