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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Ni Anchored to Hydrogen-Substituted Graphdiyne for Lithium Sulfide Cathodes in Lithium–Sulfur Batteries

Lithium–sulfur (Li–S) batteries are promising candidates for next-generation energy storage systems due to their high theoretical energy density and the low cost of sulfur. However, slow conversion kinetics between the insulating S and lithium sulfide (Li 2 S) remains as a technical challenge. In this work, we report a catalyst featuring nickel (Ni) single atoms and clusters anchored to a porous hydrogen-substituted graphdiyne support (termed Ni@HGDY), which is incorporated in Li 2 S cathodes. The rapidly synthesized catalyst was found to enhance ionic and electronic conductivity, decrease the reaction overpotential, and promote more complete conversion between Li 2 S and sulfur. The addition of Ni@HGDY to commercial Li 2 S powder enabled a capacity of over 516 mAh g Li 2 S –1 at 1 C for over 125 cycles, whereas the control Li 2 S cathode managed to maintain just over 200 mAh g Li 2 S –1 . In conclusion, these findings highlight the efficacy of Ni as a metal catalyst and demonstrate the promise of HGDY in energy storage devices.

25 ENERGY STORAGE↗
DOE OSTI2015

Electrochemically influenced cation inter-diffusion and Co 3 O 4 formation on La 0.6 Sr 0.4 CoO 3 infiltrated into SOFC cathodes

Nanosized LSC electrocatalyst was infiltrated into a porous scaffold cathode composed of Sm 2 O 3 -doped CeO 2 (SDC) and La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ (LSCF) in a commercial button solid oxide fuel cell (SOFC). To understand the stability of cathodes infiltrated with LSC, the infiltrated composite cells were subjected to both electrochemical operating and thermal aging states at 750 °C for 1500 h. Nanostructure and local chemistry evolution of La 0.6 Sr 0.4 CoO 3 (LSC) infiltrated cathodes upon operation and aging were investigated by transmission electron microscopy. After operation, the LSC remained a cubic perovskite, and the crystal grains exhibit comparable size to as-infiltrated LSC grains. Inter-diffusion of Fe from the LSCF to a Fe-incorporated LSC layer developed on the LSCF backbone. However, only sharp interfaces were observed between LSC and SDC backbone in the as-infiltrated cathode and such interfaces remain after operation. The infiltrated LSC on the SDC backbone also retains granular particle morphology. Furthermore, newly grown Co 3 O 4 nanocrystals were found in the operated cathode. After thermal aging, on the other hand, cation inter-diffusion across the interfaces of the infiltrate particles and the cathode backbones is less than that from the operated cells. Lastly, the following hypothesis is proposed: Co 3 O 4 forms on LSC arising from local charge balancing between cobalt and oxygen vacancies.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2019

Core-Shell Heterostructures as Solid Oxide Fuel Cell Electrodes Quarterly Report

The goals of the project are to synthesize and deploy core-shell heterostructures as solid oxide fuel cell (SOFC) cathodes which exhibit high oxygen reduction rates at lower operating temperatures resulting in high performance at lower operating temperature and simultaneously exhibit longterm resistance to Cr-impurity attack induced performance degradation. An ancillary objective is to eliminate cumbersome, multiple infiltration steps in the cathode to achieve high performance. The expected outcomes are (1) a novel, environmentally benign, and inexpensive synthesis tool for synthesizing complex cathode powders, scalable to high volumes; (2) decrease in energy expenditure during synthesis of cathode powders; (3) up to a factor of 1.5 improvement in maximum power density of single cells at 700ºC; and (4) significant improvements in cell performance degradation rates down to 0.02%/1000 h.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2016

A Rechargeable Al/S Battery with an Ionic‐Liquid Electrolyte

Abstract Aluminum metal is a promising anode material for next generation rechargeable batteries owing to its abundance, potentially dendrite‐free deposition, and high capacity. The rechargeable aluminum/sulfur (Al/S) battery is of great interest owing to its high energy density (1340 Wh kg −1 ) and low cost. However, Al/S chemistry suffers poor reversibility owing to the difficulty of oxidizing AlS x . Herein, we demonstrate the first reversible Al/S battery in ionic‐liquid electrolyte with an activated carbon cloth/sulfur composite cathode. Electrochemical, spectroscopic, and microscopic results suggest that sulfur undergoes a solid‐state conversion reaction in the electrolyte. Kinetics analysis identifies that the slow solid‐state sulfur conversion reaction causes large voltage hysteresis and limits the energy efficiency of the system.

Gao, Tao↗
DOE OSTI2016

A Rechargeable Al/S Battery with an Ionic‐Liquid Electrolyte

Abstract Aluminum metal is a promising anode material for next generation rechargeable batteries owing to its abundance, potentially dendrite‐free deposition, and high capacity. The rechargeable aluminum/sulfur (Al/S) battery is of great interest owing to its high energy density (1340 Wh kg −1 ) and low cost. However, Al/S chemistry suffers poor reversibility owing to the difficulty of oxidizing AlS x . Herein, we demonstrate the first reversible Al/S battery in ionic‐liquid electrolyte with an activated carbon cloth/sulfur composite cathode. Electrochemical, spectroscopic, and microscopic results suggest that sulfur undergoes a solid‐state conversion reaction in the electrolyte. Kinetics analysis identifies that the slow solid‐state sulfur conversion reaction causes large voltage hysteresis and limits the energy efficiency of the system.

Gao, Tao↗
DOE OSTI2018

Effects of Nanoimprinted Structures on the Performance of Organic Solar Cells

The effect of nanoimprinted structures on the performance of organic bulk heterojunction solar cells was investigated. The nanostructures were formed over the active layer employing the soft lithographic technique. The measured incident photon-to-current efficiency revealed that the nanostructured morphology over the active layer can efficiently enhance both light harvesting and charge carrier collection due to improvement of the absorption of incident light and the buried nanostructured cathode, respectively. The devices prepared with the imprinted nanostructures exhibited significantly higher power conversion efficiencies as compared to those of the control cells.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Effective Electrochemical Charge Storage in the High-Lithium Compound Li8ZrO6

Li8ZrO6 is a pseudolamellar compound with high lithium content. Even though it is intrinsically a poor conductor and does not contain a transition metal with easily variable oxidation states, a new synthetic approach to preparing it in nanocomposite form with intimate contact to a conductive carbon by mechanical delamination enabled galvanostatic cycling of coin half-cells containing Li8ZrO6/C as the cathode and Li-metal as the anode at 221 mAh/g (which corresponds to extracting 2 Li per formula unit) over at least 140 cycles. With a higher capacity limit, a discharge capacity of 331 mAh/g (which corresponds to extracting 3 Li per formula unit) was maintained over 15–20 cycles. Ex-situ and operando X-ray diffraction (XRD) studies of galvanostatically cycled cells showed that at these levels of charge, delithiation follows a reversible, topotactic path with only small distortions around Zr atoms. During this process, crystalline grain sizes decrease continuously, shortening diffusion lengths within grains but increasing the number of grain boundaries and electrode/electrolyte interfaces. Charge storage in Li8ZrO6 appears to involve partial oxidation of oxygen atoms and production of small-polaron holes, as supported by XRD, X-ray photoelectron spectroscopy, and pair-distribution function studies and predicted by quantum mechanical calculations. At higher depths of charge, delithiation results in amorphization of the active electrode material. The charge storage mechanism in Li8ZrO6 is unusual among lithium-ion battery electrode materials and involves a combination of mechanisms that resemble intercalation and conversion reactions. With further refinement, Li8ZrO6/C based materials open up opportunities to develop new cathode materials for lithium-ion batteries that may improve on currently existing capacity barriers.

Li diffusion↗
DOE OSTI2019

Core-Shell Heterostructures as Solid Oxide Fuel Cell Electrodes Quarterly Report

The goals of the project are to synthesize and deploy core-shell heterostructures as solid oxide fuel cell (SOFC) cathodes which exhibit high oxygen reduction rates at lower operating temperatures resulting in high performance at lower operating temperature and simultaneously exhibit longterm resistance to Cr-impurity attack induced performance degradation. An ancillary objective is to eliminate cumbersome, multiple infiltration steps in the cathode to achieve high performance. The expected outcomes are (1) a novel, environmentally benign, and inexpensive synthesis tool for synthesizing complex cathode powders, scalable to high volumes; (2) decrease in energy expenditure during synthesis of cathode powders; (3) up to a factor of 1.5 improvement in maximum power density of single cells at 700ºC; and (4) significant improvements in cell performance degradation rates down to 0.02%/1000 h.

03 NATURAL GAS↗
DOE OSTI2022

A Comprehensive Understanding of the Aging Effects of Extreme Fast Charging on High Ni NMC Cathode

As the battery industry shifts toward high Ni content cathodes, such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 [NMC811], a complete understanding of the degradation mechanisms of NMC811 under extreme fast charging (XFC) (XFC, ≤10–15 min charging) conditions is needed. Such comprehensive understanding would identify the most critical materials gaps that need to be addressed for enabling XFC long-life cells for electric vehicles. This study maps out the key aging mechanisms for NMC811 cycled at different XFC conditions (between 1C and 9C) for up to 1000 cycles. To acquire a fundamental understanding of utilization and degradation, cells are evaluated using a range of electrochemical techniques, and multimodal and multiscale microscopy techniques to quantify chemical, structural, and crystallographic degradation as a function of cycling conditions for the NMC cathode. When comparing NMC811 to NMC532, it is observed that NMC811 has a greater subsurface crystallographic degradation and displays a similar magnitude of subparticle cracking. However, the NMC811 maintains superior performance despite those advanced degradations. Here, the superior cycle life performance is attributed to the NMC811 particles having radially oriented grains and improved transport properties. NMC811 shows between 4.6× and 3.15× reduction in capacity fade than NMC532 for charging rates between 4C (e.g., 15-min charging) and 6C (10-min charging).

25 ENERGY STORAGE↗
DOE OSTI2023

Influence of electronic transport on electrochemical performance of (Cu,Mn) 3 O 4 solid oxide fuel cell cathodes

Alkaline Earth free spinel oxides provide a potential benefit over Sr-doped perovskite-based materials commonly used as electrodes in high-temperature electrochemical energy conversion devices, e.g., solid oxide fuel cells (SOFCs). Sr-segregation is a known issue leading to performance degradation. In this study, Cu x Mn 3-x O 4 (x = 1, 1.2, and 1.5) porous electrodes were examined as SOFC cathodes using electrochemical impedance spectroscopy to investigate the oxygen reduction reaction (ORR) kinetics in relation to the material's intrinsic conductivity, the extrinsic electrode structure, and the cell test design. Similar to the electronic conducting (La,Sr)MnO 3 SOFC cathodes, the ORR kinetics of Cu x Mn 3-x O 4 spinel electrodes was governed by the oxygen adsorption and diffusion at the particle surface as well as the charge transfer at the triple phase boundaries. The overall electrode polarization resistance was highly dependent on contact density with the metallic current collector, active material particle connectivity, electrode thickness, and the intrinsic electronic materials conductivity. Here, we describe the importance of effective electronic charge transport parallel to the electrode surface in maximizing the electrochemically active electrode volume and enhancing electrode performance. We discuss an approach to optimize cell and electrode design with respect to active materials properties. This aspect is critical to ensure reliable evaluation of new materials, since laboratory-scale button-cells typically exhibit a high degree of electrode microstructure (e.g. porosity, thickness) and electrical contact density variation from sample to sample.

(Cu,Mn)3O4↗
DOE OSTI2019

Cathode porosity is a missing key parameter to optimize lithium-sulfur battery energy density

While high sulfur loading has been pursued as a key parameter to build realistic high-energy lithium-sulfur batteries, less attention has been paid to the cathode porosity, which is much higher in sulfur/carbon composite cathodes than in traditional lithium-ion battery electrodes. For high-energy lithium-sulfur batteries, a dense electrode with low porosity is desired to minimize electrolyte intake, parasitic weight, and cost. Here we report the profound impact on the discharge polarization, reversible capacity, and cell cycling life of lithium-sulfur batteries by decreasing cathode porosities from 70 to 40%. According to the developed mechanism-based analytical model, we demonstrate that sulfur utilization is limited by the solubility of lithium-polysulfides and further conversion from lithium-polysulfides to Li2S is limited by the electronically accessible surface area of the carbon matrix. Finally, we predict an optimized cathode porosity to maximize the cell level volumetric energy density without sacrificing the sulfur utilization.

25 ENERGY STORAGE↗
DOE OSTI2017

Directional preparation of cobalt oxide nanoflakes grown on cobalt nanowires as composite cathode for high-performance alkaline batteries

Graphical abstract: Self-supported hierarchical porous CoO@Co core/shell arrays are prepared by combined hydrothermal plus electrodeposition methods and exhibit good electrochemical performances with high capacity & stable cycling life. - Highlights: • Construct self-supported porous CoO@Co core/branch arrays. • Porous CoO@Co composite arrays show high capacity and good cycling life. • Hierarchical porous composite structure is favorable for fast ion/electron transfer. - Abstract: Synthesis of multicomponent core/branch arrays is important for development of advanced energy storage devices. Herein we fabricate porous CoO@Co core/branch arrays by successive hydrothermal + electrodeposition methods CoO nanoflakes branch is uniformly coated on the Co nanowire core forming composite core/branch arrays (CBAs). The CoO@Co CBAs possess combined properties of highly porous structure and strong mechanical stability. As cathode for alkaline batteries, the obtained CoO@Co CBAs exhibit good electrochemical performances with high a capacity of 91.5 mAh g{sup −1} at 1 A g{sup −1} and stable high-rate cycling life (73.5 mAh g{sup −1} after 12,000 cycles at 10 A g{sup −1}). The hierarchical core/branch architecture provides positive roles in the enhancement of electrochemical properties with fast electronic transportation path, and short diffusion channels of ions. Our finding offers a new way to construct high-performance cathode of alkaline batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Ni nanoparticles embedded into cross-linked NiO nanoflakes as enhanced cathode for alkaline batteries

Highlights: • Ni/NiO arrays prepared by hydrothermal synthesis and electrodeposition methods. • Ni/NiO nanoflake arrays show high capacity for alkaline batteries. • Introducing Ni to the NiO nanoflake is favorable for fast electron transfer. - Abstract: Construction of metal/metal oxide composite arrays is highly important for developing advanced electrochemical energy devices. In this work, we report a facile electrodeposition method to embed Ni network into hydrothermal NiO nanoflake arrays. Ni nanoparticles of 10–25 nm are intimately integrated with NiO nanoflakes of 20–30 nm forming cross-linked Ni/NiO composite arrays. The electrochemical potentials of Ni/NiO composite arrays are explored as cathode of alkaline batteries by means of galvanostatic charge/discharge tests and cyclic voltammograms (CV) in KOH solution. Compared with the unmodified NiO nanoflake arrays, the Ni/NiO composite arrays show much better electrochemical properties with higher capacity (100 mAh g{sup −1} vs. 75 mAh g{sup −1} at 2 A g{sup −1}), enhanced cycling life (capacity retention: 96% vs. 82%) after 3800 cycles and improved high-rate capability. The introduction of Ni nanoparticles not only improves the electrical conductivity, but also acts as anchors to fasten the active nanoflakes to achieve long-term cycles.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Embedding sulfur into N-doped carbon nanospheres as enhanced cathode for high-performance lithium-sulfur batteries

Graphical abstract: S has been successfully embedded into N-doped carbon nanospheres as enhanced cathode exhibiting good performance with high specific capacity and cycling stability. - Highlights: • Construct N-doped carbon nanospheres (N-CNSs) are host for sulfur. • N-CNSs/S cathode show high capacity and good cycles. • N doping is favorable for fast ion/electron transfer. - Abstract: Lithium-sulfur (Li-S) batteries are considered as one of the most efficient power candidates owing to high energy density about 7–10 times larger than the commercial cathode materials. However, its practical application is impeded by severe “shuttle effect” and low cycle stability. As a consequence, in this work, we report N-doped carbon nanospheres (N-CNSs) composited with S as cathode for Li-S batteries. The stacked carbon nanosphere structure can not only improve the conductivity of cathode, but also work as barriers to retard diffusion of intermediate polysulfide. Owing to the unique structure, the N-CNSs/S cathode exhibits superior electrochemical performances with high specific capacity (1228 mAh g{sup −1} at 0.1 C), and excellent rate capability as well as good cyclic life. Our smart designed strategy may promote the development of high performance Li-S batteries.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Revealing the role of redox reaction selectivity and mass transfer in current–voltage predictions for ensembles of photocatalysts

Photocatalysts are conceptually simple reaction units where nanoscale semiconductors integrated with catalysts drive a pair of redox reactions on illumination. However, the proximity of reaction sites performing cathodic and anodic reactions poses dire challenges to realize large light-to-fuel conversion efficiencies. In this study, a powerful, yet straightforward, equivalent-circuit detail-balance modeling framework is developed and applied to evaluate the performance of photocatalytic systems featuring multiple light absorbers. Specifically, low bandgap iridium-doped strontium titanate is modeled as a Z-scheme photocatalyst to achieve desirable hydrogen evolution and iron-based redox shuttle oxidation reactions. Our model has unique capabilities to simulate competing redox reactions and address mass-transfer limitations. In a significant departure from state-of-the-art circuit models, our study develops tools to perform load-line analyses by incorporating a net electrochemical load curve that includes both desired and competing redox reactions. Consequently, reaction selectivity is predicted from equivalent circuit models for photocatalytic and photoelectrochemical systems. Our investigation into ensembles comprised of multiple, semi-transparent light absorbers reveals their potential to outperform a single, optically thick light absorber, particularly when operated under mass-transfer-limited conditions. However, this outcome hinges on minimizing mass-transfer rates of select redox species to prevent undesired reactions of hydrogen oxidation and/or redox shuttle reduction. Our findings demonstrate that reaction selectivity can be achieved by tuning asymmetry in redox species mass-transfer even with perfectly symmetric electrocatalytic charge-transfer coefficients. The influences of various kinetic, mass-transfer, and thermodynamic parameters are explored to offer crucial insights for synthesis of the next-generation of photocatalysts and selective coatings, and reactor designs.

25 ENERGY STORAGE↗
DOE OSTI2016

Engineering Platinum Alloy Electrocatalysts in Nanoscale for PEMFC Application

Fuel cells are expected to be a key next-generation energy source used for vehicles and homes, offering high energy conversion efficiency and minimal pollutant emissions. However, due to large overpotentials on anode and cathode, the efficiency is still much lower than theoretically predicted. During the past decades, considerable efforts have been made to investigate synergy effect of platinum alloyed with base metals. But, engineering the alloy particles in nanoscale has been a challenge. Most important challenges in developing nanostructured materials are the abilities to control size, monodispersity, microcomposition, and even morphology or self-assembly capability, so called Nanomaterials-by-Design, which requires interdisciplinary collaborations among computational modeling, chemical synthesis, nanoscale characterization as well as manufacturing processing. Electrocatalysts, particularly fuel cell catalysts, are dramatically different from heterogeneous catalysts because the surface area in micropores cannot be electrochemically controlled on the same time scale as more transport accessible surfaces. Therefore, electrocatalytic architectures need minimal microporous surface area while maximizing surfaces accessible through mesopores or macropores, and to "pin" the most active, highest performance physicochemical state of the materials even when exposed to thermodynamic forces, which would otherwise drive restructuring, crystallization, or densification of the nanoscale materials. In this presentation, results of engineering nanoscale platinum alloy particles down to 2 ~ 4 nm will be discussed. Based on nature of alloyed base metals, various synthesis technologies have been studied and developed to achieve capabilities of controlling particle size and particle microcomposition, namely, core-shell synthesis, microemulsion technique, thermal decomposition process, surface organometallic chemical method, etc. The results show that by careful engineering the particle size and microcomposition in nanoscale, it is able to achieve superior electrocatalytic activities comparing with traditional preparative methods. Examples to be discussed are high surface area carbon supported Pt, PtM binary, and PtMN ternary alloys, their synthesis processes, characterizations and electrocatalytic activities towards molecular oxygen reduction.

Alloy↗
DOE OSTI2025

1,10-Phenanthroline-Iron Complex-Derived Fe-N-C Electrocatalysts: Enhanced Oxygen Reduction Activity and Stability Through Synthesis Tuning

The development of electrocatalysts composed of earth-abundant elements is essential for advancing the commercial application of Proton Exchange Membrane Fuel Cells (PEMFC). Among these, single-atom electrocatalysts, such as Fe-N-C, show great promise for the oxygen reduction reaction (ORR). This study aims to improve the ORR activity and stability of Fe-N-C electrocatalysts by fine-tuning the straightforward 1,10-phenanthroline-iron complexation synthesis method. Key parameters, including iron-to-phenanthroline ratio, carbon powder surface area, and pyrolysis temperature were systematically varied to evaluate their influence on the resulting electrocatalysts. The findings of this study revealed that the electrocatalysts synthesized with 1,10-phenanthroline (Phen) and high-surface-area Black Pearls (BP) possessed much better ORR activity than electrocatalysts prepared by using Vulcan carbon (lower surface area). Interestingly, electrocatalysts prepared with BP, but with a non-bidentate nitrogen-containing ligand molecule, such as imidazole, showed a much poorer activity, as the resulting material predominantly consisted of inactive structures, such as encapsulated iron nanoparticles and iron oxide, as evidenced by HR-TEM, EXAFS, and XRD. Therefore, the results suggest that only the synergistic combination of the bidentate ligand phenanthroline (Phen) and the high-surface-area carbon support (BP) favored the formation of ORR-active Fe-N-C single-atom species upon pyrolysis. The study also unveiled a significant enhancement in electrocatalyst stability during accelerated durability tests (and air storage) as the pyrolysis temperature was increased from 700 to 1300 °C, albeit at the expense of ORR activity, likely resulting from the generation of iron particles. Pyrolysis at 1050 °C yielded the electrocatalyst with the most favorable balance of activity and stability in rotating disk measurements, while maintaining moderate durability under PEM fuel cell operation. The insights obtained in this study may guide the development of more active efficient and durable electrocatalysts, synthesized via a simple method using earth-abundant elements, for application in PEMFC cathodes.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2017

Efficient solar-driven electrochemical CO 2 reduction to hydrocarbons and oxygenates

Solar to chemical energy conversion could provide an alternative to mankind's unsustainable use of fossil fuels. One promising approach is the electrochemical reduction of CO 2 into chemical products, in particular hydrocarbons and oxygenates which are formed by multi-electron transfer reactions. Here, a nanostructured Cu-Ag bimetallic cathode is utilized to selectively and efficiently facilitate these reactions. When operated in an electrolysis cell, the cathode provides a constant energetic efficiency for hydrocarbon and oxygenate production. As a result, when coupled to Si photovoltaic cells, solar conversion efficiencies of 3-4% to the target products are achieved for 0.35 to 1 Sun illumination. Use of a four-terminal III-V/Si tandem solar cell configuration yields a conversion efficiency to hydrocarbons and oxygenates exceeding 5% at 1 Sun illumination. Here, this study provides a clear framework for the future advancement of efficient solar-driven CO 2 reduction devices. In a process analogous to natural photosynthesis, solar-driven reduction of carbon dioxide to hydrocarbon and oxygenate products is demonstrated with an overall efficiency exceeding 5%.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗