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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 883 records · Page 49
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Dye-sensitized photoelectrochemical water oxidation through a buried junction

Water oxidation has long been a challenge in artificial photosynthetic devices that convert solar energy into fuels. Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) provide a modular approach for integrating light-harvesting molecules with water-oxidation catalysts on metal-oxide electrodes. Despite recent progress in improving the efficiency of these devices by introducing good molecular water-oxidation catalysts, WS-DSPECs have poor stability, owing to the oxidation of molecular components at very positive electrode potentials. Here we demonstrate that a solid-state dye-sensitized solar cell (ss-DSSC) can be used as a buried junction for stable photoelectrochemical water splitting. A thin protecting layer of TiO 2 grown by atomic layer deposition (ALD) stabilizes the operation of the photoanode in aqueous solution, although as a solar cell there is a performance loss due to increased series resistance after the coating. With an electrodeposited iridium oxide layer, a photocurrent density of 1.43 mA cm −2 was observed in 0.1 M pH 6.7 phosphate solution at 1.23 V versus reversible hydrogen electrode, with good stability over 1 h. We measured an incident photon-to-current efficiency of 22% at 540 nm and a Faradaic efficiency of 43% for oxygen evolution. While the potential profile of the catalyst layer suggested otherwise, we confirmed the formation of a buried junction in the as-prepared photoelectrode. The buried junction design of ss-DSSs adds to our understanding of semiconductor–electrocatalyst junction behaviors in the presence of a poor semiconducting material.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Design principles for self-forming interfaces enabling stable lithium-metal anodes

Significance It is possible to nearly double the energy density of existing lithium-ion batteries by using lithium metal anodes. However, it has been known for decades that the lithium dendrites and mossy lithium formed during charging (electrodeposition) limit the cycle life of the batteries. It is important to change the growth behavior of lithium metal, which is closely related to the properties of the solid–electrolyte interface (SEI) formed via spontaneous reactions between the lithium metal and the electrolyte. In this experimental-modeling integrated study, we reveal the design principles of the SEI that facilitates the dendrite-free and dense deposition of lithium and demonstrate one of the best cycling performances of lithium metal anode to date under practically relevant conditions.

25 ENERGY STORAGE↗
DOE OSTI2018

Chemically linked metal-matrix nanocomposites of boron nitride nanosheets and silver as thermal interface materials

Herein, novel hybrid nanocomposite thermal interface materials (TIMs) relying on the chemical linkage of silver, boron nitride nanosheets (BNNSs), and organic ligands are reported. These TIMs were prepared using a co-electrodeposition/chemisorption approach where the electrolytic reduction of silver ions into silver nano-/micro-crystals was coupled with the conjugation of ligand-coated nanosheets onto silver crystals. Furthermore, the influence of bond strength of silver/nanosheet links on the thermal, mechanical, and structural properties is investigated using a combination of techniques; including laser flash analysis, phase-sensitive transient thermoreflectance, nanoindentation, and electron microscopy. Internal nanostructure was found to be strongly dependent on the linker chemistry. While the chemical grafting of 4-cyano-benzoyl chloride (CBC) and 2-mercapto-5-benzimidazole carboxylic acid (MBCA) on BNNSs led to the uniform distribution of functionalized-nanosheets in the silver crystal matrix, the physical binding of 4-bromo-benzoyl chloride (BBC) linkers on nanosheets caused the aggregation and phase separation. The thermal conductivity was 236-258 W/m-K and 306-321 W/m-K for physically and chemically conjugated TIMs, respectively, while their hardness varied from 495 to 400 MPa and from 240 to 360 MPa, respectively. The corresponding ratio of thermal conductivity to hardness, which is a critical parameter controlling the performance of TIMs, was ultrahigh for the chemically conjugated TIMs: 1.3x10-6 m2/K-s for MBCA-BNNS and 8.5x10-7 m2/K-s for CBC-BNNS. We anticipate that these materials can satisfy some of the emerging thermal management needs arising from the improved performance and efficiency, miniaturization, and/or high throughput of electronic devices, energy storage devices, energy conversion systems, light-emitting diodes, and telecommunication components.

2-D nanomaterials↗
DOE OSTI2020

Development of Solar Cells with Trapezoidal Grid Fingers

In concentrator solar cells, traditional metallic contacts cover a substantial portion of the device area, resulting in reflected light that diminishes the amount of current collected. In this paper, we developed trapezoidal front grid fingers to decrease the optical shadowing and the resulting loss of the device short-circuit current. By using a negative photoresist, a thick metal layer can be deposited by metal evaporation. The formation of an organic and metallic reflective deposit under the negative sloped photoresist is observed, though. By removing this deposit, a similar short-circuit current to typical Ni/Au contacts deposited by electrodeposition is obtained. Even though the Ti/Al grid fingers have larger width, they have the same effective shadowing due to the trapezoidal shape. At high concentration, a higher efficiency is obtained as well due to a high fill factor and improved open circuit voltage.

14 SOLAR ENERGY↗
DOE OSTI2017

Application of Sol-Gel Method as a Protective Layer on a Specular Reflective Surface for Secondary Reflector in a Solar Receiver

Highly-specular reflective surfaces that can withstand elevated-temperatures are desirable for many applications including reflective heat shielding in solar receivers and secondary reflectors, which can be used between primary concentrators and heat collectors. A high-efficiency, high-temperature solar receiver design based on arrays of cavities needs a highly-specular reflective surface on its front section to help sunlight penetrate into the absorber tubes for effective flux spreading. Since this application is for high-temperature solar receivers, this surface needs to be durable and to maintain its optical properties through the usable life. Degradation mechanisms associated with elevated temperatures and thermal cycling, which include cracking, delamination, corrosion/oxidation, and environmental effects, could cause the optical properties of surfaces to degrade rapidly in these conditions. Protected mirror surfaces for these applications have been tested by depositing a thin layer of SiO2 on top of electrodeposited silver by means of the sol-gel method. To obtain an effective thin film structure, this sol-gel procedure has been investigated extensively by varying process parameters that affect film porosity and thickness. Endurance tests have been performed in a furnace at 150 degrees C for thousands of hours. This paper presents the sol-gel process for intermediate-temperature specular reflective coatings and provides the long-term reliability test results of sol-gel protected silver-coated surfaces.

14 SOLAR ENERGY↗
DOE OSTI2022

Longevity evaluation of SiC based alpha voltaic batteries with surface alpha sources

The alpha emitting actinide 241 Am is electrodeposited on the surface of the Pt electrode of in-house fabricated SiC Schottky diodes. With 17 nCi 241 Am directly coated on the top of a device, the 2-pi geometry yields a high energy (5.486 MeV) and a long-term irradiation accumulating to a high fluence (1.6 × 10 9 alpha particles’ infusion/month). The forward, reverse I/V, and dark current, are periodically measured to monitor key characteristics of device durability for any sign of degradation over time. The direct deposition of actinides on the surface of the device also enables the evaluation of radiation damage through alpha particles’ energy spectroscopic performance, which shows a clear spectrum degradation that can be reversed by optical excitation of the device prior to spectrum acquisition. As an analytical aide, the device performance is also simulated by Allpix 2 . Lastly, this study provides an insight into the durability of 4H-SiC as an energy converter option for alpha-voltaic batteries and the survivability in the other harsh environment found in nuclear fuel cycle, high energy physics, fission, fusion, and space exploration where rad-hard sensors are required.

Americium↗
DOE OSTI2016

TH-EF-207A-02: Imaging Pancreatic Î{sup 2}-Cell Function with 51/52Mn-PET

Purpose: To image β-cells noninvasively using radio-manganese PET and to develop efficient small cyclotron production of {sup 51}Mn (t1/2=46m, β{sup +}=97%) and {sup 52}Mn (t1/2=5.6d, β{sup +}=29%). Methods: {sup 51}Mn and {sup 52}Mn were produced by 16 MeV proton irradiation (GE PETtrace) of electrodeposited {sup 54}Fe on silver and Cr metal pressed into a silver disc, respectively. {sup 51}Mn was radiochemically isolated from target material by anion exchange chromatography and {sup 52}Mn was isolated by ethanolic anion exchange trap-and-release. A final injectable product of {sup 51}Mn{sup 2+} or {sup 52}Mn{sup 2+} was obtained in 0.01M pH 6.0 NaOAc. To assess pancreatic uptake, fasted ICR mice were administered and intravenous bolus or infusion of {sup 52}Mn{sup 2+}. Additionally, to demonstrate the correlation between β-cell function and {sup 52}Mn{sup 2+} pancreatic uptake, prior to tracer administration groups of ICR mice were administered glibenclamide (5mg/kg) and diazoxide (20 mg/kg) as an insulin release stimulator and blocker, respectively. To validate PET ROI quantification, ex vivo biodistribtution studies were conducted on each subject after the final imaging time-point. Results: Dynamic PET data using a left atrium ROI revealed that {sup 52}Mn{sup 2+} cleared from the blood with a 10 second half-life. Significant uptake was seen in the pancreas (approximately 20% ID/g, SUVmean= 5.5), liver, kidneys, intestine, heart, and thyroid. Pancreatic uptake was found to be highly sensitive to volatile anesthesia administration (p=0.0002), insulin release stimulation by glibenclamide (p=0.017), and by insulin release inhibition by diazoxide (p=0.046). Excellent agreement was found between in vivo PET ROI quantification and ex vivo biodistribution measurements. Conclusion: This work demonstrates the feasibility of using radiomanganese-PET for measuring functional β-cell mass in vivo. The decay characteristics and dosimetric properties of {sup 51}Mn are well suited for clinical PET, which will allow for rapid translation and application.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2017

Electroplating lithium transition metal oxides

Materials synthesis often provides opportunities for innovation. We demonstrate a general low-temperature (260°C) molten salt electrodeposition approach to directly electroplate the important lithium-ion (Li-ion) battery cathode materials LiCoO 2 , LiMn 2 O 4 , and Al-doped LiCoO 2 . The crystallinities and electrochemical capacities of the electroplated oxides are comparable to those of the powders synthesized at much higher temperatures (700° to 1000°C). In conclusion, this new growth method significantly broadens the scope of battery form factors and functionalities, enabling a variety of highly desirable battery properties, including high energy, high power, and unprecedented electrode flexibility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Designer interphases for the lithium-oxygen electrochemical cell

An electrochemical cell based on the reversible oxygen reduction reaction: 2Li+ + 2e- + O2 ↔ Li2O2, provides among the most energy dense platforms for portable electrical energy storage. Such Lithium-Oxygen (Li-O2) cells offer specific energies competitive with fossil fuels and are considered promising for electrified transportation. Multiple, fundamental challenges with the cathode, anode, and electrolyte have limited practical interest in Li-O2 cells because these problems lead to as many practical shortcomings, including poor rechargeability, high overpotentials, and specific energies well below theoretical expectations. We create and study in-situ formation of solid-electrolyte interphases (SEIs) based on bromide ionomers tethered to a Li anode that take advantage of three powerful processes for overcoming the most stubborn of these challenges. The ionomer SEIs are shown to protect the Li anode against parasitic reactions and also stabilize Li electrodeposition during cell recharge. Bromine species liberated during the anchoring reaction also function as redox mediators at the cathode, reducing the charge overpotential. Finally, the ionomer SEI forms a stable interphase with Li, which protects the metal in high Gutmann donor number liquid electrolytes. Such electrolytes have been reported to exhibit rare stability against nucleophilic attack by Li2O2 and other cathode reaction intermediates, but also react spontaneously with Li metal anodes. We conclude that rationally designed SEIs able to regulate transport of matter and ions at the electrolyte/anode interface provide a promising platform for addressing three major technical barriers to practical Li-O2 cells.

25 ENERGY STORAGE↗
DOE OSTI2021

Stabilized Nanocrystalline Alloys: The Intersection of Grain Boundary Segregation with Processing Science

Processing science for nanocrystalline metals has largely focused on far-from-equilibrium methods that can generate many grain boundaries with excess defect energy. Conversely, the science of stabilizing nanocrystalline alloys has largely focused on the lowering of that excess defect energy through grain boundary segregation, bringing nanocrystalline structures closer to equilibrium. With increasing technological adoption of stabilized nanocrystalline alloys, there is a substantial need for research at the intersection of these two fields. This review lays out the basic thermodynamic issues of the two subfields and surveys the literature on the most common processing methods, including severe plastic deformation, ball milling, physical vapor deposition, and electrodeposition. We provide an overview of studies that have examined grain boundary segregation through each of these methods and identify general themes. We conclude that there is substantial scope for more systematic work at the intersection of these fields to understand how nonequilibrium processing affects grain boundary segregation.

Materials Science↗
DOE OSTI2020

Imaging Cycle-Induced Damage of MnO 2 Microparticles

MnO 2 has been proposed as an electrode material in electrochemical energy storage devices. However, poor cycle life, especially in aqueous electrolytes, remains a detriment to commercialization. Prior studies have suggested a number of explanations for this capacity loss; however, experiments aimed at elucidating the details of the degradation process (es) are sparse. We describe here a microtube-membrane construct that allows for electrodeposition of monodisperse MnO 2 microparticles distributed across the membrane surface, and for subsequent electrochemical cycling of these MnO 2 particles. This allowed for a detailed analysis of the effect of cycling on the MnO 2 , by simply imaging the membrane surface before and after cycling. When an aqueous electrolyte was used, gross changes in particle shape, size and morphology were observed over the course of 500 cycles. Partial dissolution occurred as well. No such changes were observed when the MnO 2 particles were cycled (up to 500 times) in a propylene carbonate electrolyte solution.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Reducing Zinc Redistribution and Extending Cycle Life Via Electrochemical Synthesis of Zinc/Zinc Oxide Anodes in Rechargeable Alkaline Batteries

Redistribution of zinc over the electrode surface, also known as shape change, is a major problem and a cause of failure in alkaline zinc anode batteries. To mitigate this phenomenon, we propose a scalable approach based on an in situ formed, highly porous electrochemically synthesized ZnO matrix with uniformly electrodeposited zinc particles. This results in ∼70% improvement in cycle life performance at a rate of 10 mA cm −2 compared to control Zn anodes, which have not gone through the formation process. A quantitative electrolyte analysis revealed under-saturated zincate ion concentration in the electrochemically synthesized ZnO/Zn cells indicating reduced zincate movement. Post mortem analysis of the anodes indicated higher retention of both Zn and ZnO on the electrochemically synthesized ZnO anodes signifying reduced redistribution of active material. Image analysis of the cycled anodes revealed a narrower Zn particle size distribution (62−79 μ m) in contrast to a wider particle size distribution of 51–96 μ m observed in the control anodes. The formation approach results in electrochemically synthesized ZnO/Zn anodes providing a stable ZnO matrix in which Zn particles retain their localized distribution on cycling better than control electrodes conventionally made by pasting zinc particles together with a binder.

Kolhekar, Snehal (ORCID:0000000210321153)↗
DOE OSTI2021

An Electrochemically Activated Nanofilm for Sustainable Mg Anode with Fast Charge Transfer Kinetics

Highly reversible Mg plating/stripping is key for rechargeable Mg batteries and has typically been successfully demonstrated using transient electrochemical techniques such as cyclic voltammetry measurements. Furthermore, little effort has been invested in studying the stability of the electrode/electrolyte interface over an extended time. We report here the development of an in situ generated surface film for Mg anodes based on electrodeposited bismuth (E_Bi). This film improves the interfacial stability of Mg in contact with the electrolyte, particularly over an extended time, and possesses fast charge-transfer kinetics (<30 Ω∙cm 2 ) and low non-time-sensitive interfacial film resistance (ca. 5 Ω∙cm 2 ) for active Mg species.

25 ENERGY STORAGE↗
DOE OSTI2023

Electrochemical Deposition with Redox Replacement of Lanthanum with Uranium in Molten LiCl-KCl

Electrochemical recovery of dilute concentrations of actinides from spent nuclear fuel would reduce the longevity of storing high-level nuclear waste. Electrochemical deposition with redox replacement (EDRR) is used in a molten salt medium for the selective electrochemical recovery of uranium in the presence of excess concentrations of lanthanum. In each EDRR cycle, after a short electrodeposition pulse, the deposited lanthanum is spontaneously replaced by uranium at open circuit. After repeated cycles, uranium metal was obtained on a tungsten electrode immersed in LiCl-KCl melt that contained 1 wt.% lanthanum chloride – 0.15 wt.% uranium 4+ chloride. Here, scanning electron microscopy and energy dispersive X-ray spectroscopy analysis revealed uranium particles approximately 0.5 - 1 μm with well-defined rectangular shapes; and with 20 – 60 times more uranium recovered on the surface of the electrode than lanthanum.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Stable Lithium Plating in “Lithium Metal-Free” Solid-State Batteries Enabled by Seeded Lithium Nucleation

In the “Li 0 -free” architecture, cells are manufactured with a bare anode current collector and the Li metal anode is plated in situ during the first charging step. While this architecture has many attractive qualities from manufacturing and energy density perspectives, stable Li plating in solid-state “Li 0 -free” cells can be challenging. It is generally accepted that the Li overpotential affects Li homogeneity in “Li 0 -free” cells. We demonstrate that the nucleation overpotential for Li plating in solid-state “Li 0 -free” cells using commercial current collectors can be eliminated by introducing metal clusters that guide Li nucleation. Au is used as model alloying metal cluster. Here, we demonstrate stable Li plating with thickness 16.5 μ m (3.3 mAh cm −2 ) in oxide solid-state electrolyte “Li 0 -free” cells enabled by Au metal clusters. It is shown that 97% of the in situ plated Li can be reversibly stripped at 60 °C and 2.5 MPa. Conversely, Au interlayers which are flat and continuous instead of clustered in morphology consistently showed short-circuiting during in situ Li plating, limiting Li electrodeposition to <0.1 mAh cm −2 . These results can help guide future studies of Li nucleation and growth at solid/solid interfaces, as well as offer alternative manufacturing pathways for “Li 0 -free” solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2023

Evaluation of Lithium Metal Anode Volumetric Expansion through Laser Plasma Focused Ion Beam Cross-Sectional Imaging

Lithium metal is an ideal anode for high energy density batteries, however the implementation of lithium metal anodes remains challenging. Beyond the development of highly efficient electrolytes, degradation processes restrict cycle life and reduce practical energy density. Herein lithium volumetric expansion and degradation pathways are studied in half cells through coupling electrochemical analysis with cross-sectional imaging of the intact electrode stack using a cryogenic laser plasma focused ion beam and scanning electron microscope. Here, we find that the volumetric capacity is compromised as early as the first cycle, at best reaching values only half the theoretical capacity (1033 vs 2045 mAh cm -3 ). By the 101st electrodeposition, the practical volumetric capacity decreases to values ranging from 143 to 343 mAh cm -3 .

25 ENERGY STORAGE↗