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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 361 records · Page 20
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Ambient Synthesis of Single‐Atom Catalysts from Bulk Metal via Trapping of Atoms by Surface Dangling Bonds

Abstract Single‐atom catalysts (SACs) feature the maximum atom economy and superior performance for various catalysis fields, attracting tremendous attention in materials science. However, conventional synthesis of SACs involves high energy consumption at high temperature, complicated procedures, a massive waste of metal species, and poor yields, greatly impeding their development. Herein, a facile dangling bond trapping strategy to construct SACs under ambient conditions from easily accessible bulk metals (such as Fe, Co, Ni, and Cu) is presented. When mixing graphene oxide (GO) slurry with metal foam and drying in ambient conditions, the M 0 would transfer electrons to the dangling oxygen groups on GO, obtaining M δ+ (0 < δ < 3) species. Meanwhile, M δ+ coordinates with the surface oxygen dangling bonds of GO to form MO bonds. Subsequently, the metal atoms are pulled out of the metal foam by the MO bonds under the assistance of sonication to give M SAs/GO materials. This synthesis at room temperature from bulk metals provides a versatile platform for facile and low‐cost fabrication of SACs, crucial for their mass production and practical application in diverse industrial reactions.

Qu, Yunteng↗
DOE OSTI2023

Atomically Dispersed Silver Atoms Embedded in NiCo Layer Double Hydroxide Boost Oxygen Evolution Reaction

Abstract Bimetallic layered double hydroxides (LDHs) are promising catalysts for anodic oxygen evolution reaction (OER) in alkaline media. Despite good stability, NiCo LDH displays an unsatisfactory OER activity relative to the most robust NiFe LDH and CoFe LDH. Herein, a novel NiCo LDH electrocatalyst modified with single‐atom silver grown on carbon cloth (Ag SA ‐NiCo LDH/CC) that exhibits exceptional OER activity and stability in 1.0 m KOH is reported. The Ag SA ‐NiCo LDH/CC catalyst only requires a low overpotential of 192 mV to reach a current density of 10 mA cm −2 , obviously boosting the OER activity of NiCo LDH/CC (410 mV@10 mA cm −2 ). Inspiringly, Ag SA ‐NiCo LDH/CC can maintain its high activity for up to 500 h at a large current density of 100 mA cm −2 , exceeding most single‐atom OER catalysts. In situ Raman spectroscopy studies uncover that the in situ formed NiCoOOH during OER is the real active species. Hard X‐ray absorption spectrum (XAS) and density functional theory (DFT) calculations validate that single‐atom Ag occupying Ni site increases the chemical valence of Ni elements, and then weakens the adsorption of oxygen‐contained intermediates on Ni sites, fundamentally accounting for the enhanced OER performance.

Chemistry↗
DOE OSTI2021

H-Atom Assignment and Sb–O Bonding of [Mes 3 SbOH][O 3 SPh] Confirmed by Neutron Diffraction, Multipole Modeling, and Hirshfeld Atom Refinement

Neutron wavelength-resolved Laue diffraction experiments permit accurate refinement of the H-atom positions and anisotropic displacement parameters of [Mes 3 SbOH][O 3 SPh]. A multipole-based charge density refinement and a topological analysis of the refined electron density were also performed. Hirshfeld atom refinement (HAR) recovers the neutron-determined H-atom parameters, and the quantum-mechanical electron density used in HAR recovers the electron density topology from the refined multipole model. We report these results confirm that [Mes 3 SbOH][O 3 SPh] does indeed feature a hydroxystibonium cation with a nominal Sb–O single bond and not a stibine oxide with an Sb=O/Sb + –O – bond.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Cation-poor complex metallic alloys in Ba(Eu)–Au–Al(Ga) systems: Identifying the keys that control structural arrangements and atom distributions at the atomic level

Four complex intermetallic compounds BaAu 6±x Ga 6±y (x = 1, y = 0.9) (I), BaAu 6±x Al 6±y (x = 0.9, y = 0.6) (II), EuAu 6.2 Ga 5.8 (III), and EuAu 6.1 Al 5.9 (IV) have been synthesized, and their structures and homogeneity ranges have been determined by single crystal and powder X-ray diffraction. Whereas I and II originate from the NaZn 13 -type structure (cF104–112, Fm3C), III (tP52, P4/nbm) is derived from the tetragonal Ce 2 Ni 17 Si 9 -type, and IV (oP104, Pbcm) crystallizes in a new orthorhombic structure type. Both I and II feature formally anionic networks with completely mixed site occupation by Au and triel (Tr = Al, Ga) atoms, while a successive decrease of local symmetry from the parental structures of I and II to III and, ultimately, to IV correlates with increasing separation of Au and Tr on individual crystallographic sites. Density functional theory-based calculations were employed to determine the crystallographic site preferences of Au and the respective triel element to elucidate reasons for the atom distribution (“coloring scheme”). Chemical bonding analyses for two different “EuAu 6 Tr 6 ” models reveal maximization of the number of heteroatomic Au–Tr bonds as the driving force for atom organization. The Fermi levels fall in broad pseudogaps for both models allowing some electronic flexibility. Spin-polarized band structure calculations on the “EuAu 6 Tr 6 ” models hint to singlet ground states for europium and long-range magnetic coupling for both EuAu 6.2 Ga 5.8 (III) and EuAu 6.1 Al 5.9 (IV). This is substantiated by experimental evidence because both compounds show nearly identical magnetic behavior with ferromagnetic transitions at T C = 6 K and net magnetic moments of 7.35 μB/f.u. at 2 K. As a result, the effective moments of 8.3 μB/f.u., determined from Curie–Weiss fits, point to divalent oxidation states for europium in both III and IV.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

An Algorithm for Atom-Centered Lossy Compression of the Atomic Orbital Basis in Density Functional Theory Calculations

Large atomic-orbital (AO) basis sets of at least triple and preferably quadruple-ζ (QZ) size are required to adequately converge Kohn–Sham density functional theory (DFT) calculations toward the complete basis set limit. However, incrementing the cardinal number by one nearly doubles the AO basis dimension, and the computational cost scales as the cube of the AO dimension, so this is very computationally demanding. Here, in this work, we develop and test a threshold-based natural atomic orbital (NAO) scheme in which ϵ-NAOs are obtained as eigenfunctions of atomic blocks of the density matrix in a one-center orthogonalized representation. This enables compression of the AO basis that is optimal for a given threshold, 10 –ϵ , by discarding NAOs with occupation numbers below that threshold. Extensive pilot test calculations using the Hartree–Fock functional and taking the converged density matrix as input suggest that a threshold of 10 –5 can yield a compression factor (ratio of AO to compressed ϵ-NAO dimension) between 2.5 and 4.5 for the QZ pc-3 basis. The errors in relative energies are typically less than 0.1 kcal/mol when the compressed basis is used instead of the uncompressed basis. Between 10 and 100 times smaller errors (i.e., usually less than 0.01 kcal/mol) can be obtained with a threshold 10 –7 , while the compression factor is typically between 2 and 2.5.

basis sets↗
DOE OSTI2019

Quasi-Atomic Bond Analyses in the Sixth Period: I. Relativistic Accurate Atomic Minimal Basis Sets for the Elements Cesium to Radon

Full-valence relativistic accurate atomic minimal basis set (AAMBS) orbitals are developed for the sixth-row elements from cesium to radon, including the lanthanides. Saturated primitive atomic basis sets are developed and subsequently used to form the AAMBS orbitals. By use of a saturated basis, properties computed based on the AAMBS orbitals are basis set independent. In molecules, the AAMBS orbitals can be used to construct valence virtual orbitals (VVOs) that provide chemically meaningful abinitio lowest unoccupied molecular orbitals (LUMOs) with basis set independent orbital energies. The optimized occupied molecular orbitals complemented with the VVOs form a set of full-valence molecular orbitals. They can be transformed into a set of oriented quasi-atomic orbitals (QUAOs) that provide information on intramolecular bonding via an intrinsic density analysis. The development of the AAMBS for the sixth row is introduced in this work.

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

Improved Models for Metallic Nanoparticle Cores from Atomic Pair Distribution Function (PDF) Analysis

X-ray atomic pair distribution functions (PDFs) were collected from a range of canonical metallic nanomaterials, both elemental and alloyed, prepared using different synthesis methods and exhibiting drastically different morphological properties. Widely applied shape-tuned attenuated crystal (AC) fcc models proved inadequate, yielding structured, coherent, and correlated fit residuals. However, equally simple discrete cluster models could account for the largest amplitude features in these difference signals. A hypothesis testing based approach to nanoparticle structure modeling systematically ruled out effects from crystallite size, composition, shape, and surface faceting as primary factors contributing to the AC misfit. On the other hand, decahedrally twinned cluster cores were found to be the origin of the AC structure misfits for a majority of the nanomaterials reported here. It is further motivated that the PDF can readily differentiate between the arrangement of domains in these multiply twinned motifs. Most of the nanomaterials surveyed also fall within the sub-5 nm size regime where traditional electron microscopy cannot easily detect and quantify domain structures, with sampling representative of the average nanocrystal synthesized. Here, the results demonstrate that PDF analysis is a powerful method for understanding internal atomic interfaces in small noble metallic nanomaterials. Such core cluster models, easily built algorithmically, should serve as starting structures for more advanced models able to capture atomic positional disorder, ligand induced or otherwise, near nanocrystal surfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

High-resolution studies of the Majorana atomic chain platform

Ordered assemblies of magnetic atoms on the surface of conventional superconductors can be used to engineer topological superconducting phases and realize Majorana fermion quasiparticles (MQPs) in a condensed matter setting. Recent experiments have shown that chains of Fe atoms on Pb generically have the required electronic characteristics to form a one-dimensional topological superconductor and have revealed spatially resolved signatures of localized MQPs at the ends of such chains. Here we report higher-resolution measurements of the same atomic chain system performed using a dilution refrigerator scanning tunnelling microscope (STM). With significantly better energy resolution than previous studies, we show that the zero-bias peak (ZBP) in Fe chains has no detectable splitting from hybridization with other states. The measurements also reveal that the ZBP exhibits a distinctive ‘double eye’ spatial pattern on nanometre length scales. Theoretically we show that this is a general consequence of STM measurements of MQPs with substantial spectral weight in the superconducting substrate, a conclusion further supported by measurements of Pb overlayers deposited on top of the Fe chains. Lastly, we report experiments performed with superconducting tips in search of the particle–hole symmetric MQP signature expected in such measurements.

Electronic properties and materials↗