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DOE OSTI2020

Hidden figures of photo-charging: a thermo-electrochemical approach for a solar-rechargeable redox flow cell system

Achieving high current densities without thermal performance degradation at high temperatures is one of the main challenges for enhancing the competitiveness of photo-electrochemical energy storage systems. We describe a system that overcomes this challenge by incorporating an integrated photoelectrode with a redox flow cell, which functions as a coolant for the excess heat from the photo-absorber. We perform quantitative analyses to theoretically validate and highlight the merit of the system. Practical operation parameters, including daily temperature and redox reaction kinetics, are modeled with respect to heat and charge transfer mechanisms. Our analyses show a profound impact on the resulting solar-to-chemical efficiencies and stored power, which are 21.8% higher than that of a conventional photovoltaic-assisted energy storage system. This paves the way for reassessing the merit of photovoltaic-integrated systems, which have hitherto been underrated as renewable energy storage systems.

25 ENERGY STORAGE↗

DOE OSTI2021

Doping-modulated strain control of bifunctional electrocatalysis for rechargeable zinc–air batteries

Changes in the local atomic arrangement in a crystal caused by lattice-mismatch-induced strain can efficiently regulate the performance of electrocatalysts for zinc–air batteries (ZABs) in many manners, mainly due to modulated electronic structure configurations that affect the adsorption energies for oxygen-intermediates formed during oxygen reduction and evolution reactions (ORR and OER). However, the application of strain engineering in electrocatalysis has been limited by the strain relaxation caused by structural instability such as dissolution and destruction, leading to insufficient durability towards the ORR/OER. In this work, we propose a doping strategy to modulate the phase transition and formation of self-supported cobalt fluoride–sulfide (CoFS) nanoporous films using a low amount of copper (Cu) as a dopant. This well-defined Cu–CoFS heterostructure overcomes the obstacle of structural instability. Our study of the proposed Cu–CoFS also helps establish the structure–property relationship of strained electrocatalysts by unraveling the role of local strain in regulating the electronic structure of the catalyst. As a proof-of-concept, the Cu–CoFS electrocatalyst with doping-modulated strain exhibited superior onset potentials of 0.91 V and 1.49 V for the ORR and OER, respectively, surpassing commercial Pt/C@RuO 2 and benchmarking non-platinum group metal (non-PGM) catalysts. ZABs with the Cu–CoFS catalyst delivered excellent charge/discharge cycling performance with an extremely low voltage gap of 0.5 V at a current density of 10 mA cm –2 and successively 0.93 V at a high current density of 100 mA cm –2 and afforded an outstanding peak power density of 255 mW cm –2 .

25 ENERGY STORAGE↗

DOE OSTI2024

Durable and High-Performance SOECs Based on Proton Conductors for Hydrogen Production

Proton-conducting solid oxide electrolysis cells (P-SOECs) are a promising technology for cost-effective and efficient production of green hydrogen. Breakthroughs in materials development, optimization of cell structure, and achievement of high performance and durability are essential to significantly increase the commercial competitiveness of these technologies. The main objective of this project is to gain scientific knowledge for the rational design, fabrication, and demonstration of a robust, highly efficient, and low-cost SOEC technology based on a proton-conducting electrolyte membrane for hydrogen production. We focused on better understanding the degradation mechanisms of proton-conducting electrolytes, air electrodes, and catalyst materials under electrolysis mode to develop an effective strategy for rationalizing new materials that are vital for enhancing cell performance and durability. The scope includes enhancing the performance and durability of the electrolyte and electrode materials under realistic operating conditions, developing highly active and robust catalysts to minimize electrode losses while improving tolerance to contaminant poisoning, revealing the mechanism of enhanced activity and stability of the catalyst, and understanding the underlying degradation mechanisms. In addition, various characterization techniques were employed to gain a fundamental understanding of the materials’ behavior and their impact on cell performance, providing vital information to guide materials discovery and cell design. After defect chemistry engineering, the optimized donor and acceptor co-doped electrolytes BaMo/W 0.03 Ce 0.71 Yb 0.26 O 3-δ (BM/W03) showed substantially improved chemical stability against high concentrations of CO 2 and H 2 O compared to the state-of-the-art electrolyte (BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3-δ , BZCYYb1711) while maintaining comparable ionic conductivity and ionic transference number. To bypass the inherent trade-off between conductivity and chemical stability, we fabricated a bi-layer electrolyte composed of BZCYYb1711 coated with a highly-stable thin layer of BaHf 0.83 Yb 0.17 O 3-δ (BHYb). This bi-layer electrolyte displayed excellent chemical stability against high concentration CO 2 ; there was no detectable formation of BaCO 3 after exposure to 97% CO 2 (with 3% H 2 O) at 500 °C for 1000 hours and the rate of degradation in resistance was about 0.4% per 1,000 hours (kh). In contrast, the same BZCYYb1711 electrolyte without a BHYb coating degraded significantly under the same testing conditions; the degradation rate was increased to 5.1%/kh. In addition, a triple conducting air electrode Ba 0.9 Pr 0.1 Hf 0.1 Y0.1Co 0.8 O 3-δ (BPHYC) was developed by heavily doping transition metal ions into a proton-conducting material. This air electrode material, composed of 3 distinct phases, exhibits superior electrocatalytic activity due to the synergistic effect from the three component phases. Moreover, an active and durable catalyst, La 2 Ni 0.5 Fe 0.5 O 4+δ (LNF), was developed, showing excellent catalytic activity and contaminant tolerance, with a degradation rate of only 0.49%/kh when exposed to high concentrations of steam and Cr. Finally, single cells were constructed from the best electrolytes, electrodes, and catalyst coatings developed in this project. These cells demonstrated superior high current density at a given cell voltage, high roundtrip efficiency, and remarkable durability (up to 1000 hours of operation).

08 HYDROGEN↗

NASA NTRS1983

Direct coronal heating from dissipation of magnetic field

The visible corona of the Sun appears to be heated by direct dissipation of magnetic fields. The magnetic fields in the visible corona are tied at both ends to the photosphere where the active convection continually rotates and shuffles the footpoints in a random pattern. The twisting and wrapping of flux tubes about each other produce magnetic neutral sheets in a state of dynamical nonequilibrium such that the current sheets become increasingly concentrated with the passage of time. Dissipation of the high current densities takes place regardless of the high electrical conductivity of the fluid. The convection on the feet of the lines of force at the surface of the Sun goes directly (within a matter of 10 to 20 hours) into heat in the corona. The rate of doing work seems adequate to supply the necessary 10 to the 7th power ergs/square cm. sec for the active corona.

Parker, E. N.↗

DOE OSTI2024

Elucidating the degradation mechanisms of Pt-free anode anion-exchange membrane fuel cells after durability testing

The development of anion-exchange membrane fuel cells (AEMFCs) has recently accelerated due to synergistic improvements yielding highly conductive membranes, stable ionomers, and enhanced alkaline electrocatalysts. However, cell durability, especially under realistic conditions, still poses a major challenge. Herein, we employ low-loadings of Pt-free Pd-based catalysts in the anode of AEMFCs and elucidate potential degradation mechanisms impacting long-term performance under conditions analogous to the real-world (high current density, H 2 –air (albeit CO 2 -free), and intermittent operation). Our high-performing AEMFCs achieve impressive performance with power densities approaching 1 W cm —2 and current densities up to 3.5 A cm —2 . Over a 200 h period of continuous operation in H 2 –air at a current density of 600 mA cm —2 , our model Pd/C–CeO 2 anode cell exhibits record stability (~30 μV h —1 degradation) compared to the literature and up to 6× better stability than our Pd/C and commercial Pt/C anode cells. Following an 8 h shutdown, the Pd/C–CeO 2 anode cell was restarted and continued for an additional 300 h with a higher degradation rate of ~600 μV h —1 . Thorough in situ evaluations and post-stability analyses provide insights into potential degradation mechanisms to be expected during extended operation under more realistic conditions and provide mitigation strategies to enable the widespread development of highly durable AEMFCs.

08 HYDROGEN↗

NASA NTRS1977

A hollow cathode hydrogen ion source

High current density ion sources have been used to heat plasmas in controlled thermonuclear reaction experiments. High beam currents imply relatively high emission currents from cathodes which have generally taken the form of tungsten filaments. This paper describes a hydrogen ion source which was primarily developed to assess the emission current capability and design requirements for hollow cathodes for application in neutral injection devices. The hydrogen source produced ions by electron bombardment via a single hollow cathode. Source design followed mercury ion thruster technology, using a weak magnetic field to enhance ionization efficiency. A 1.3-cm-diam hollow cathode using a low work function material dispenser performed satisfactorily over a discharge current range of 10-90 A. Cylindrical probe measurements taken without ion extraction indicate maximum ion number densities on the order of 10 trillion/cu cm. Discharge durations ranged from 30 sec to continuous operation. Tests with beam extraction at 2.5 keV and 30 A discharge current yield average ion beam current densities of 0.1 A/sq cm over a 5-cm extraction diameter. Results of this study can be used to supply the baseline information needed to scale hollow cathodes for operation at discharge currents of hundreds of amperes using distributed cathodes.

Sovey, J. S.↗

DOE OSTI2022

Membrane‐electrode assembly design parameters for optimal CO 2 reduction

Commercial-scale generation of carbon-containing chemicals and fuels by means of electrochemical CO 2 reduction (CO 2 R) requires electrolyzers operating at high current densities and product selectivities. Membrane-electrode assemblies (MEAs) have been shown to be suitable for this purpose. In such devices, the cathode catalyst layer controls both the rate of CO 2 R and the distribution of products. In this study, we investigate how the ionomer-to-catalyst ratio (I:Cat), catalyst loading, and catalyst-layer thickness influence the performance of a cathode catalyst layer containing Ag nanoparticles supported on carbon. In this paper, we explore how these parameters affect the cell performance and establish the role of the exchange solution (water vs. CsHCO 3 ) behind the anode catalyst layer in cell performance. We show that a high total current density is best achieved using an I:Cat ratio of 3 at a Ag loading of 0.01–0.1 mg Ag /cm 2 and with a 1.0 M solution of CsHCO 3 circulated behind the anode catalyst layer. For these conditions, the optimal CO partial current density depends on the voltage applied to the MEA. The work also reveals that the performance of the cathode catalyst layer is limited by a combination of the electrochemically active surface area and the degree to which mass transfer of CO 2 to the surface of the Ag nanoparticles and the transport of OH – anions away from it limit the overall catalyst activity. Hydration of the ionomer in the cathode catalyst layer is found not to be an issue when using an exchange solution. The insights gained allowed for a Ag CO 2 R MEA that operates between 200 mA/cm 2 and 1 A/cm 2 with CO faradaic efficiencies of 78–91%, and the findings and understanding gained herein should be applicable to a broad range of CO 2 R MEA-based devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Electrolyte design for Li metal-free Li batteries

Li metal, with the lowest thermodynamically achievable negative electrochemical potential and the highest specific capacity (3860 mAh g -1 ), is the ultimate anode choice for Li batteries. However, the highest reported Li plating/stripping Coulombic efficiency (CE) of 99.5% after extensive efforts is still too low for the Li metal-free (all the Li metal in cycling comes from cathode, without anode pre-lithiation) Li metal batteries. The low CE is attributed to both non-uniform Li plating/stripping on the lithiophobic Cu current collector and Li dendrite growth through lithiophilic organic–inorganic solid electrolyte interphase (SEI) formed in carbonate electrolytes. Here, we use a lithiophilic Bismuth graphite blend (Bi–Gr) substrate to replace lithiophobic Cu current collector to seed a uniform Li nucleation, and form a lithiophobic LiF-rich SEI rather than lithiophilic organic-rich SEI to suppress Li dendrite growth. Molecular dynamics simulations reveal the preferential reduction of anions in 2.0 M LiPF 6 in tetrahydrofuran/2-methyl tetrahydrofuran (2.0 M LiPF 6 –mixTHF) electrolyte to generate LiF-rich SEI on plated Li. Bi–Gr substrate and 2.0 M LiPF 6 –mixTHF electrolyte enable the Li anodes to achieve a record high CE of 99.83% at a high capacity of 1.0 mAh cm -2 and current of 0.5 mA cm -2 . The Bi particles serve as dispersed nucleation centers that promote uniform Li deposition with strong adhesion to the substrate to avoid dead Li, while the lithiophobic LiF-rich SEI promotes lateral Li growth and suppresses the vertical Li dendrite growth even at a high current density of 3.0 mA cm -2 and high areal capacities of 3.0 mAh cm -2 . The regulation of Li nucleation and growth enables the Li metal-free LiFePO 4 full cells to achieve 100 cycles at a practical areal capacity of >2.0 mAh cm -2 . This article highlights the benefits of simultaneous substrate design to improve Li nucleation and electrolyte design to promote lithiophobic SEI growth, enabling a promising and practical route Li metal-free Li metal batteries.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Lithium-conducting covalent-organic-frameworks as artificial solid-electrolyte-interphase on silicon anode for high performance lithium ion batteries

Not provided.

Chemistry↗

DOE OSTI2025

Quaternary Cu 2 TSiS 4 (T = Fe, Mn) Anodes for Li-Ion Batteries

Developing high-capacity and fast-charging anode materials is critical for achieving high-performance Li-ion batteries (LIBs). Herein, polycrystalline quaternary transition metal silicon sulfides, Cu 2 TSiS 4 (T = Fe, Mn), were synthesized using a solid-state method and investigated as anode materials in LIBs. Cu 2 FeSiS 4 retains a reversible capacity of 670 mAh g –1 at 200 mA g –1 for 400 cycles, while Cu 2 MnSiS 4 suffers from a fast capacity loss in the initial 50 cycles. More importantly, Cu 2 FeSiS 4 can maintain a reversible capacity of 379 mAh g –1 after 700 cycles at a high current density of 2 A g –1 , demonstrating high cyclic stability and fast-charging capacity. To further understand the structure degradation and phase transformation, we investigated the postcycling electrodes using multiple techniques, including the scanning electron microscope with energy-dispersive X-ray spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy techniques. The results indicated that Cu 2 FeSiS 4 undergoes reversible phase transitions with Li 2 S as a major product component. To further assess the performance for practical applications, Cu 2 FeSiS 4 was coupled with LiFePO 4 to make LiFePO 4 ||Cu 2 FeSiS 4 full cells, which delivered superior electrochemical performance. These results demonstrate great promise for using quaternary transition metal silicon sulfides as anodes to achieve low-cost and sustainable LIBs.

25 ENERGY STORAGE↗

DOE OSTI2025

Editors’ Choice—Molten Salt Electrolysis in Chloride Melts for Energy-Efficient Iron Metal Production

This study explores chloride molten salt electrolysis (CMSE) as a promising route for energy-efficient iron metal (Fe) production. Moderate temperature (500 °C) LiCl-KCl molten salts offer excellent thermodynamic stability, high ionic conductivity and diffusivity, and high solubility for FeCl 3 , thereby enabling efficient Fe metal extraction at high electrowinning rates. Here, we demonstrate the two essential steps for converting taconite ore into Fe metal. First, Fe 2 O 3 from taconite pellets was selectively leached in HCl yielding a high-purity FeCl 3 aqueous solution, while the gangue components settled at the bottom. Then, anhydrous FeCl 3 was electrolyzed in a LiCl-KCl eutectic molten salt at 500 °C at high current density (1 A cm −2 ) and at high Coulombic efficiency (>85%). Analysis of the electrowon Fe deposits revealed dendritic structures with purity of >99 wt%, which could be further improved to nearly 100 wt% through arc re-melting. CMSE offers low specific energy consumption (3.7 kWhr kg −1 ), competitive with H 2 -DRI and other electrolytic approaches being pursued globally. Our findings underscore the potential of CMSE as an energy-efficient route for electrosynthesis of Fe metal.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Magnesium‐Mediated Electrochemical Synthesis of Ammonia

Metal-mediated electrochemical synthesis of ammonia (NH3) is a promising method to activate N2 at room temperature. While a Li-mediated approach has been optimized to produce NH3 at high current density and selectivity, Li's scarcity and its highly negative plating potential limit scalability and energy efficiency. Alternative mediators have been proposed, but only Ca has shown some promise, achieving ≈50% Faradaic efficiency (FE), though requiring voltages beyond -3 V. Here, we report a Mg-mediated nitrogen reduction reaction (Mg-NRR), where N2 is activated on Mg to form Mg3N2, followed by protolysis to release NH3 and regenerate Mg. A notable NH3 FE of 25.28 ± 3.80% is achieved at a current density of -45 mA cm-2, corresponding to an NH3 partial current density of -11.30 ± 1.77 mA cm-2 under 6 bar N2. Isotope-labeled experiments confirm that NH3 originates from N2, with similar FE (25.15 ± 1.01%). Importantly, NH3 production is demonstrated at a total cell potential as low as -3 V. This Li-free Mg-NRR system offers key advantages, including lower energy input and use of earth-abundant materials, making it a scalable route for sustainable NH3 synthesis.

Goyal, Ishita↗

NASA NTRS1993

A High Performance H2-Cl2 Fuel Cell for Space Power Applications

NASA has numerous airborne/spaceborne applications for which high power and energy density power sources are needed. The proton exchange membrane fuel cell (PEMFC) is an attractive candidate for such a power source. PEMFC's offer many advantages for airborne/spaceborne applications. They have high power and energy densities, convert fuel to electrical power with high efficiency at both part and full load, and can rapidly startup and shutdown. In addition, PEMFC's are lightweight and operate silently. A significant impediment to the attainment of very high power and energy densities by PEMFC's is their current exclusive reliance on oxygen as the oxidant. Conventional PEMFC's oxidize hydrogen at the anode and reduce oxygen at the cathode. The electrode kinetics of oxygen reduction are known to be highly irreversible, incurring large overpotential losses. In addition, the modest open circuit potential of 1.2V for the H2-O2 fuel cell is unattainable due to mixed potential effects at the oxygen electrode. Because of the high overpotential losses, cells using H2 and O2 are capable of achieving high current densities only at very low cell voltages, greatly curtailing their power output. Based on experimental work on chlorine reduction in a gas diffusion electrode, we believe significant increases in both the energy and power densities of PEMFC systems can be achieved by employing chlorine as an alternative oxidant.

Anderson, Everett B.↗

NASA NTRS1977

A hollow cathode hydrogen ion source

Sovey, J. S.↗

NASA NTRSDate not supplied

Electrifying Aircraft Propulsion: Thermal Issues of Megawatt Scale Power Dense Electric Machines and Material Solutions

Aircraft are the last major mode of transportation to undergo electrification for many reasons, where the underlying reason is the sensitivity of aircraft performance to mass. This sensitivity demands that efficient, megawatt (MW)-scale high specific power density powertrains be developed to impact regional, single aisle and larger aircraft that account for the majority of fuel burn in commercial aviation. Developing MW-scale high specific power electric powertrains (machines, cables/busbars and power electronics) remains a significant challenge. While advanced power semiconductors have enabled higher voltages, densities, and operational frequencies this also leads to passing high current through smaller volumes when considering electric machines and power electronics. This poses significant thermal challenges. This is particularly true for electric machines that strive to surpass 13 kW/kg, which studies have shown to be desirable for electric aircraft propulsion. The necessity of handling high current densities to achieve MW power levels dictates that greater than 10kW of waste heat will be generated. Moreover, most of the heat is generated in the stator winding which is a mixture of electrical conductor (copper or aluminum), potting material, magnet wire (electrical) insulation and high voltage electrical insulation. Although the electrical conductor is a fantastic thermal conductor, it is also the source of the heat (carrying the electrical current) and is thermally isolated by the other materials. Simply letting the machine run at increased temperatures is an attractive idea, however the reality is that most of the suitable electric insulations and potting material candidates are not likely to satisfactorily operate at higher temperatures with reasonable life expectancies. The likelihood of developing new polymers that can satisfy the necessary functions (mechanical and electrical), operate at higher temperatures with acceptable lifetime in the near term is small. This has led the researchers at the NASA Glenn Research Center to examine electrically insulative materials in high power destiny electric machines, their thermal environment, and what solutions are realistic from a materials point of view. This presentation will touch on both the thermal challenges of electric machines and NASA Glenn’s research into material solutions.

Electric Aircraft Propulsion↗

NASA NTRS1991

Performance of NbN superconductive tunnel junctions as SIS mixers at 205 GHz

Small area (less than 1 sq micron), high-current-density NbN/MgO/NbN tunnel junctions with I-V characteristics suitable for high-frequency mixers have been fabricated. Mesa-geometry junctions with an area of about 1 sq micron and critical current density of 5-10 kA/sq cm are integrated with superconducting microstrip lines designed to resonate out the junction capacitance. A study was made of the mixer gain and noise performance near 205 GHz as a function of the inductance provided by the microstrip line. This has confirmed, at a high millimeter-wave frequency, values of junction capacitance of 85 fF/sq micron and recently measured values of a magnetic penetration depth of 380 nm. Mixer noise temperatures as low as 134 K at 1.5 K have been obtained for properly tuned junctions. A significant improvement in mixer performance on cooling from 4.2 K to 1.5 K was observed. Edge-geometry junctions with an area of 0.3 sq microns and critical current density of 18-25 kA/sq cm have also been fabricated. These junctions give a mixer noise temperature of 145 K at 4.2 K without the use of integrated tuning elements. These are the best results ever achieved for NbN-based SIS mixers.

Mcgrath, W. R.↗

DOE OSTI2022

Covalent Organic Framework as an Efficient Protection Layer for a Stable Lithium‐Metal Anode

Abstract Lithium (Li) metal shows great potential for achieving high‐energy‐density rechargeable batteries. However, the practical applications of Li‐metal batteries are still challenged by the formation of Li dendrites and unstable solid‐electrolyte interphase (SEI) on metallic Li. Herein, a thin covalent organic framework layer is in situ fabricated on Li (COF‐Li) to suppress Li dendrite growth and mitigate the side reaction on the Li anode. The COF has a periodic and uniform porosity, allowing for selectively sieving Li ions and guiding a uniform Li deposition. As a result, the COF‐Li exhibits a non‐dendrite morphology during repeated Li plating/stripping and demonstrates a remarkable cycle life over 13 200 h with an extremely low overpotential of only 16 mV at a high current density of 10 mA cm −2 and a high areal capacity of 10 mAh cm −2 .

He, Jiarui↗

DOE OSTI2022

Covalent Organic Framework as an Efficient Protection Layer for a Stable Lithium-Metal Anode

We report Lithium (Li) metal shows great potential for achieving high-energy-density rechargeable batteries. However, the practical applications of Li-metal batteries are still challenged by the formation of Li dendrites and unstable solid-electrolyte interphase (SEI) on metallic Li. Herein, a thin covalent organic framework layer is in situ fabricated on Li (COF-Li) to suppress Li dendrite growth and mitigate the side reaction on the Li anode. The COF has a periodic and uniform porosity, allowing for selectively sieving Li ions and guiding a uniform Li deposition. As a result, the COF-Li exhibits a non-dendrite morphology during repeated Li plating/stripping and demonstrates a remarkable cycle life over 13 200 h with an extremely low overpotential of only 16 mV at a high current density of 10 mA cm -2 and a high areal capacity of 10 mAh cm -2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗