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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Electrically Insulated Catalyst–Ionomer Anode Interfaces toward Durable Alkaline Membrane Electrolyzers

Anion-exchange-membrane water electrolysis (AEMWE) is an emerging technology for scalable hydrogen production. AEMWE has poor durability when operating without supporting electrolyte due to the oxidation of ionomers and membranes in contact with the anode oxygen evolution reaction (OER) catalyst. We report a new “passivated” anode architecture for AEMWE where the OER catalysts and ionomers are physically separated with a thin film amorphous oxide coating that is electrically insulating but conductive to hydroxide ions. We find that 2–3 nm of HfO x passivation layers show sufficient hydroxide ion transport to minimally limit the cell performance while suppressing ionomer degradation with both Ir (500 mA·cm –2 for 40 h) and CoO x (1.0 A·cm –2 for 100 h) model porous-transport-layer-supported catalysts in AEMWE. As a result, this interfacial engineering approach guides electrode design to improve the durability of AEMWE, particularly for systems operating with pure-water feed.

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

High-pressure CO 2 permeation properties and stability of ceramic-carbonate dual-phase membranes

CO 2 permeation properties and stability of ceramic-carbonate dual-phase membranes at high pressures/temperatures are critical to their CO 2 separation and membrane reactor applications, but such data are not available in the literature. Here, this work aims to study the effect of high transmembrane pressure on CO 2 permeation flux and the stability of molten carbonate in the dual-phase samarium-doped ceria (SDC) and molten-carbonate (MC) membranes. Dead-end porous SDC tubular supports were made by a cold isostatic press (CIP)/sintering method with a low porosity (below 7%), and gas-tight SDC-MC membranes were prepared by direct infiltration of molten lithium and sodium carbonate mixture into SDC pores, with a MC volume fraction less than 7%. CO 2 permeation/separation tests were performed on the SDC-MC membranes using feed gas of equal molar CO 2 /N 2 mixture at feed pressures up to 15 atm and sweep gas of helium at 1 atm. CO 2 permeation flux for the SDC-MC membranes depends logarithmically on feed/permeate CO 2 pressure ratio in 660–810°C. The temperature dependence of CO 2 permeation shows activation energy of 30 kJ/mol. Due to the small MC volume fraction and hence low effective carbonate conductivity, CO 2 permeation of the SDC-MC membranes is dominated by the carbonate ionic conduction in the MC phase. The SDC-MC membranes remain in the same structure, morphology, and gas-tightness after CO 2 separation tests at high feed pressures and temperatures, showing high stability of SDC-MC membranes for high-temperature, high-pressure separation and chemical reaction applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Critical Practices in Rigorously Assessing the Inherent Activity of Nanoparticle Electrocatalysts

Accurate activity measurements for electrocatalytic materials are the backbone of impactful electrocatalyst research. Inherent to accurate measurements is the correct accounting of the active catalyst sites and the design of experiments to ensure that these sites are participating in the measured reaction. Improvements in electrocatalyst activity for fuel cell reactions (hydrogen oxidation and oxygen reduction) are essential for the widespread adoption of this carbon-neutral energy source. Activities for these half-reactions can be reported in a variety of ways including specific activities, mass activities, volumetric activities, and half-wave potentials. These values are traditionally measured with a rotating disk electrode (RDE) in which the electrocatalyst is supported on a porous active layer film attached to the RDE. To accurately measure electrocatalyst activity with an RDE, two major sources of errors must be addressed: (i) accurate electrochemical surface area (ECSA) quantification and (ii) fast diffusion of reactants through the active layer film. In this contribution, we first aim to detail through RDE experiments and mass transport modeling the potential errors that can be observed when these factors are not properly addressed. We then present recommendations and discuss techniques for properly constructing electrocatalyst thin films and characterizing the ECSA on monometallic and novel alloy electrocatalysts. These practices, when adopted, ensure greater confidence and reliability in reports of electrocatalyst activity.

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

Ternary PtIrNi Catalysts for Efficient Electrochemical Ammonia Oxidation

Due to high energy density, carbon-free feature, and easiness to be liquefied, ammonia (NH 3 ) has proved to be an effective alternative to hydrogen in low temperature fuel cells via its direct the ammonia oxidation reaction (AOR) for electricity generation. However, the kinetically sluggish AOR has prohibitively hindered the attractive direct ammonia fuel cell (DAFC) applications. Here we report an efficient AOR catalyst, in which ternary PtIrNi alloy nanoparticles well dispersed on a binary composite support consisting of porous silicon dioxide (SiO 2 ) and carboxyl-functionalized carbon nanotube (PtIrNi/SiO 2 -CNT-COOH) through a sonochemical-assisted synthesis strategy. The PtIrNi alloy nanoparticles, with the aid of abundant OHad provided by porous SiO 2 , and the improved electrical conductivity by CNTs, exhibit remarkable catalytic activity for the AOR in alkaline media. It is evidenced by a lower onset potential (~0.40 V vs. RHE) at room temperature, than that of commercial PtIr/C (ca. 0.43 V vs. RHE). Increasing NH 3 concentrations and operation temperatures significantly improve AOR performance of this catalyst. Specifically, AOR activity of the optimal PtIrNi nanoparticle catalyst can be significantly enhanced by elevating the temperature to 80ºC, with a much lower onset potential (~0.32 V vs. RHE), indicating that DAFC can be operated at higher temperature for increased performance. Constant-potential density functional theory (DFT) calculations showed that the Pt-Ir ensembles on {100}-terminated surfaces serve as the active site. Importantly, the introduction of Ni raises the center energy of the density of states projected onto the group d-orbitals of surface sites and thus lowers the theoretical onset potential for *NH 2 dehydrogenation to *NH when compared to Pt and Pt 3 Ir alloy.

25 ENERGY STORAGE↗
DOE OSTI2025

Ultrahigh pressure compaction-resistant thin film crosslinked composite reverse osmosis membranes

In this study, we present a class of thin-film crosslinked (TFX) composite reverse osmosis (RO) membranes that resist physical compaction at ultrahigh pressures (up to 200 bar). Since RO membranes experience compaction at virtually all pressure ranges, the ability to resist compaction has widespread implications for RO membrane technology. The process described herein involves crosslinking a phase inverted porous polyimide (PI) support membrane followed by interfacial polymerization of a polyamide layer, thereby forming a fully thermoset composite membrane structure. We explore a range of phase inversion membrane formation parameters such as PI concentration, solvent-cosolvent ratios, coagulation bath composition, and crosslinking methods in addition to interfacial polymerization reaction chemistry and conditions. Overall, TFX membranes exhibit significantly less compaction compared to hand-cast and commercial high-pressure RO membranes, experiencing less than 10% decline in water permeance and maintaining salt rejection over 99% for NaCl solutions up to 180,000 mg/L with 200 bar applied pressure.

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

Optical sensing of aqueous nitrate anion by a platinum( II ) triimine salt based solid state material

Selective and quantitative measurement of aqueous nitrate (NO 3 – ) anion is achieved using solid [Pt(Cl-4-tpy)Cl]ClO 4 salt (Cl-4-tpy = 4-chloro-2,2':6'2''-terpyridine), and as the salt supported on controlled porous glass. This detection method relies on the color change of the Pt(II) complex from yellow to red and intense luminescence response upon ClO 4 – exchange with NO 3 – due to concomitant enhancement of Pt∙∙∙Pt interactions. Finally, the spectroscopic response is highly selective for NO 3 – over a large range of halides and oxoanions.

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

High-Platinum-Content Catalysts on Atomically Dispersed and Nitrogen Coordinated Single Manganese Site Carbons for Heavy-Duty Fuel Cells

Fuel cells for heavy-duty vehicles (HDVs) have attracted considerable attention because of their unique scalability, better fuel economy, the less demand for hydrogen refilling infrastructure. However, the potential application requires more stringent fuel cell durability up to 25,000 h. Membrane electrode assemblies (MEAs) made from platinum group metal (PGM) catalyst with relatively high loading 0.3 mgPt cm –2 play a crucial role in ensuring high-power and long-term durability. Integrating fine PGM nanoparticles and robust carbon support with strengthened interactions is critical for improving MEA performance and durability. Herein, a unique atomically dispersed and nitrogen coordinated single Mn site-rich carbon (M–N–C) support was developed for high content (40 wt%) platinum catalysts for the oxygen reduction reaction (ORR) cathode with reduced thickness. Compared with two controls studied in this work (e.g., a porous graphitic carbon-supported Pt and a commercial TKK Pt/C catalysts), the Pt (40 wt%)/Mn–N–C catalyst exhibited much enhanced catalytic activity and stability for the ORR in both aqueous acidic electrolyte and polymer electrolyte-based MEA. Here, we carefully elucidated the—role of the Mn–N–C support in promoting Pt catalyst concerning its high surface area, partially graphitic structure, and nitrogen dopants, providing better Pt nanoparticle dispersion, and strengthened interactions between Pt and carbon. Consequently, the MEA from the Pt (40 wt%)/Mn–N–C catalyst generated a 1.61 A cm –2 at 0.7 V based on HDV conditions (0.2 mgPt cm –2 and 250 kPa air). More importantly, the MEA is highly durable and can retain 1.31 A cm –2 at 0.7 V after 30,000 voltage cycles (~19% loss), surpassing the commercial Pt/C catalyst (loss of ~56%). Therefore, the Mn–N–C carbon-supported Pt catalyst holds a great promise to meet the challenging DOE target (1.07 A cm –2 at 0.7 V after 150,000 cycles) for HDVs.

25 ENERGY STORAGE↗
DOE OSTI2022

Catalytic reactor

A catalytic reactor constructed of a thermally conductive housing defining a reaction zone having disposed therein: (a) a plurality of catalytic elements, each comprising a porous material having a catalyst supported thereon, and (b) a plurality of heat transfer elements, each comprising a porous, thermally conductive, and essentially catalytically inactive material; wherein the plurality of catalytic elements and the plurality of heat transfer elements are disposed in an alternating configuration within the reaction zone. The catalytic reactor is useful in chemical reactions where heat transfer is a rate limiting step.

Smith, Warren F.↗
DOE OSTI2021

The Coordination Chemistry and Stoichiometry of Extracted Diglycolamide Complexes of Lanthanides in Extraction Chromatography Materials

Industrial rare earth element (REE) separations predominantly utilize solvent extraction processes tailored toward conventional resources such as bastnäsite, monazite, and ion adsorption clays. Advances in diglycolamide (DGA) chemistry have shown effective extraction characteristics for REE separations. However, limitations associated with traditional DGA solvent extraction techniques, such as third-phase formation and gelling, have hindered commercial viability. By supporting DGA extractants on porous resins such as polystyrene divinyl benzene (PS-DVB), the desirable combination of solvent extraction selectivity and ease of operation of sorbent columns can be achieved. To design a low-cost model for such solid-supported DGAs, extraction characteristics as influenced by the underlying coordination chemistry must be explored to achieve efficient functional systems. Within this study, we report novel DGA resin materials, each incorporating one of the DGAs N,N,N’,N’-tetra-(1-octyl)-3-oxapentane-1,5-diamide (TODGA), N,N'-dimethyl-N,N'-dioctyl-3-oxapentane-1,5-diamide (DMDODGA), and 2,2'-oxybis(1-(3-(((2-ethylhexyl)thio)methyl)-4-methylpyrrolidin-1-yl)ethan-1-one) (DEHPDGA). The affinity of DGAs across the lanthanide (Ln) series was evaluated for both hydrochloric acid and nitric acid media with varying Ln feed concentrations to study distribution ratios and loading characteristics. Focusing on dysprosium, extended X-Ray Absorption Fine Structure (EXAFS) and density functional theory (DFT) calculations were also utilized to explore coordination chemistry and their effects on ligand performance. The general trend for both acid media resulted in DMDODGA having the highest extraction strength of all three DGAs at varying acid concentrations. Coordination-chemistry analysis supported by loading data, DFT calculations, and EXAFS results under forced loading conditions posited less than the expected 3:1 ligand-to-metal coordination.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Structural Characterization of the Platinum Nanoparticle Hydrogen-Evolving Catalyst Assembled on Photosystem I by Light-Driven Chemistry

Directed assembly of abiotic catalysts onto biological redox protein frameworks is of interest as an approach for the synthesis of biohybrid catalysts that combine features of both synthetic and biological materials. In this report, we provide a multiscale characterization of the platinum nanoparticle (NP) hydrogen-evolving catalysts that are assembled by light-driven reductive precipitation of platinum from an aqueous salt solution onto the photosystem I protein (PSI), isolated from cyanobacteria as trimeric PSI. The resulting PSI-NP assemblies were analyzed using a combination of X-ray energy-dispersive spectroscopy (XEDS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), small-angle X-ray scattering (SAXS), and high-energy X-ray scattering with atomic pair distribution function (PDF) analyses. The results show that the PSI-supported NPs are approximately 1.8 nm diameter disk-shaped particles that assemble at discrete sites with 145 Å separation. This separation is too large to be consistent with NP nucleation and growth at a site adjacent to the F B cofactor site. Instead, we suggest a mechanism for NP growth at hydrophobic sites on the PSI stromal surface. The NPs photoreductively assembled on the PSI stromal surface are found to be analogous to the nanostructures produced by successive cycles of atomic layer deposition (ALD) of platinum onto 40 nm porous anodic alumina oxide supports, although the mechanisms for nucleation appear to differ. In conclusion, this work establishes a foundation for the investigation of the reductive assembly of abiotic metal catalysts at sites connected to photochemically reducing equivalent production in PSI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Raman Microscopy Investigation of GLP-1 Peptide Association with Supported Phospholipid Bilayers

A wide range of important biological processes occur at phospholipid membranes including cell signaling, where a peptide or small molecule targets a membrane-localized receptor protein. In this work, we report the adaptation of confocal-Raman microscopy to quantify populations of unlabeled glucagon-like peptide-1 (GLP-1), a membrane-active 30-residue incretin peptide, in supported phospholipid bilayers deposited on the interior surfaces of wide-pore porous silica particles. Quantification of lipid bilayer-associated peptide is achieved by measuring the Raman scattering intensity of the peptide relative to that of the supported-lipid bilayer, which serves as an internal standard. The dependence of the bilayer-associated GLP-1 population on the solution-concentration of GLP-1 produces an isotherm used to determine the equilibrium constant for peptide-bilayer association and the maximum peptide surface coverage. The maximum coverage of GLP-1 in the lipid bilayer was found to be only 1/5th of a full monolayer based on its hydrodynamic radius. The saturation coverage, therefore, is not limited by the size of GLP-1 but by the ability of the bilayer to accommodate the peptide at high concentrations within the bilayer. Raman spectra show that GLP-1 association with the supported bilayer is accompanied by structural changes consistent with the intercalation of the peptide into bilayer, where the observed increase in acyl-chain order would increase the lipid density and provide free volume needed to accommodate the peptide. Furthermore, these results were compared with previous measurements of the association of fluorescently-labeled GLP-1 with a planar-supported bilayer; the unlabeled peptide exhibits a 3-fold greater affinity for the lipid-bilayer on the porous-silica support suggesting that the fluorescent label alters GLP-1 lipid-bilayer association.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Influence of Ordered Mesoporous Oxides in Plasma-Assisted Ammonia Synthesis

Widespread implementation of dielectric barrier discharge (DBD)-assisted NH 3 synthesis, a nascent technology operating under sustainable, ambient conditions, is hindered by low energy yields due to, in part, poor fundamental understanding. Porous oxides used to support metal nanoparticle catalysts have shown significant energy yield contributions for DBD-assisted NH 3 synthesis even without metal. Using an AC-powered, coaxial, single-stage reactor at 16 kV with equimolar (N 2 /H 2 ) feed, we measured NH 3 synthesis rates in the presence of different nonordered oxides, ordered SiO 2 structures (SBA-15 and MCM-41), and ordered Al-incorporated analogues (γ-Al 2 O 3 -coated with varying Al-loadings and Al-substitution, respectively: Al 2 O 3 -SBA-15 and Al-MCM-41). We systematically quantified NH 3 energy yield dependence on pore structures and material identities (i.e., ordered pores and Al incorporation) known to facilitate higher DBD-assisted NH 3 synthesis rates. SBA-15 displayed a higher steady-state energy yield than MCM-41, indicating that framework type is a crucial factor, with both ordered porous systems outperforming fumed SiO 2 . 10 wt % Al maximized in situ NH 3 uptake among the various Al loadings, exhibiting a higher steady-state energy yield and similar power to SBA-15. However, Al-MCM-41 had a similar steady-state energy yield and lower power than MCM-41, likely due to the extended γ-Al 2 O 3 surface that has a dielectric constant higher than that of SiO 2 . Both Al-incorporated analogues benefit from surface acid sites that can adsorb NH 3 in situ, resulting in higher overall NH 3 energy yields than that of their parent ordered SiO 2 . Al 2 O 3 -SBA-15 shielded more NH 3 than Al-MCM-41, likely due to a higher acid site density than the acid site identity. Furthermore, Al incorporation via γ-Al 2 O 3 coating more successfully improves the NH 3 energy yield; together with the high-performing ordered framework, these analogues are potential metal catalyst supports with promising energy yields for DBD-assisted synthesis of NH 3 and other chemicals.

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

Fabrication and Characterization of Composite Membranes for the Concentration of Lithium Containing Solutions Using Forward Osmosis

In this study, an energy and highly time efficient, cost effective, and scalable forward osmosis (FO) composite polyvinylidene fluoride (PVDF) membrane is developed to concentrate lithium chloride recovered from naturally occurring geothermal brine resources. Dense thin robust defect-free Kynar-PVDF membranes are fabricated on porous PVDF hollow fiber supports. Various membrane fabrication parameters such as membrane thickness, coating solution concentration, cross-linker concentration, and curing temperature are studied to develop a defect-free dense membrane. Advanced characterization tools such as FIB-SEM, Raman, FTIR spectroscopy, and XRD are used to study the surface and cross-sectional morphology, chemistry of crosslinking, crystallinity and chemical structure of the dense PVDF membrane. FO is utilized to concentrate LiCl in the solution from 36 to 175 g L -1 with an average water transfer rate of 0.450 L m -2 h -1 (LMH) at 85 °C. Furthermore, the membrane showed stable performance for more than 550 h while maintaining the purity of the concentrated lithium chloride solution of >99.99 wt%. Overall, the results suggest that the FO-based technology is an innovative, time and energy efficient approach compared to the conventional technologies for concentration of battery grade LiCl for application in lithium ion batteries and other clean energy technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Graphite crystals in catalytically-graphitized glass-like carbon

Catalytic graphitization of glass-like carbon leads to enhanced growth of micro-sized graphitic crystals with unusual shapes of wires, filaments, tubes, rods, whiskers, and spirals. Similar particles with axial symmetry are also found in pure glass-like carbon heat-treated at high temperatures. Nonetheless, the presence of a graphitization catalyst, Si in this case, in the heat-treatment process supports the transformation of porous, disordered carbon structure towards the graphitic atomic order and the formation of manifold peculiar polyhedral wires and particles of geometry distinct from the plate-like shape typical for conventional graphite. In contrast to conventional carbon nanotubes and fibers, the graphene layers are stacked perpendicular to the tube axis, while the size of the most common tube fibers can reach up to 10 μm in diameter and 100 μm in length. X-ray diffraction, Raman spectroscopy, scanning and transmission electron microscopy, small-angle X-ray scattering combined with complementary techniques have been used to characterize the structure of the glass-like carbon derived from furfuryl alcohol catalytically-graphitized using Si particles at 3000 °C. Finally, since control of graphite shape is vital to achieving the level of performance required in contemporary applications, the obtained results demonstrate that the catalytic graphitization method may be employed to produce filamentous graphite crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Carbon molecular sieve membrane for gas separations

An ultrathin high permselectivity carbon molecular sieve membrane (CMSM) for industrial gas separations is provided. The CMSM includes porous metal or ceramic supports to provide superior stability at high temperatures, pressures and chemical environments. The CMSM also offers the potential for cost-effective gas processing while overcoming disadvantages found in alternative media that are fragile and susceptible to shock due to thermal cycling and prone to end-sealing problems under industrial conditions.

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

Process and apparatus for continuous production of porous structures

An apparatus and process are presented for continuous production of metal-based micro-porous structures of pore sizes from 0.3 nm to 5.0 μm from a green part of characteristic diffusion mass transfer dimension less than 1 mm through chemical reactions in a continuous flow of gas substantially free of oxygen. The produced micro-porous structures include i) thin porous metal sheets of thickness less than 200 μm and pore sizes in the range of 0.1 to 5.0 μm, ii) porous ceramic coating of thickness less than 40 μm and ceramic particle sizes of 200 nm or less on a porous metal-based support structures of pore sizes in the range of 0.1 to 5 μm.

Liu, Wei↗
DOE OSTI2020

EGS Collab Experiment 1: DNA tracer data on transport through porous media

This submission contains DNA tracer data that supports the analysis and conclusions of the publication, "DNA tracer transport through porous media -The effect of DNA length and adsorption." https://doi.org/10.1029/2020WR028382. This experiment used DNA as an artificial reservoir tracer. Groundwater tracing is an effective way to identify fluid flow pathways and estimate hydrogeologic properties, which are important premises for building reliable hydrological models for transport predictions or contamination mitigations. The objective of this study was to understand the effect of DNA length (i.e., number of base pairs for dsDNA) and adsorption on DNA transport.

15 GEOTHERMAL ENERGY↗
DOE OSTI2022

Nano-porous GaN cladding and scattering loss in edge emitting laser diodes

We report continuous wave operation of electrically injected InGaN laser diodes using nano-porous GaN n-side cladding with 33% porosity. At 454 nm emission wavelength, the pulsed injection slope efficiency is 0.24 W/A with a high loss of 82 cm -1 . The considerable 60 cm -1 of excess loss of the nano-porous clad lasers is attributed to scattering at pores in unintentionally 3% porosified layers, supported by numerical modeling. Simulations comparing porous GaN cladding to AlInN cladding for lasers operating at 589 nm indicate that the porous cladding provides similar internal loss and lower thermal impedance.

36 MATERIALS SCIENCE↗