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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 847 records · Page 47
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Spin pinning effect to reconstructed oxyhydroxide layer on ferromagnetic oxides for enhanced water oxidation

Producing hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. With spin-dependent kinetics in OER, to manipulate the spin ordering of ferromagnetic OER catalysts (e.g., by magnetization) can reduce the kinetic barrier. However, most active OER catalysts are not ferromagnetic, which makes the spin manipulation challenging. In this work, we report a strategy with spin pinning effect to make the spins in paramagnetic oxyhydroxides more aligned for higher intrinsic OER activity. The spin pinning effect is established in oxideFM/oxyhydroxide interface which is realized by a controlled surface reconstruction of ferromagnetic oxides. Under spin pinning, simple magnetization further increases the spin alignment and thus the OER activity, which validates the spin effect in rate-limiting OER step. The spin polarization in OER highly relies on oxyl radicals (O∙) created by 1 st dehydrogenation to reduce the barrier for subsequent O-O coupling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

High-energy and low-cost membrane-free chlorine flow battery

Abstract Grid-scale energy storage is essential for reliable electricity transmission and renewable energy integration. Redox flow batteries (RFB) provide affordable and scalable solutions for stationary energy storage. However, most of the current RFB chemistries are based on expensive transition metal ions or synthetic organics. Here, we report a reversible chlorine redox flow battery starting from the electrolysis of aqueous NaCl electrolyte and the as-produced Cl 2 is extracted and stored in the carbon tetrachloride (CCl 4 ) or mineral spirit flow. The immiscibility between the CCl 4 or mineral spirit and NaCl electrolyte enables a membrane-free design with an energy efficiency of >91% at 10 mA/cm 2 and an energy density of 125.7 Wh/L. The chlorine flow battery can meet the stringent price and reliability target for stationary energy storage with the inherently low-cost active materials (~$5/kWh) and the highly reversible Cl 2 /Cl − redox reaction.

25 ENERGY STORAGE↗
DOE OSTI2022

Surface restructuring of a perovskite-type air electrode for reversible protonic ceramic electrochemical cells

Reversible protonic ceramic electrochemical cells (R-PCECs) are ideally suited for efficient energy storage and conversion; however, one of the limiting factors to high performance is the poor stability and insufficient electrocatalytic activity for oxygen reduction and evolution of the air electrode exposed to the high concentration of steam. Here we report our findings in enhancing the electrochemical activity and durability of a perovskite-type air electrode, Ba 0.9 Co 0.7 Fe 0.2 Nb 0.1 O 3-δ (BCFN), via a water-promoted surface restructuring process. Under properly-controlled operating conditions, the BCFN electrode is naturally restructured to an Nb-rich BCFN electrode covered with Nb-deficient BCFN nanoparticles. When used as the air electrode for a fuel-electrode-supported R-PCEC, good performances are demonstrated at 650 °C, achieving a peak power density of 1.70 W cm –2 in the fuel cell mode and a current density of 2.8 A cm –2 at 1.3 V in the electrolysis mode while maintaining reasonable Faradaic efficiencies and promising durability.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

Heterogenous electromediated depolymerization of highly crystalline polyoxymethylene

Abstract Post-consumer plastic waste in the environment has driven the scientific community to develop deconstruction methods that yield valued substances from these synthetic macromolecules. Electrocatalysis is a well-established method for achieving challenging transformations in small molecule synthesis. Here we present the first electro-chemical depolymerization of polyoxymethylene—a highly crystalline engineering thermoplastic (Delrin®)—into its repolymerizable monomer, formaldehyde/1,3,5-trioxane, under ambient conditions. We investigate this electrochemical deconstruction by employing solvent screening, cyclic voltammetry, divided cell studies, electrolysis with redox mediators, small molecule model studies, and control experiments. Our findings determine that the reaction proceeds via a heterogeneous electro-mediated acid depolymerization mechanism. The bifunctional role of the co-solvent 1,1,1,3,3,3-hexafluoro-2-propanol (HFIP) is also revealed. This study demonstrates the potential of electromediated depolymerization serving as an important role in sustainable chemistry by merging the concepts of renewable energy and circular plastic economy.

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

A scalable membrane electrode assembly architecture for efficient electrochemical conversion of CO2 to formic acid

Abstract The electrochemical reduction of carbon dioxide to formic acid is a promising pathway to improve CO 2 utilization and has potential applications as a hydrogen storage medium. In this work, a zero-gap membrane electrode assembly architecture is developed for the direct electrochemical synthesis of formic acid from carbon dioxide. The key technological advancement is a perforated cation exchange membrane, which, when utilized in a forward bias bipolar membrane configuration, allows formic acid generated at the membrane interface to exit through the anode flow field at concentrations up to 0.25 M. Having no additional interlayer components between the anode and cathode this concept is positioned to leverage currently available materials and stack designs ubiquitous in fuel cell and H 2 electrolysis, enabling a more rapid transition to scale and commercialization. The perforated cation exchange membrane configuration can achieve >75% Faradaic efficiency to formic acid at <2 V and 300 mA/cm 2 in a 25 cm 2 cell. More critically, a 55-hour stability test at 200 mA/cm 2 shows stable Faradaic efficiency and cell voltage. Technoeconomic analysis is utilized to illustrate a path towards achieving cost parity with current formic acid production methods.

08 HYDROGEN↗
DOE OSTI2025

Enhancing surface activity and durability in triple conducting electrode for protonic ceramic electrochemical cells

With the material system operating at lower temperatures, protonic ceramic electrochemical cells (PCECs) can offer high energy efficiency and reliable performance for both power generation and hydrogen production, making them a promising technology for reversible energy cycling. However, PCEC faces technical challenges, particularly regarding electrode activity and durability under high current density operations. To address these challenges, we introduce a nano-architecture oxygen electrode characterized by high porosity and triple conductivity, designed to enhance catalytic activity and interfacial stability through a self-assembly approach, while maintaining scalability. Electrochemical cells incorporating this advanced electrode demonstrate robust performance, achieving a peak power density of 1.50 W cm −2 at 600 °C in fuel cell mode and a current density of 5.04 A cm −2 at 1.60 V in electrolysis mode, with enhanced stability on transient operations and thermal cycles. The underlying mechanisms are closely related to the improved surface activity and mass transfer due to the dual features of the electrode structure. Additionally, the enhanced interfacial bonding between the oxygen electrode and electrolyte contributes to increased durability and thermomechanical integrity. This study underscores the critical importance of optimizing electrode microstructure to achieve a balance between surface activity and durability.

Protonic Ceramic Electrochemical Cells↗
DOE OSTI2025

Interconnected nanoconfining pore networks enhance catalyst CO 2 interaction in electrified reactive capture

Systems that sequentially capture and upgrade CO 2 from air to fuels/fuel-intermediates, such as syngas and ethylene, rely on an energy-intensive CO 2 release process. Electrified reactive capture systems transform CO 2 obtained directly from carbonate capture liquid into products. Previous reactive capture systems show a decline in Faradaic efficiencies (FE) at current densities above 200 mA/cm 2 . Here we show the chemical origins of this problem, finding that prior electrocatalyst designs failed to arrest, activate, and reduce in situ-generated CO 2 (i-CO 2 ) before it traversed the catalyst layer and entered the tailgas stream. We develop a templated synthesis to define pore structures and the sites of Ni single atoms, and find that carbon-nitrogen-based nanopores are effective in accumulating i-CO 2 via short-range, non-electrostatic interactions between CO 2 molecules and the nanochannel walls. These interactions confine and enrich i-CO 2 within the pores, enhancing its binding and activation. We report as a result carbonate electrolysis at 300 mA/cm 2 with FE to CO of 50% ± 3%, and with <1% CO 2 in the tailgas outlet stream. This corresponds to a projected energy efficiency (EE) to 2:1 syngas of 46% at 300 mA/cm 2 when H 2 is added using a water electrolyzer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Pathways to cost competitive and viable lithium production from Salton Sea geothermal brines

Lithium supply chains remain heavily concentrated in hard rock and brine resources, creating significant supply risks. Geothermal brines represent an underutilized alternative, yet commercial progress is hindered by the absence of facility-scale cost assessments. Here, we present a techno-economic analysis of large-scale lithium extraction from Salton Sea geothermal brines, drawing on primary company disclosures, process patents, and brine resource modeling. Caused by varying lithium and impurity concentrations, brine dilution over time, and process configurations (e.g., production via carbonation and conversion vs. electrolysis), we find that large-scale production costs may reach ~10,000 United States dollars per ton, but increase up to 22,000 United States dollars per ton with higher certainty of brine modeling, raising concerns about economic competitiveness to conventional low-cost sources. Finally, a project feasibility-focused scenario analyses shows that leveraging brine pre-treatment by-product sales could lower long-term lithium break-even prices by ~5,000 United States dollars per ton, whereas capital cost optimization of 20% could further reduce lithium break-even prices by 10%.

Wesselkaemper, Jannis↗
DOE OSTI2022

Gas diffusion electrodes, reactor designs and key metrics of low-temperature CO 2 electrolysers

We report that CO 2 emissions can be recycled via low-temperature CO 2 electrolysis to generate products such as carbon monoxide, ethanol, ethylene, acetic acid, formic acid and propanol. In recent years, progress has been made towards an industrially relevant performance by leveraging the development of gas diffusion electrodes (GDEs), which enhance the mass transport of reactant gases (for example, CO 2 ) to the active electrocatalyst. Innovations in GDE design have thus set new benchmarks for CO 2 conversion activity. In this Review, we discuss GDE-based CO 2 electrolysers, in terms of reactor designs, GDE composition and failure modes, to identify the key advances and remaining shortfalls of the technology. This is combined with an overview of the partial current densities, efficiencies and stabilities currently achieved and an outlook on how phenomena such as carbonate formation could influence the future direction of the field. Our aim is to capture insights that can accelerate the development of industrially relevant CO 2 electrolysers.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction

Water electrolysis is a key technology to establish CO 2 -neutral hydrogen production. Nonetheless, the near-surface structure of electrocatalysts during the anodic oxygen evolution reaction (OER) is still largely unknown, which hampers knowledge-driven optimization. Here using operando X-ray absorption spectroscopy and density functional theory calculations, we provide quantitative near-surface structural insights into oxygen-evolving CoO x (OH) y nanoparticles by tracking their size-dependent catalytic activity down to 1 nm and their structural adaptation to OER conditions. We uncover a superior intrinsic OER activity of sub-5 nm nanoparticles and a size-dependent oxidation leading to a near-surface Co–O bond contraction during OER. We find that accumulation of oxidative charge within the surface Co 3+ O 6 units triggers an electron redistribution and an oxyl radical as predominant surface-terminating motif. This contrasts the long-standing view of high-valent metal ions driving the OER, and thus, our advanced operando spectroscopy study provides much needed fundamental understanding of the oxygen-evolving near-surface chemistry.

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

Concentrating on solar for hydrogen

Hydrogen generated by sunlight could play a major role in a low-carbon future, but high-efficiency demonstrations have been limited mostly to very small scales. New research now evaluates a complete system that generates 0.5 kg of hydrogen per day with 20% device (5.5% system) efficiency while showing the benefits of coupled light absorption and water electrolysis.

08 HYDROGEN↗
DOE OSTI2023

Lowering the operating temperature of protonic ceramic electrochemical cells to <450 °C

Protonic ceramic electrochemical cells (PCECs) can be employed for power generation and sustainable hydrogen production. Lowering the PCEC operating temperature can facilitate its scale-up and commercialization. However, achieving high energy efficiency and long-term durability at low operating temperatures is a long-standing challenge. Here, in this work, we report a simple and scalable approach for fabricating ultrathin, chemically homogeneous, and robust proton-conducting electrolytes and demonstrate an in situ formed composite positive electrode, Ba 0.62 Sr 0.38 CoO 3–δ –Pr 1.44 Ba 0.11 Sr 0.45 Co 1.32 Fe 0.68 O 6–δ , which significantly reduces ohmic resistance, positive electrode–electrolyte contact resistance and electrode polarization resistance. The PCECs attain high power densities in fuel-cell mode (~0.75 W cm –2 at 450 °C and ~0.10 W cm –2 at 275 °C) and exceptional current densities in steam electrolysis mode (–1.28 A cm –2 at 1.4 V and 450 °C). At 600 °C, the PCECs achieve a power density of ~2 W cm –2 . Additionally, we demonstrate the direct utilization of methane and ammonia for power generation at <450 °C. Our PCECs are also stable for power generation and hydrogen production at 400 °C.

25 ENERGY STORAGE↗
DOE OSTI2025

Decoupling the catalytic and degradation mechanisms of cobalt active sites during acidic water oxidation

Advancement of iridium-free catalysts for the low-pH oxygen evolution reaction (OER) is required to enable multi-gigawatt-scale proton-exchange water electrolysis. Cobalt-based materials might address this requirement, but little is known about the mechanism of operation of these OER catalysts at low pH. Here we investigate the nature and evolution of the active cobalt sites along with charge- and mass-transfer processes that support their catalytic function within a cobalt–iron–lead oxide material using in situ spectroscopic, gravimetric and electrochemical techniques. We demonstrate that corrosion of the cobalt sites and their reformation through electrooxidation of dissolved Co 2+ do not affect the catalytic mechanism and are decoupled from the OER. The OER-coupled charge transfer is supported by Co (3+δ)+ -oxo-species, which are structurally different from those reported for alkaline/near-neutral conditions and are formed on a relatively slow timescale of minutes. These mechanistic insights might assist in developing genuinely practical catalysts for this vital technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Mitigation of hydrogen crossover in liquid alkaline water electrolysers using gas recombination catalysts

The rising demand for hydrogen calls for improvements in the efficiency of liquid alkaline water electrolysers (LAWEs), which can be fulfilled by advanced electrodes or separators. Nevertheless, they also intensify hydrogen crossover and safety concerns, thus mandating efficient mitigation strategies. Here we studied the correlation between cathodes and hydrogen crossover behaviours and mitigated safety risks by designing a gas recombination catalyst (GRC). We attribute the elevated hydrogen crossover associated with platinum-based cathodes to their preferential utilization for the hydrogen evolution reaction that creates elevated hydrogen supersaturation, as evidenced by direct measurements of dissolved hydrogen concentration. Varying the placement of platinum layers relative to the cathode–separator interface also supports this conclusion. The implementation of a GRC reduces hydrogen crossover by 95% without affecting LAWE performance and functions for over 1,000 h at 1 A cm−2. This study provides insights into hydrogen supersaturation and the crossover mechanism, as well as offering a promising pathway to enhance the efficiency and reliability of alkaline water electrolysis.

Liu, Haotian↗
DOE OSTI2020

Triple ionic–electronic conducting oxides for next-generation electrochemical devices

Triple ionic–electronic conductors (TIECs) are materials that can simultaneously transport electronic species alongside two ionic species. The recent emergence of TIECs provides intriguing opportunities to maximize performance in a variety of electrochemical devices, including fuel cells, membrane reactors and electrolysis cells. However, the potential application of these nascent materials is limited by lack of fundamental knowledge of their transport properties and electrocatalytic activity. The goal of this Review is to summarize and analyse the current understanding of TIEC transport and electrochemistry in single-phase materials, including defect formation and conduction mechanisms. In this work, we particularly focus on the discovery criteria (for example, crystal structure and ion electronegativity), design principles (for example, cation and anion substitution chemistry) and operating conditions (for example, atmosphere) of materials that enable deliberate tuning of the conductivity of each charge carrier. Lastly, we identify important areas for further advances, including higher chemical stability, lower operating temperatures and discovery of n-type TIEC materials.

25 ENERGY STORAGE↗
DOE OSTI2024

Materials descriptors for advanced water dissociation catalysts in bipolar membranes

The voltage penalty driving water dissociation (WD) at high current density is a major obstacle in the commercialization of bipolar membrane (BPM) technology for energy devices. Here, in this study, we show that three materials descriptors, that is, electrical conductivity, microscopic surface area and (nominal) surface-hydroxyl coverage, effectively control the kinetics of WD in BPMs. Using these descriptors and optimizing mass loading, we design new earth-abundant WD catalysts based on nanoparticle SnO 2 synthesized at low temperature with high conductivity and hydroxyl coverage. These catalysts exhibit exceptional performance in a BPM electrolyser with low WD overvoltage (η wd ) of 100 ± 20 mV at 1.0 A cm -2 . The new catalyst works equivalently well with hydrocarbon proton-exchange layers as it does with fluorocarbon-based Nafion, thus providing pathways to commercializing advanced BPMs for a broad array of electrolysis, fuel-cell and electrodialys is applications.

Sasmal, Sayantan↗
DOE OSTI2022

Revitalizing interface in protonic ceramic cells by acid etch

Protonic ceramic electrochemical cells hold the promise to be operated at intermediate temperatures below 600 °C. Although the high proton conductivity of the bulk electrolyte has been demonstrated, it cannot be fully utilized in electrochemical full cells due to unknown causes. A practical solution is thus urgently needed. Here we showed that it comes from poor contacts between the low-temperature processed oxygen electrode-electrolyte interface. We demonstrated that a simple acid treatment can effectively rejuvenate the high-temperature annealed electrolyte surface, resulting in reactive bonding between the oxygen electrode and the electrolyte and improved electrochemical performance and stability. This enables exceptional protonic ceramic fuel-cell performance down to 350 °C, with peak power densities of 1.6 W cm -2 at 600 °C, 650 mW cm -2 at 450 °C, and 300 mW cm -2 at 350 °C, as well as stable electrolysis operations at large current densities above 3.9 A cm -2 under 1.4 V applied voltage at 600 °C. Furthermore, our work highlights the critical role of interfacial engineering in ceramic electrochemical devices and offers new understanding and practices towards sustainable energy infrastructure.

08 HYDROGEN↗
DOE OSTI2025

Co-sputtered CuNi heteroatomic electrocatalyst for enhanced 5-hydroxymethylfurfural selective electrochemical conversion

The electrochemical conversion of biomass-derived 5-hydroxymethylfurfural (HMF) represents a promising, economically viable, and environmentally sustainable approach for producing value-added chemicals using renewable energy and in situ hydrogen generated through water electrolysis. However, the electrochemical hydrogenation (ECH) of HMF remains challenging due to the inherently low catalytic activity and selectivity of the electrodes, compounded by competition with the kinetically favored hydrogen evolution reaction (HER) in aqueous electrolytes. In this work, we demonstrate that Cu x Ni 100−x heteroatomic thin films, fabricated via direct current (DC) magnetron co-sputtering, achieve a more than one order of magnitude increase in the HMF to 2,5-Bis-hydroxymethylfuran (BHMF) conversion rate, with nearly 50% faradic efficiency (FE) for BHMF, when compared to pure Cu and Ni electrodes (~ 10% BHMF FE). Our results suggest that the synergistic interaction between Cu and Ni creates an optimal catalytic environment for both HMF and adsorbed hydrogen (H ads ) species, thereby enhancing BHMF formation through the ECH pathway.

36 MATERIALS SCIENCE↗