Search NASA⌕ Search

SEARCH · Search NASA

Results for “synthesis (scalable processing)”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Continuous injection synthesis of indium arsenide quantum dots emissive in the short-wavelength infrared

With the emergence of applications based on short-wavelength infrared light, indium arsenide quantum dots are promising candidates to address existing shortcomings of other infrared-emissive nanomaterials. However, III–V quantum dots have historically struggled to match the high-quality optical properties of II–VI quantum dots. Here we present an extensive investigation of the kinetics that govern indium arsenide nanocrystal growth. Based on these insights, we design a synthesis of large indium arsenide quantum dots with narrow emission linewidths. We further synthesize indium arsenide-based core-shell-shell nanocrystals with quantum yields up to 82% and improved photo- and long-term storage stability. We then demonstrate non-invasive through-skull fluorescence imaging of the brain vasculature of murine models, and show that our probes exhibit 2–3 orders of magnitude higher quantum yields than commonly employed infrared emitters across the entire infrared camera sensitivity range. Finally, we anticipate that these probes will not only enable new biomedical imaging applications, but also improved infrared nanocrystal-LEDs and photon-upconversion technology.

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

Scaling relationships and theory for vibrational frequencies of adsorbates on transition metal surfaces

Adsorbate vibrational excitations are an important fingerprint of molecule/surface interactions, affecting temperature contributions to the free energy and impacting reaction rate and equilibrium constants. Furthermore, vibrational spectra aid in identifying species and adsorption sites present in experimental studies. Despite their importance, knowledge of how adsorbate frequencies scale across materials is lacking. Here, by combining previously reported experimental data and our own density-functional theory calculations, we reveal linear correlations between vibrational frequencies of adsorbates on transition metal surfaces. Through effective-medium theory, linear muffin-tin orbital theory, and the d-band model, we rationalize the squares of the frequencies to be fundamentally linear in their scaling across transition metal surfaces. We identify the adsorbate-binding energy as a descriptor for certain molecular vibrations and rigorously relate errors in frequencies to errors in adsorption energies. Here, we also discuss the impact of scaling on surface thermochemistry and adsorbate coverage.

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

Redox-switchable breathing behavior in tetrathiafulvalene-based metal–organic frameworks

Metal–organic frameworks (MOFs) that respond to external stimuli such as guest molecules, temperature, or redox conditions are highly desirable. Herein, we coupled redox-switchable properties with breathing behavior induced by guest molecules in a single framework. Guided by topology, two flexible isomeric MOFs, compounds 1 and 2, with a formula of In(Me 2 NH 2 ) (TTFTB), were constructed via a combination of [In(COO) 4 ]- metal nodes and tetratopic tetrathiafulvalene-based linkers (TTFTB). The two compounds show different breathing behaviors upon the introduction of N 2 . Single-crystal X-ray diffraction, accompanied by molecular simulations, reveals that the breathing mechanism of 1 involves the bending of metal–ligand bonds and the sliding of interpenetrated frameworks, while 2 undergoes simple distortion of linkers. Reversible oxidation and reduction of TTF moieties changes the linker flexibility, which in turn switches the breathing behavior of 2. The redox-switchable breathing behavior can potentially be applied to the design of stimuli-responsive MOFs.

carbon capture↗
DOE OSTI2018

Retrosynthesis of multi–component metal-organic frameworks

Crystal engineering of metal–organic frameworks (MOFs) has allowed the construction of complex structures at atomic precision, but has yet to reach the same level of sophistication as organic synthesis. The synthesis of complex MOFs with multiple organic and/or inorganic components is ultimately limited by the lack of control over framework assembly in one-pot reactions. Herein, we demonstrate that multi-component MOFs with unprecedented complexity can be constructed in a predictable and stepwise manner under simple kinetic guidance, which conceptually mimics the retrosynthetic approach utilized to construct complicated organic molecules. Four multi-component MOFs were synthesized by the subsequent incorporation of organic linkers and inorganic clusters into the cavity of a mesoporous MOF, each composed of up to three different metals and two different linkers. Furthermore, we demonstrated the utility of such a retrosynthetic design through the construction of a cooperative bimetallic catalytic system with two collaborative metal sites for three-component Strecker reactions.

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

Myths and reality of HPbI 3 in halide perovskite solar cells

All-inorganic perovskites have a special place in halide perovskite family because of their potential for better stability. However, the representative cesium lead iodide (CsPbI 3 ) is metastable and spontaneously converts to the non-perovskite structure at room temperature. Here, we demonstrate that what appears to be all-inorganic CsPbI 3 stabilized in its perovskite form using the purported intermediate known as hydrogen lead iodide (HPbI 3 ) is, in fact, the hybrid perovskite cesium dimethylammonium lead iodide (Cs 1-x DMA x PbI 3 , x = 0.2 to 0.5). Thus, many of the reported all-inorganic perovskites are actually still hybrid organic-inorganic perovskites, as strongly evidenced by a wide battery of experimental techniques presented here. Solar cells based on the representative composition Cs 0.7 DMA 0.3 PbI 3 can achieve an average power conversion efficiency of 9.27 ± 1.28% (max 12.62%). These results provide an alternative angle to look at previous results pertaining all-inorganic CsPbI 3 while the DMA cation is now revealed as an alternative A site cation.

14 SOLAR ENERGY↗
DOE OSTI2018

Passive directional sub-ambient daytime radiative cooling

Demonstrations of passive daytime radiative cooling have primarily relied on complex and costly spectrally selective nanophotonic structures with high emissivity in the transparent atmospheric spectral window and high reflectivity in the solar spectrum. Here, we show a directional approach to passive radiative cooling that exploits the angular confinement of solar irradiation in the sky to achieve sub-ambient cooling during the day regardless of the emitter properties in the solar spectrum. We experimentally demonstrate this approach using a setup comprising a polished aluminum disk that reflects direct solar irradiation and a white infrared-transparent polyethylene convection cover that minimizes diffuse solar irradiation. Measurements performed around solar noon show a minimum temperature of 6 °C below ambient temperature and maximum cooling power of 45 W m –2 . Our passive cooling approach, realized using commonly available low-cost materials, could improve the performance of existing cooling systems and enable next-generation thermal management and refrigeration solutions.

14 SOLAR ENERGY↗
DOE OSTI2019

Thermal radiation control from hot graphene electrons coupled to a photonic crystal nanocavity

Controlling thermal radiation is central in a range of applications including sensing, energy harvesting, and lighting. The thermal emission spectrum can be strongly modified through the electromagnetic local density of states (EM LDOS) in nanoscale-patterned metals and semiconductors. However, these materials become unstable at high temperature, preventing improvements in radiative efficiency and applications such as thermophotovoltaics. Here, we report stable high-temperature thermal emission based on hot electrons (>2000 K) in graphene coupled to a photonic crystal nanocavity, which strongly modifies the EM LDOS. The electron bath in graphene is highly decoupled from lattice phonons, allowing a comparatively cool temperature (700 K) of the photonic crystal nanocavity. This thermal decoupling of hot electrons from the LDOS-engineered substrate opens a broad design space for thermal emission control that would be challenging or impossible with heated nanoscale-patterned metals or semiconductor materials.

14 SOLAR ENERGY↗
DOE OSTI2019

Discovery of TaFeSb-based half-Heuslers with high thermoelectric performance

Discovery of thermoelectric materials has long been realized by the Edisonian trial and error approach. However, recent progress in theoretical calculations, including the ability to predict structures of unknown phases along with their thermodynamic stability and functional properties, has enabled the so-called inverse design approach. Compared to the traditional materials discovery, the inverse design approach has the potential to substantially reduce the experimental efforts needed to identify promising compounds with target functionalities. By adopting this approach, here we have discovered several unreported half-Heusler compounds. Among them, the p-type TaFeSb-based half-Heusler demonstrates a record high ZT of ~1.52 at 973 K. Additionally, an ultrahigh average ZT of ~0.93 between 300 and 973 K is achieved. Such an extraordinary thermoelectric performance is further verified by the heat-to-electricity conversion efficiency measurement and a high efficiency of ~11.4% is obtained. Our work demonstrates that the TaFeSb-based half-Heuslers are highly promising for thermoelectric power generation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

High-throughput screening for discovery of benchtop separations systems for selected rare earth elements

Abstract Rare earth (RE) elements (scandium, yttrium, and the lanthanides) are critical for their role in sustainable energy technologies. Problems with their supply chain have motivated research to improve separations methods to recycle these elements from end of life technology. Toward this goal, we report the synthesis and characterization of the ligand tris[(1-hydroxy-2-oxo-1,2-dihydropyridine-3-carboxamido)ethyl]amine, H 3 1·TFA (TFA = trifluoroacetic acid), and complexes 1·RE (RE = La, Nd, Dy). A high-throughput experimentation (HTE) screen was developed to quantitatively determine the precipitation of 1·RE as a function of pH as well as equivalents of H 3 1·TFA. This method rapidly determines optimal conditions for the separation of RE mixtures, while minimizing materials consumption. The HTE-predicted conditions are used to achieve the lab-scale separation of Nd/Dy ( SF Nd/Dy = 213 ± 34) and La/Nd ( SF La/Nd = 16.2 ± 0.2) mixtures in acidic aqueous media.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Controlling Directionality and Dimensionality of Radiation by Perturbing Separable Bound States in the Continuum

Here, a bound state in the continuum (BIC) is an unusual localized state that is embedded in a continuum of extended states. Here, we present the general condition for BICs to arise from wave equation separability. Then we show that by exploiting perturbations of certain symmetry such BICs can be turned into resonances that radiate with a tailorable directionality and dimensionality. Using this general framework, we construct new examples of separable BICs and resonances that can exist in optical potentials for ultracold atoms, photonic systems, and systems described by tight binding. Such resonances with easily reconfigurable radiation allow for applications such as the storage and release of waves at a controllable rate and direction, as well systems that switch between different dimensions of confinement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗