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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 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Highly Ordered Eutectic Mesostructures via Template‐Directed Solidification within Thermally Engineered Templates

Template-directed self-assembly of solidifying eutectics results in emergence of unique microstructures due to diffusion constraints and thermal gradients imposed by the template. Here, the importance of selecting the template material based on its conductivity to control heat transfer between the template and the solidifying eutectic, and thus the thermal gradients near the solidification front, is demonstrated. Simulations elucidate the relationship between the thermal properties of the eutectic and template and the resultant microstructure. The overarching finding is that templates with low thermal conductivities are generally advantageous for forming highly organized microstructures. When electrochemically porosified silicon pillars (thermal conductivity < 0.3 Wm −1 K −1 ) are used as the template into which an AgCl-KCl eutectic is solidified, 99% of the unit cells in the solidified structure exhibit the same pattern. In contrast, when higher thermal conductivity crystalline silicon pillars (≈100 Wm −1 K −1 ) are utilized, the expected pattern is only present in 50% of the unit cells. The thermally engineered template results in mesostructures with tunable optical properties and reflectances nearly identical to the simulated reflectances of perfect structures, indicating highly ordered patterns are formed over large areas. This work highlights the importance of controlling heat flows in template-directed self-assembly of eutectics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Intensified Catalytic Conversion of CO2 into High Value Chemicals

The utilization of CO2 produced from power generation plants as a feedstock for creating new valuable products offers a strategy to reduce GHG emissions, offset carbon capture costs, and facilitate the rebalancing of the carbon cycle. After considering the thermodynamic requirement of potential products from CO2 utilization and their market size, formic acid is a desirable target that offers widespread utility in industrial chemical production and chemical energy storage as a liquid fuel. To effectively utilize CO2 from power generation plants, UK proposes an enhanced bimetallic oxide carbon utilization process (EBOCU) that enables electrochemical CO2 conversion to formic acid. The UK intensified electrocatalytic process combines three main components: 1) a novel bimetallic oxide electrocatalyst; 2) a stable electrochemical reactor using robust electrodes; and 3) a pressurized electrochemical reactor. The output from this project showed the economic viability of producing high-value formic acid from CO2 to both offset the cost associated with post-combustion CCS and reduce GHG emissions. This project developed and screened a series engineered catalysts to selectively reduce CO2 directly to formic acid. The best performing catalyst based on formic acid production, stability, and Faradaic efficiency, was immobilized on carbon electrodes, and tested inside a flow through reactor. After lab-scale testing was completed, the experimental data was used to perform a Life-Cycle Analysis (LCA) and conduct an Initial Technical and Economic Feasibility Study. The LCA showed a pathway to a net negative CO2 utilization process with the incorporation of renewable energy, while the TEA showed the potential to produce formic acid below the current commercial price. The UK EBOCU process was successfully demonstrated at the TRL3 level and has a clear pathway to further development and contribution to the nation’s ambitious decarbonization goals.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2022

Resolving Charge Distribution for Compositionally Heterogeneous Battery Cathode Materials

The isostructural nature of Li-layered cathodes allows for accommodating multiple transition metals (TMs). However, little is known about how the local TM stoichiometry influences the charging behavior of battery particles thus impacting battery performance. In this work, we develop heterogeneous compositional distributions in polycrystalline LiNi 1–x–y Mn x Co y O 2 (NMC) particles to investigate the interplay between local stoichiometry and charge distribution. These NMC particles exhibit a broad, continuous distribution of local Ni/Mn/Co stoichiometry, which does not compromise the global layeredness. The local Mn and Ni concentrations in individual NMC particles are positively and negatively correlated with the electrochemically induced Ni oxidation, respectively, whereas the Co concentration does not impose a clear effect on the Ni oxidation. The resulting material delivers excellent reversible capacity, rate capability, and cycle life at high operating voltages. Engineering Ni/Mn/Co distribution in NMC particles may provide a path toward controlling the charge distribution and thus chemomechanical properties of polycrystalline battery particles.

25 ENERGY STORAGE↗
DOE OSTI2022

Oxygen-Plasma-Induced Hetero-Interface NiFe2O4/NiMoO4 Catalyst for Enhanced Electrochemical Oxygen Evolution

The electrolysis of water to produce hydrogen is an effective method for solving the rapid consumption of fossil fuel resources and the problem of global warming. The key to its success is to design an oxygen evolution reaction (OER) electrocatalyst with efficient conversion and reliable stability. Interface engineering is one of the most effective approaches for adjusting local electronic configurations. Adding other metal elements is also an effective way to enrich active sites and improve catalytic activity. Herein, high-valence iron in a heterogeneous interface of NiFe 2 O 4 /NiMoO 4 composite was obtained through oxygen plasma to achieve excellent electrocatalytic activity and stability. In particular, 270 mV of overpotential is required to reach a current density of 50 mA cm -2 , and the overpotential required to reach 500 mA cm -2 is only 309 mV. The electron transfer effect for high-valence iron was determined by X-ray photoelectron spectroscopy (XPS). The fast and irreversible reconstruction and the true active species in the catalytic process were identified by in situ Raman, ex situ XPS, and ex situ transmission electron microscopy (TEM) measurements. This work provides a feasible design guideline to modify electronic structures, promote a metal to an active oxidation state, and thus develop an electrocatalyst with enhanced OER performance.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Corrosion Engineering of Part‐Per‐Million Single Atom Pt 1 /Ni(OH) 2 Electrocatalyst for PET Upcycling at Ampere‐Level Current Density

The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While conventional recycling strategies often lead to plastic down-cycling, the electrochemical strategy of recovering valuable monomers enables an ideal, circular plastic economy. Here a corrosion synthesized single atom Pt 1 /Ni(OH) 2 electrocatalyst with part-per-million noble Pt loading for highly efficient and selective upcycling of polyethylene terephthalate (PET) into valuable chemicals (potassium diformate and terephthalic acid) and green hydrogen is reported. Electro-oxidation of PET hydrolysate, ethylene glycol (EG), to formate is processed with high Faraday efficiency (FE) and selectivity (>90%) at the current density close to 1000 mA cm −2 (1.444 V vs RHE). The in situ spectroscopy and density functional theory calculations provide insights into the mechanism and the understanding of the high efficiency. Remarkably, the electro-oxidation of EG at the ampere-level current density is also successfully illustrated by using a membrane-electrode assembly with high FEs to formate integrated with hydrogen production for 500 h of continuous operation. In conclusion, this process allows valuable chemical production at high space-time yield and is highly profitable (588–700 $\$$ ton −1 PET), showing an industrial perspective on single-atom catalysis of electrochemical plastic upcycling.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Defect Engineering of WO 3 by Rapid Flame Reduction for Efficient Photoelectrochemical Conversion of Methane into Liquid Oxygenates

Photoelectrochemical (PEC) conversion is a promising way to use methane (CH 4 ) as a chemical building block without harsh conditions. However, the PEC conversion of CH 4 to value-added chemicals remains challenging due to the thermodynamically favorable overoxidation of CH 4 . Here, we report WO 3 nanotube (NT) photoelectrocatalysts for PEC CH 4 conversion with high liquid product selectivity through defect engineering. By tuning the flame reduction treatment, we carefully controlled the oxygen vacancies of WO 3 NTs. The optimally reduced WO 3 NTs suppressed overoxidation of CH4 showing a high total C1 liquid selectivity of 69.4% and a production rate of 0.174 μmol cm –2 h –1 . Scanning electrochemical microscopy revealed that oxygen vacancies can restrain the production of hydroxyl radicals, which, in excess, could further oxidize C1 intermediates to CO 2 . Additionally, band diagram analysis and computational studies elucidated that oxygen vacancies thermodynamically suppress overoxidation. In conclusion, this work introduces a strategy for understanding and controlling the selectivity of photoelectrocatalysts for direct conversion of CH 4 to liquids.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Unraveling the core of fuel cell performance: engineering the ionomer/catalyst interface

The biggest obstacle to the widespread implementation of polymer electrolyte membrane fuel cells (PEMFCs) is their cost, primarily due to the use of platinum catalysts. The high intrinsic catalyst activity exhibited on a rotating disk electrode (RDE) is rarely realized in a membrane electrode assembly (MEA), which is a long-standing challenge for PEMFCs and a cause of low catalyst utilization. To translate the high RDE performance of a catalyst into a MEA, the design of an ideal ionomer/catalyst interface is proposed: a thin, conformal ionomer film covers the maximum surface of a Pt nanoparticle and thus simultaneously maximizes catalyst utilization, (i.e., high mass activity and electrochemically active surface area) and O 2 diffusion rate (i.e., high current density performance) without compromising proton conduction. Building such an interface is a long-standing challenge due to the lack of interaction between the ionomer and catalyst particles, resulting in large ionomer agglomerates and inhomogeneous ionomer coverage over the catalyst nanoparticle, with consequent poor fuel cell performance. In this work, this ionomer/catalyst interface has been engineered, utilizing the electrostatic attraction between positively charged catalyst and negatively charged ionomer particles in a catalyst ink and preserved in a solid catalyst layer. As a result, this interface leads to previously unachieved proton exchange membrane fuel cell performance in terms of both catalyst utilization (75% vs. 45%) and peak/rated power density (i.e., 1.430/0.930 W cm -2 , H 2 /air, cathode Pt loading: 0.1 mgPt cm -2 ) for pure Pt catalysts, even better than those of Pt alloy catalysts. This work demonstrates the formation of an interface in the liquid phase (using ultra-small-angle X-ray scattering in combination with cryo-TEM, isothermal–titration–calorimetry) and the preservation of the interface in the solid catalyst layer (using TEM) and estimates the effective coverage and thickness of the ionomer film (using limiting current density, RDE and fuel cell performance).

25 ENERGY STORAGE↗
DOE OSTI2020

Degradation of solid oxide electrolysis cells: Phenomena, mechanisms, and emerging mitigation strategies—A review

Solid oxide electrolysis cell (SOEC) is a promising electrochemical device with high efficiency for energy storage and conversion. However, the degradation of SOEC is a significant barrier to commercial viability. In this review article, the typical degradation phenomena of SOEC are summarized, with great attention into the anodes/oxygen electrodes, including the commonly used and newly developed anode materials. Meanwhile, mechanistic investigations on the electrode/electrolyte interfaces are provided to unveil how the intrinsic factor, oxygen partial pressure , and the electrochemical operation conditions, affect the interfacial stability of SOEC. At last, this paper also presents some emerging mitigation strategies to circumvent long-term degradation, which include novel infiltration method, development of new anode materials and engineering of the microstructure.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Chemical Vapor Transformation of Lithium Metal: Mechanism and Enhanced Stability

Constructing a stable solid electrolyte interface (SEI) with high productivity and scalability is essential for the practical application of thin Li metal anodes. Here, in this work, we report a chemical vapor transformation (CVT) strategy in which Li metal is exposed to trimethylaluminum (TMA), inducing a rapid and spontaneous surface reaction that forms a robust, multilayered SEI. In situ quartz crystal microbalance (QCM) and quadrupole mass spectrometry (QMS), combined with ex situ X-ray photoelectron spectroscopy (XPS), UV Raman spectroscopy, and density functional theory (DFT) calculations, reveal that TMA removes the native passivation layer, reacts with Li metal, and drives a coupled bulk-surface transformation involving Li–Al interdiffusion. The resulting SEI exhibits a chemically graded structure consisting of an inner Li–Al alloy and an outer amorphous carbon layer formed via demethylation and ligand-exchange pathways. This modified surface exhibits significantly enhanced stability compared to that of bare Li in electrochemical cycling using liquid and solid-state electrolytes. This work unveils a unique surface-mediated bulk transformation mechanism for lithium metal and establishes CVT as a scalable and fundamentally distinct approach for the interfacial engineering of reactive metals.

Li metal↗
DOE OSTI2022

Emergence of ferrimagnetism in Li-intercalated NiPS 3

AbstractIntercalation has become a powerful approach to tune the intrinsic properties and introduce novel phenomena in layered materials. Intercalating van der Waals (vdW) magnetic materials is a promising route to engineer the low-dimensional magnetism. Recently, metal thiophosphates, MPX 3 , has been widely studied because their magnetic orders are highly tunable and persist down to the two-dimensional limit. In this work, we used electrochemical technique to intercalate Li into NiPS 3 single crystals and found the emergence of ferrimagnetism at low temperature in Li-intercalated NiPS 3 . Such tuning of magnetic properties highlights the effectiveness of intercalation, providing a novel strategy to manipulate the magnetism in vdW magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1971

A study of alternative methods for reclaiming oxygen from carbon dioxide and water by a solid-electrolyte process for spacecraft applications

Two alternative technical approaches were studied for application of an electrochemical process using a solid oxide electrolyte (zirconia stabilized by yttria or scandia) to oxygen reclamation from carbon dioxide and water, for spacecraft life support systems. Among the topics considered are the advisability of proceeding to engineering prototype development and fabrication of a full scale model for the system concept, the optimum choice of method or approach to be carried into prototype development, and the technical problem areas which exist.

Source record↗
NASA NTRS1985

Design of a regenerative fuel cell system for Space Station

The NASA Space Station will employ alkaline regenerative fuel cells (RFCs) as its sole electrochemical energy storage system, in virtue of demonstrated technology readiness and a high degree of system-level design flexibility. NASA Johnson and NASA Lewis are currently engaged in the development of a 10-kW alkaline engineering model system, for 1987 delivery, which will encompass a fully autonomous 120-V system with 55 percent overall electrical efficiency and a 20,000-hr service life.

Hoberecht, M. A.↗