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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Surface-Enhanced Raman Scattering (SERS) Studies of Disc-on-Pillar (DOP) Arrays: Contrasting Enhancement Factor with Analytical Performance

The use of nanomachining methods capable of reproducible construction of nano-arrayed devices have revolutionized the field of plasmonic sensing by the introduction of a diversity of rationally engineered designs. Significant strides have been made to fabricate plasmonic platforms with tailored interparticle gaps to improve their performance for surface-enhanced Raman scattering (SERS) applications. Over time, a dichotomy has emerged in the implementation of SERS for analytical applications, the construction of substrates, optimization of interparticle spacing as a means to optimize electromagnetic field enhancement at the localized surface plasmon level, and the substrate sensitivity over extended areas to achieve quantitative performance. Here, we assessed the enhancement factor of plasmonic Ag/SiO 2 /Si disc-on-pillar (DOP) arrays of variable pitch with its analytical performance for quantitative applications. Experimental data were compared with those from finite-difference time-domain (FDTD) simulations used in the optimization of the array dimensions. A self-assembled monolayer (SAM) of benzenethiol rendered highly reproducible signals (RSD ~4–10%) and SERS substrate enhancement factor (SSEF) values in the orders of 10 6 –10 8 for all pitches. Furthermore, spectra corresponding to rhodamine 6G (R6G) and 4-aminobenzoic acid demonstrated the advantages of using the more densely packed DOP arrays with a 160 nm pitch (gap= 40 nm) for quantitation in spite of the strongest SSEF was attained for a pitch of 520 nm corresponding to a 400 nm gap.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Birefringent Glass‐Engraved Tilted Pillar Metasurfaces for High Power Laser Applications

Abstract Birefringent materials—which are highly needed in high power laser systems—may be limited in usage due to the laser‐induced damage threshold of traditional birefringent materials. This work reports here on all‐glass metasurfaces, fabricated by angled etching through sacrificial metal nanoparticle (NP) etching masks, for generation of effective birefringence in the formed layer. As a result, a fused silica metasurface, monolithic to the underlying substrate, is demonstrated to exhibit a birefringence of 6.57° under 375 nm illumination. Full‐wave analysis shows a good agreement with the measurement and presents potential paths forward to increasing the effective metasurface birefringence. This is the first demonstration, to the best of knowledge, of an etching technique to obtain the resulting tilted pillar‐like nanofeatures. The anisotropy of the metasurface nanoelements along the two window in‐plane major axes presents different effective paths for the two polarizations and thus generates birefringence in a nonbirefringent material. Additionally, the imparted anisotropy lends itself to manipulation of physical properties of the surface as well, with metasurface feature orientation suppressing water flow along one principal axis and giving rise to water flow steering capabilities.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Isoreticular Expansion of Metal–Organic Frameworks via Pillaring of Metal Templated Tunable Building Layers: Hydrogen Storage and Selective CO2 Capture

The deliberate construction of isoreticular eea-metal–organic frameworks (MOFs) (Cu-eea-1, Cu-eea-2 and Cu-eea-3) and rtl-MOFs (Co-rtl-1 and Co-rtl-2) has been accomplished based on the ligand-to-axial pillaring of supermolecular building layers. The use of different metal ions resulted in two types of supermolecular building layers (SBLs): Kagome (kgm) and square lattices (sql) which further interconnect to form anticipated 3D-MOFs. The isoreticular expansion of (3,6)-connected Cu-MOFs has been achieved with desired eea-topology based on kgm building layers. In addition, two (3,6)-connected Co-rtl-MOFs were also successfully constructed based on sql building layers. The Cu-eea-MOFs were shown to act as hydrogen storage materials with appreciable amount of hydrogen uptake abilities. Moreover Cu-eea-MOFs have also exhibited remarkable CO2 capture ability at ambient condition compared to nitrogen and methane, due to the presence of amide functionalities.

Maity, Kartik↗
DOE OSTI2020

Water-Pillared Sodium Vanadium Bronze Nanowires for Enhanced Rechargeable Magnesium Ion Storage

Owing to the advantages of high safety, low cost, high theoretical volumetric capacities, and environmental friendliness, magnesium-ion batteries (MIBs) have more feasibility for large-scale energy storage compared to lithium-ion batteries. However, lack of suitable cathode materials due to sluggish kinetics of magnesium ion is one of the biggest challenges. Herein, water-pillared sodium vanadium bronze nanowires (Na 2 V 6 O 16 ·1.63H 2 O) are reported as cathode material for MIBs, which display high performance in magnesium storage. The hydrated sodium ions provide excellent structural stability. The charge shielding effect of lattice water enables fast Mg 2+ diffusion. It exhibits high specific capacity of 175 mAh g -1 , long cycle life (450 cycles), and high coulombic efficiency (≈100%). At high current density of 200 mA g -1 , the capacity retention is up to 71% even after 450 cycles (compared to the highest capacity), demonstrating excellent long-term cycling performance. The nature of charge storage kinetics is explored. Furthermore, a highly reversible structure change during the electrochemical process is proved by comprehensive electrochemical analysis. The remarkable electrochemical performance makes Na 2 V 6 O 16 ·1.63H 2 O a promising cathode material for low-cost and safe MIBs.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Electrochemical DNA sensors on the basis of electropolymerized thionine and Azure B with addition of pillar[5]arene as an electron transfer mediator

A DNA sensor was developed on the basis of glassy carbon electrode coated with polymeric forms of thionine and Azure B. Introduction of carbon black and pillar[5]arene into the electrode composition increases the efficiency of polymerization and the oxidation peak currents of dyes due to the mediating effect of the macrocycle. The addition of DNA onto the sensor surface and into the reaction mixture differently influences the electrochemical activity of poly(Azure B) and polythionine. The control of changes in current-voltage characteristics allowed us to identify the heat denaturation of DNA and its oxidation by reactive oxygen species generated upon the reaction of hydrogen peroxide and copper(II) salt. The DNA sensors can find application in the diagnosis of DNA damage on exposure to carcinogens and in screening of cytotoxic anticancer drugs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Friction Hydro-Pillar Processing of a High Carbon Steel: Joint Structure and Properties

A coupled experimental and theoretical study is reported here on friction hydro-pillar processing of AISI 4140 steel, which is a novel solid-state joining technique to repair and fill crack holes in thick-walled components by an external stud. The stud is rotated and forced to fill a crack hole by plastic flow. During the process, frictional heating occurs along the interface of the stud and the wall of crack hole leading to thermal softening of the stud that eases its plastic deformation. The effect of the stud force, its rotational speed and the total processing time on the rate of heat generation and resulting transient temperature field is therefore examined to correlate the processing variables with the joint structure and properties in a systematic and quantitative manner, which is currently scarce in the published literature. The results show that a gentler stud force rate and greater processing time can promote proper filling of the crack hole and facilitate a defect-free joint between the stud and original component.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Experimentally quantifying critical stresses associated with basal slip and twinning in magnesium using micro-pillars

Basal slip and {01$\bar{1}$2} twinning are two major plastic deformation mechanisms in hexagonal closed-packed magnesium. Here in this paper, we quantify the critical stresses associated with basal slip and twinning in single-crystal and bi-crystal magnesium samples by performing in situ compression of micropillars with different diameters in a scanning electron microscope. The micropillars are designed to favor either slip or twinning under uniaxial compression. Compression tests imply a negligible size effect related to basal slip and twinning as pillar diameter is greater than 10 μm. The critical resolved shear stresses are deduced to be 29 MPa for twinning and 6 MPa for basal slip from a series of micropillar compression tests. Employing full-field elasto-visco-plastic simulations, we further interpret the experimental observations in terms of the local stress distribution associated with multiple twinning, twin nucleation, and twin growth. Our simulation results suggest that the twinning features being studied should not be close to the top surface of the micropillar because of local stress perturbations induced by the hard indenter.

36 MATERIALS SCIENCE↗
DOE OSTI2020

In Situ Micro-Pillar Compression to Examine Radiation-Induced Hardening Mechanisms of FeCrAl Alloys

Here, the effects of 5 MeV Fe 2+ ion irradiation at 300°C on the microstructure evolution and deformation behavior of a FeCrAl C26M alloy are presented. It has been found that dislocation loop density increases an order of magnitude from 1 dpa to 16 dpa irradiations, whereas, the dislocation loop size saturates with increasing damage. Micropillars, 600 nm in diameter and 1.3 µm in height, were fabricated and compressed inside grains with <001>, <011> and <111> crystallographic orientations, respectively. {112} <111> has been identified as the primary slip system in both unirradiated and irradiated alloy. The increase in yield stress after irradiation is observed with measurable variation along <001> and <011> vs. along <111>. By applying the Orowan dispersed barrier model, the increase of yield stress is found mainly due to the slip resistance of radiation generated defect loops. Detailed transmission electron microscopy (TEM) studies were performed to quantify the Burgers vector and the distribution of irradiation induced dislocations at elevated strains. It is revealed that localized shear instability is caused by avalanche slip events of ½<111> dislocations gliding out of tested pillars. Simultaneously, a large number of sessile/immobile <100> dislocations formed in the vicinity of slip band, leading to the hardening at elevated strains.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Morphology engineering of iridium electrodes via modifying titanium substrates with controllable pillar structures for highly efficient oxygen evolution reaction

Nowadays, Ti is the well-chosen anode substrate material for proton exchange membrane electrolyzer cells (PEMECs) and modifications of the substrate surfaces are essential for the fabrication of highly efficient electrodes. Herein, we introduce the morphology engineering of Ir/Ti electrodes with different acid treatments of hydrochloric acid (HCl) and oxalic acid (OA), and the comparative benefits of these two acid treatment methods are studied from the aspects of their impacts on the morphology, interfacial contact resistance (ICR), and oxygen evolution reaction (OER) performances of resultant electrodes. Notably, compared to the flat surface from OA treatment, Ti substrates with the pillar structure could be successfully achieved via HCl etching. Further, the HCl and the oxalic acid (OA) treatments would reduce the interfacial contact resistance (ICR) to 15.2% and 5.5% of the pristine Ti substrate at 1.38 MPa, respectively. By iridium electrodeposition on Ti substrates, Ir/Ti electrodes with different catalyst loadings are fabricated. With similar low-loadings of about 0.05 mgIr cm –2 , an Ir/Ti electrode with HCl treated substrate exhibits a lower overpotential of ~283 mV at 10 mA cm –2 current density than 305 mV from OA treatment, due to the boosted reaction areas from HCl treatment.

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

Theoretical design and performance of three-dimensional, pillared FeS 2 cathodes

Three-dimensional (3D) electrode design can provide improved capacities and rate capabilities over conventional two-dimensional electrodes by enhancing electrical and ionic transport. Here, expanding upon our previous modeling efforts for conversion chemistry lithium-ion batteries, we develop a pseudo-four-dimensional (P4D) approach that is subsequently used to investigate the design of a pillared FeS 2 electrode. The model considers transport in three dimensions with an additional “fourth” dimension corresponding to the solid-state lithium transport within the active material particles. Additionally, we allow for expansion of the active material during the conversion reaction to understand how internal stresses impact the electrochemical performance of the cell. By optimizing the model with respect to areal capacity, we are able to predict areal capacities up to 16.8 mAh/cm 2 for an areal current density of 1.78 mA/cm 2 and a 103% improvement for the three-dimensional electrodes over planar electrodes of equal volume. Despite the promising results, our simulations suggest that 3D design may be difficult for conversion cathode materials due to the large internal stresses that arise during conversion. Nevertheless, the model is robust and adaptable to other materials that may be more suitable for 3D electrodes due to a lesser change in volume during discharge.

Conversion cathode materials↗
DOE OSTI2020

Intrinsic size dependent plasticity in BCC micro-pillars under uniaxial tension and pure torsion

The mechanical behavior of submicron body-centered cubic (BCC) micro-pillars is investigated by three-dimensional dislocation dynamics (DD) simulations to better understand the governing mechanisms for size dependent plasticity under uniaxial tension and pure torsion. A formula is developed to compute the incremental plastic twist due to dislocation motion in DD simulations. The DD simulations show that different dislocation microstructures are created depending on the loading conditions, which leads to different size dependent mechanical behavior. While in tension plasticity is mainly governed by the kinetics of dislocation motion controlled partly by the surface dislocation sources, plastic flow in torsion is controlled by dislocation pile-ups associated with strain gradients. The simulation results also reveal a Bauschinger effect and plastic recovery under cyclic twist, which have been observed in recent experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2015

The influence of a silica pillar in lamellar tetratitanate for selective catalytic reduction of NO{sub x} using NH{sub 3}

Highlights: • Potassium ions significantly affected the SCR. • The introduction of silica in the catalyst promotes the NH{sub 3}-SCR reaction. • The catalysts activities were not significantly influenced by SO{sub 2} addition. - Abstract: Silica-pillared layered titanate (SiO{sub 2}–Ti{sub 4}O{sub 9}) was prepared by intercalating organosilanes into the interlayers of a layered K{sub 2}Ti{sub 4}O{sub 9} followed by calcination at 500 °C. The lamellar titanates produced were used as a support to prepare vanadium catalysts (1 and 2 wt%) through wet impregnation for selective catalytic reduction (SCR) of NO. The catalysts were characterized using nitrogen adsorption (BET), X-ray diffraction (XRD), temperature programmed reduction (H{sub 2}-TPR), nuclear magnetic resonance ({sup 29}Si NMR), and infrared spectroscopy (FT-IR). Reduction of NO by NH{sub 3} was studied in a fixed-bed reactor packed with the catalysts and fed a mixture comprising 1% NH{sub 3}, 1% NO, 10% O{sub 2}, and 34 ppm SO{sub 2} (when used) in helium. The results demonstrate that activity is correlated with the support, i.e., with acidic strength of catalysts. The potassium in the support, K{sub 2}Ti{sub 4}O{sub 9}, significantly affected the reaction and level of vanadium species reduction. The catalyst (1VSiT) with 1 wt% vanadium impregnated on the SiO{sub 2}–Ti{sub 4}O{sub 9} support reduced ∼80% of the NO. Approximately the same conversion rate was generated on the catalyst (2VSiT) with 2 wt% vanadium using the same support. The increased NH{sub 3} adsorption demonstrate that introduction of silica in the catalyst promotes the NH{sub 3}-SCR reaction. More importantly, 2VSiT and 1VSiT were strongly resistant to SO{sub 2} poisoning.

36 MATERIALS SCIENCE↗
DOE OSTI2015

CdS-pillared CoAl-layered double hydroxide nanosheets with superior photocatalytic activity

Graphical abstract: - Highlights: • CdS nanocrystals were intercalated into CoAl-LDH interlayer. • The nanohybrid display superior visible-light photocatalytic activity. • A photoexcitation model for the pillared heterostructured system was proposed. - Abstract: A new nanohybrid was synthesized by mixing the positively charged 2D nanosheets of CoAl-layered double hydroxide (CoAl-LDH) and the negatively charged CdS nanosol suspensions. It was revealed that the CdS nanoparticles were intercalated into the interlayer region of CoAl-LDH with a spacing of 2.62 nm. The obtained nanohybrid exhibited a mesoporous texture with an expanded specific surface area of 62 m{sup 2} g{sup −1} and a superior photocatalytic activity in the degradation of acid red with a reaction constant of 1.26 × 10{sup −2} min{sup −1} under visible-light radiation, which is more than 2 times those of his parents CoAl-LDH and CdS.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Characterization of electronic structures from CdS/Si nanoheterostructure array based on silicon nanoporous pillar array

Highlights: • CdS/Si nanoheterostructure array has been fabricated through a CBD method. • The electronic properties have been investigated by the I–V and C–V techniques. • The onset voltages, characteristic frequency and built-in potential are investigated. • The electronic structures can be tuned through the annealing treatments. - Abstract: The electronic properties of heterostructures are very important to its applications in the field of optoelectronic devices. Understanding and control of electronic properties are very necessary. CdS/Si nanoheterostructure array have been fabricated through growing CdS nanocrystals on the silicon nanoporous pillar array using a chemical bath deposition method. The electronic properties of CdS nanoheterostructure array have been investigated by the current–voltage, complex impedance spectroscopy and capacitance–voltage techniques. The onset voltages, characteristic frequency and built-in potential are gradually increased with increasing the annealing temperature. It is indicated that the electronic structures of CdS/Si nanoheterostructure array can be tuned through the annealing treatments.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Fabrication of a Pillared ZSM-5 Framework for Shape Selectivity of Ethane Dehydroaromatization

Ethane, the second major component of shale gas, is a prospective raw feedstock to valuable chemicals and fuels. Innovative pillared ZSM-5 with various lamellar thicknesses and Si/Al ratios were successfully synthesized with the dual-template method; 0.67 wt % Mo were dispersed over these lamellar ZSM-5, and evaluated for ethane dehydroaromatization. The influence of zeolite morphology and the texture property for the reduction/acidity nature of MoOx species were investigated by X-ray diffraction, scanning electron microscopy, N2-sorption, H2-temperature programmed reduction/oxidation, and NH3-temperature-programmed desorption. The high concentration of acidic sites not only increases ethane conversion and aromatic selectivity, but intensely induces surface coking. Therefore, a moderate Si/Al ratio is utilized to balance catalytic reactivity and stability. Thicker zeolite layers with a long diffusion path exhibited fair ethane conversion, but high aromatization yield. It is of significant importance that the lamellar Mo/MFI catalyst, with Si/Al = 50 and 210 nm layer thickness, demonstrated excellent regenerability during a multicycle reaction/oxidation operation, which could be a promising system for industrial optimization and process deployment.

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

Impact of Ligands on the Ion–Ion Selectivity of Ligand-Appended-Pillar[ n ]arene Channels

Ligand-appended pillar[5]arene (LAP) channels are emerging as a promising platform for ion-selective membranes. In this study, we investigated the ion selectivities of three LAP channels functionalized with distinct ligands: diglycolamine, carbamoylmethyl phosphine oxide, and propionamide phosphonic acid. These ligands were chosen based on their demonstrated affinities for lanthanides in solvent extraction studies. We examined the selectivity of each channel toward a series of monovalent, divalent, and trivalent ions: Li + , Na + , K + , Mg 2+ , Ca 2+ , La 3+ , Eu 3+ , and Yb 3+ . To quantify ion-channel interactions and the energetics of translocation, we computed the potential of mean force (PMF) profiles for each ion. These PMFs were subsequently recast into permeability coefficients, enabling a direct evaluation of ion permselectivity. Our results reveal distinct selectivity patterns governed by the chemical nature of the appended ligands. The diglycolamine-functionalized channel exhibits strong interactions with monovalent ions, leading to replication of the Li + bulk hydration shell within the channel. This promotes preferential transport Li + ions while effectively excluding divalent and trivalent species. In contrast, the carbamoylmethyl phosphine oxide-functionalized channel displays a reduced selectivity between monovalent ions while similarly exhibiting an effective rejection of divalent and trivalent ions. This arises from steric hindrance around channel-lining oxygens imposed by the ligand's bulky phenyl groups which limits heavy ion coordination and promotes retention of hydration shells effectively increasing effective ion size. The propionamide phosphonic acid-functionalized channel exhibits a different trend, favoring ions with lower hydration free energies, with K + ions showing enhanced permeation. These findings highlight the critical role of ligand-ion interactions in modulating ion selectivity within LAP channels. In particular, the strong coordination exhibited by diglycolamine and propionamide phosphonic acid ligands significantly influences the ion transport energetics and selectivity profiles.

hydration↗
DOE OSTI2017

MOF-Sensitized Solar Cells Enabled by a Pillared Porphyrin Framework

Metal–organic frameworks (MOFs) are highly ordered, functionally tunable supramolecular materials with the potential to improve dye-sensitized solar cells (DSSCs). Several recent reports have indicated that photocurrent can be generated in Grätzel-type DSSC devices when MOFs are used as the sensitizer. However, the specific role(s) of the incorporated MOFs and the potential influence of residual MOF precursor species on device performance are unclear. Herein, we describe the assembly and characterization of a simplified DSSC platform in which isolated MOF crystals are used as the sensitizer in a planar device architecture. We selected a pillared porphyrin framework (PPF) as the MOF sensitizer, taking particular care to avoid contamination from light-absorbing MOF precursors. Photovoltaic and electrochemical characterization under simulated 1-sun and wavelength-selective illumination revealed photocurrent generation that is clearly ascribable to the PPF MOF. In conclusion, continued refinement of highly versatile MOF structure and chemistry holds promise for dramatic improvements in emerging photovoltaic technologies.

14 SOLAR ENERGY↗
DOE OSTI2022

Dehydrogenation of Propane and n -Butane Catalyzed by Isolated PtZn 4 Sites Supported on Self-Pillared Zeolite Pentasil Nanosheets

Propene and 1,3-butadiene are important building-block chemicals that can be produced by dehydrogenation of propane and butane over Pt catalysts. The challenge is to develop highly active and selective catalysts that are resistant to deactivation by Pt sintering and coke formation. We have recently shown that these objectives can be met for propane dehydrogenation using atomically dispersed Pt atoms anchored to neighboring ≡SiOZn-OH groups bonded to the framework dealuminated zeolite BEA. In the present study, we demonstrate that significantly superior performance can be achieved by using self-pillared pentasil (SPP) zeolite nanosheets. Following catalyst reduction in H 2 , atomic-resolution, scanning transmission electron microscopy (STEM) and X-ray absorption spectroscopy (XAS) indicate that Pt is stabilized in structures well approximated as (≡Si-O-Zn) 4-5 Pt. These species are highly active, selective, and stable for propane dehydrogenation (PDH) to give propene and for n-butane dehydrogenation (BDH) to give 1,3-butadiene. No catalyst deactivation was observed after 12 days of time on stream, and the selectivity remained at nearly 100% for PDH conducted at 823 K and a weight hourly space velocity (WHSV) of 1,350 h -1 . The apparent rate coefficient for PDH over this catalyst is significantly higher than that reported previously for Pt-containing catalysts. For BDH at 823 K and a WHSV of 3560 h -1 , the selectivity to butene isomers and 1,3-butadiene is 98.9%, and the selectivity to 1,3-butadiene is 45%. Here, we propose that the high catalyst stability observed during PDH and BDH is a consequence of a large fraction of the Pt-containing centers being located on the external surface of the zeolite nanosheets, where nascent coke precursors can desorb before condensing to form coke.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗