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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 1,045 records · Page 58
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

A Molecular Surface Functionalization Approach to Tuning Nanoparticle Electrocatalysts for Carbon Dioxide Reduction

Conversion of the greenhouse gas carbon dioxide (CO 2 ) to value-added products is an important challenge for sustainable energy research, and nanomaterials offer a broad class of heterogeneous catalysts for such transformations. Here we report a molecular surface functionalization approach to tuning gold nanoparticle (Au NP) electrocatalysts for reduction of CO 2 to CO. The N -heterocyclic (NHC) carbene-functionalized Au NP catalyst exhibits improved faradaic efficiency (FE = 83%) for reduction of CO 2 to CO in water at neutral pH at an overpotential of 0.46 V with a 7.6-fold increase in current density compared to that of the parent Au NP (FE = 53%). Tafel plots of the NHC carbene-functionalized Au NP (72 mV/decade) vs parent Au NP (138 mV/decade) systems further show that the molecular ligand influences mechanistic pathways for CO 2 reduction. The results establish molecular surface functionalization as a complementary approach to size, shape, composition, and defect control for nanoparticle catalyst design.

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

Atomic Linkage Flexibility Tuned Isotropic Negative, Zero, and Positive Thermal Expansion in MZrF 6 (M = Ca, Mn, Fe, Co, Ni, and Zn)

The controllable isotropic thermal expansion with a broad coefficient of thermal expansion (CTE) window is intriguing but remains challenge. Herein we report a cubic MZrF 6 series (M = Ca, Mn, Fe, Co, Ni and Zn), which exhibit controllable thermal expansion over a wide temperature range and with a broader CTE window (–6.69 to +18.23 × 10 –6 /K). In particular, an isotropic zero thermal expansion (ZTE) is achieved in ZnZrF 6 , which is one of the rarely documented hightemperature isotropic ZTE compounds. By utilizing temperature dependent high-energy synchrotron X-ray total scattering diffraction, it is found that the flexibility of metal···F atomic linkages in MZrF 6 plays a critical role in distinct thermal expansions. The flexible metal···F atomic linkages induce negative thermal expansion (NTE) for CaZrF 6 , whereas the stiff ones bring positive thermal expansion (PTE) for 6. Thermal expansion could be transformed from striking negative, to zero, and finally to considerable positive though tuning the flexibility of metal···F atomic linkages by substitution with a series of cations on M sites of MZrF 6 . In conclusion, the present study not only extends the scope of NTE families and rare high-temperature isotropic ZTE compounds but also proposes a new method to design systematically controllable isotropic thermal expansion frameworks from the perspective of atomic linkage flexibility.

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

Fine-Tuning the Activity of Metal–Organic Framework Supported Cobalt Catalysts for the Oxidative Dehydrogenation of Propane

Few-atom cobalt-oxide clusters, when dispersed on a Zr-based metal–organic framework (MOF) NU-1000, have previously been shown to be active for the oxidative dehydrogenation (ODH) of propane at low temperatures (< 230 °C), affording a selective and stable propene production catalyst. In our current work, a series of promoter ions with varying Lewis acidity, including Ni(II), Zn(II), Al(III), Ti(IV) and Mo(VI), are anchored as metal-oxide,hydroxide clusters to NU-1000 via SIM (solvothermal deposition within MOFs–specifically the nodes) followed by incorporation of Co(II) ions via vapor-phase AIM (atomic layer deposition (ALD) in MOFs). This process yields a series of NU-1000-supported bimetallic-oxo,hydroxo,aqua clusters. Using difference envelope density (DED) analyses, the spatial locations of the promoter ions and catalytic cobalt ions are determined. For all samples the SIM-anchored promoter ions are sited between pairs of Zr 6 nodes along the MOF c-axis (channel-aligned axis) whereas the location of the AIM-anchored cobalt ions varies depending on the identity of promoter metal ion. With Ni(II)-, Al(III)-, or Ti(IV)-containing clusters as promoters, the oxy-cobalt species are sited atop the promoter sites; with Mo(VI) they grow exclusively on the MOF nodes sites (hexa-Zr(IV)- oxo,hydroxo,aqua units); with Zn(II) they grow on both the node and promoter. The NU-1000- supported bimetallic-oxide clusters are active for propane ODH after thermal activation under O 2 to open a cobalt coordination site and to oxidize Co(II) to Co(III), as evidenced by operando Xray absorption spectroscopy at the Co K-edge. The cobalt component is exclusively responsible for the observed catalysis. In accord with the decreasing Lewis acidity of the promoter ion, catalytic activity increases in the order: Mo(VI)<Ti(IV)<Al(III)<Zn(II)<Ni(II). The finding is attributed to increasing ease of formation Co(III)-O• species and stabilization of a cobalt(III)- oxyl/propane transition state as the Lewis acidity of the promoter ions decreases. (The promoterfree catalyst is sited on the oxy-Zr(IV) node of the MOF and is inferior catalytically to the strongly promoted versions of the catalyst.) The relative Lewis acidities of the promoters are inferred from the initial pKa values of aqua complexes of the corresponding single metal ions. Departures from the (ODH-rate)/(promoter-pKa) correlation are paralleled by differences in cobalt catalyst siting or structure. The combined results point to an increasing ability to fine-tune, with close to atomic specificity, the structure-dependent activity of MOF-supported heterogeneous catalysts for gas phase chemical reactions. When coupled with mechanistic studies–computational or experimental–this ability may translate into informed prediction of improved catalysts for propane ODH and other chemical reactions.

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

Reticular Electronic Tuning of Porphyrin Active Sites in Covalent Organic Frameworks for Electrocatalytic Carbon Dioxide Reduction

Here, the electronic character of porphyrin active sites for electrocatalytic reduction of CO 2 to CO in a two-dimensional covalent organic framework (COF) was tuned by modification of the reticular structure. Efficient charge transport along the COF backbone promotes electronic connectivity between remote functional groups and the active sites and enables the modulation of the catalytic properties of the system. A series of oriented thin films of these COFs was found to reduce CO 2 to CO at low overpotential (550 mV) with high selectivity (faradaic efficiency of 87%) and at high current densities (65 mA/mg), a performance well beyond related molecular catalysts in regard to selectivity and efficiency. The catalysts are stable for more than 12 h without any loss in reactivity. X-ray absorption measurements on the cobalt L-edge for the modified COFs enable correlations between the inductive effects of the appended functionality and the electronic character of the reticulated molecular active sites.

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

Tuning the Redox Activity of Metal–Organic Frameworks for Enhanced, Selective O 2 Binding: Design Rules and Ambient Temperature O 2 Chemisorption in a Cobalt–Triazolate Framework

Metal–organic frameworks (MOFs) with coordinatively unsaturated metal sites are appealing as adsorbent materials due to their tunable functionality and ability to selectively bind small molecules. Through the use of computational screening methods based on periodic density functional theory, we investigate O 2 and N 2 adsorption at the coordinatively unsaturated metal sites of several MOF families. A variety of design handles are identified that can be used to modify the redox activity of the metal centers, including changing the functionalization of the linkers (replacing oxido donors with sulfido donors), anion exchange of bridging ligands (considering μ-Br – , μ-Cl – , μ-F – , μ-SH – , or μ-OH – groups), and altering the formal oxidation state of the metal. As a result, we show that it is possible to tune the O 2 affinity at the open metal sites of MOFs for applications involving the strong and/or selective binding of O 2 . In contrast with O 2 adsorption, N 2 adsorption at open metal sites is predicted to be relatively weak across the MOF dataset, with the exception of MOFs containing synthetically elusive V 2+ open metal sites. As one example from the screening study, we predicted that exchanging the μ-Cl – ligands of M 2 Cl 2 (BBTA) (H 2 BBTA = 1H,5H-benzo(1,2-d:4,5-d')bistriazole) with μ-OH – groups would significantly enhance the strength of O 2 adsorption at the open metal sites without a corresponding increase in the N 2 affinity. Experimental investigation of Co 2 Cl 2 (BBTA) and Co 2 (OH) 2 (BBTA) confirms that the former exhibits weak physisorption of both N 2 and O 2 , whereas the latter is capable of chemisorbing O 2 at room temperature in a highly selective manner. The O 2 chemisorption behavior is attributed to the greater electron-donating character of the μ-OH – ligands and the presence of H-bonding interactions between the μ-OH – bridging ligands and the reduced O 2 adsorbate.

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

Ions Tune Interfacial Water Structure and Modulate Hydrophobic Interactions at Silica Surfaces

The structure and ultrafast dynamics of the electric double layer (EDL) are central to chemical reactivity and physical properties at solid/aqueous interfaces. While the Gouy–Chapman–Stern model is widely used to describe EDLs, it is solely based on the macroscopic electrostatic attraction of electrolytes for the charged surfaces. Structure and dynamics in the Stern layer are, however, more complex because of competing effects due to the localized surface charge distribution, surface–solvent–ion correlations, and the interfacial hydrogen bonding environment. Here, we report combined time-resolved vibrational sum frequency generation (TR-vSFG) spectroscopy with ab initio DFT-based molecular dynamics simulations (AIMD/DFT-MD) to get direct access to the molecular-level understanding of how ions change the structure and dynamics of the EDL. We show that innersphere adsorbed ions tune the hydrophobicity of the silica–aqueous interface by shifting the structural makeup in the Stern layer from dominant water–surface interactions to water–water interactions. This drives an initially inhomogeneous interfacial water coordination landscape observed at the neat interface toward a homogeneous, highly interconnected in-plane 2D hydrogen bonding (2D-HB) network at the ionic interface, reminiscent of the canonical, hydrophobic air–water interface. This ion-induced transformation results in a characteristic decrease of the vibrational lifetime (T 1 ) of excited interfacial O–H stretching modes from T 1 ~ 600 fs to T 1 ~ 250 fs. Hence, we propose that the T 1 determined by TR-vSFG in combination with DFT-MD simulations can be widely used for a quantitative spectroscopic probe of the ion kosmotropic/chaotropic effect at aqueous interfaces as well as of the ion-induced surface hydrophobicity.

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

Morphology and Activity Tuning of Cu 3 Pt/C Ordered Intermetallic Nanoparticles by Selective Electrochemical Dealloying

Improving the catalytic activity of Pt-based bimetallic nanoparticles is a key challenge in the application of proton-exchange membrane fuel cells. Electrochemical dealloying represents a powerful approach for tuning the surface structure and morphology of these catalyst nanoparticles. We present a comprehensive study of using electrochemical dealloying methods to control the morphology of ordered Cu 3 Pt/C intermetallic nanoparticles, which could dramatically affect their electrocatalytic activity for the oxygen reduction reaction (ORR). Depending on the electrochemical dealloying conditions, the nanoparticles with Pt-rich core–shell or porous structures were formed. We further demonstrate that the core–shell and porous morphologies can be combined to achieve the highest ORR activity. Lastly, this strategy provides new guidelines for optimizing nanoparticles synthesis and improving electrocatalytic activity.

36 MATERIALS SCIENCE↗
DOE OSTI2022

The Global Atmosphere‐aerosol Model ICON‐A‐HAM2.3–Initial Model Evaluation and Effects of Radiation Balance Tuning on Aerosol Optical Thickness

Abstract The Hamburg Aerosol Module version 2.3 (HAM2.3) from the ECHAM6.3‐HAM2.3 global atmosphere‐aerosol model is coupled to the recently developed icosahedral nonhydrostatic ICON‐A (icon‐aes‐1.3.00) global atmosphere model to yield the new ICON‐A‐HAM2.3 atmosphere‐aerosol model. The ICON‐A and ECHAM6.3 host models use different dynamical cores, parameterizations of vertical mixing due to sub‐grid scale turbulence, and parameter settings for radiation balance tuning. Here, we study the role of the different host models for simulated aerosol optical thickness (AOT) and evaluate impacts of using HAM2.3 and the ECHAM6‐HAM2.3 two‐moment cloud microphysics scheme on several meteorological variables. Sensitivity runs show that a positive AOT bias over the subtropical oceans is remedied in ICON‐A‐HAM2.3 because of a different default setting of a parameter in the moist convection parameterization of the host models. The global mean AOT is biased low compared to MODIS satellite instrument retrievals in ICON‐A‐HAM2.3 and ECHAM6.3‐HAM2.3, but the bias is larger in ICON‐A‐HAM2.3 because negative AOT biases over the Amazon, the African rain forest, and the northern Indian Ocean are no longer compensated by high biases over the sub‐tropical oceans. ICON‐A‐HAM2.3 shows a moderate improvement with respect to AOT observations at AERONET sites. A multivariable bias score combining biases of several meteorological variables into a single number is larger in ICON‐A‐HAM2.3 compared to standard ICON‐A and standard ECHAM6.3. In the tropics, this multivariable bias is of similar magnitude in ICON‐A‐HAM2.3 and in ECHAM6.3‐HAM2.3. In the extra‐tropics, a smaller multivariable bias is found for ICON‐A‐HAM2.3 than for ECHAM6.3‐HAM2.3.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2017

Tuning nanoparticle size for enhanced functionality in perovskite thin films deposited by metal organic deposition

Because of pressing global environmental challenges, focus has been placed on materials for efficient energy use, and this has triggered the search for nanostructural modification methods to improve performance. Achieving a high density of tunable-sized second-phase nanoparticles while ensuring the matrix remains intact is a long-sought goal. In this paper, we present an effective, scalable method to achieve this goal using metal organic deposition in a perovskite system REBa 2 Cu 3 O 7 (rare earth (RE)) that enhances the superconducting properties to surpass that of previous achievements. We present two industrially compatible routes to tune the nanoparticle size by controlling diffusion during the nanoparticle formation stage by selecting the second-phase material and modulating the precursor composition spatially. Combining these routes leads to an extremely high density (8 × 10 22 m -3 ) of small nanoparticles (7 nm) that increase critical currents and reduce detrimental effects of thermal fluctuations at all magnetic field strengths and temperatures. This method can be directly applied to other perovskite materials where nanoparticle addition is beneficial.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Tuning fresh: radiation through rewiring of central metabolism in streamlined bacteria

Most free-living planktonic cells are streamlined and in spite of their limitations in functional flexibility, their vast populations have radiated into a wide range of aquatic habitats. Here we compared the metabolic potential of subgroups in the Alphaproteobacteria lineage SAR11 adapted to marine and freshwater habitats. Our results suggest that the successful leap from marine to freshwaters in SAR11 was accompanied by a loss of several carbon degradation pathways and a rewiring of the central metabolism. Examples for these are C1 and methylated compounds degradation pathways, the Entner-Doudouroff pathway, the glyoxylate shunt and anapleuretic carbon fixation being absent from the freshwater genomes. Evolutionary reconstruc tions further suggest that the metabolic modules making up these important freshwater metabolic traits were already present in the gene pool of ancestral marine SAR11 populations. The loss of the glyoxylate shunt had already occurred in the common ancestor of the freshwater subgroup and its closest marine relatives, suggesting that the adaptation to freshwater was a gradual process. Furthermore, our results indicate rapid evolution of TRAP transporters in the freshwater clade involved in the uptake of low molecular weight carboxylic acids. We propose that such gradual tuning of metabolic pathways and transporters toward locally available organic substrates is linked to the formation of subgroups within the SAR11 clade and that this process was critical for the freshwater clade to find and fix an adaptive phenotype.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Tuning the catalytic CO hydrogenation to straight- and long-chain aldehydes/alcohols and olefins/paraffins

Here, the catalytic CO hydrogenation is one of the most versatile large-scale chemical syntheses leading to variable chemical feedstock. While traditionally mainly methanol and long-chain hydrocarbons are produced by CO hydrogenation, here we show that the same reaction can be tuned to produce long-chain n-aldehydes, 1-alcohols and olefins, as well as n-paraffins over potassium-promoted CoMn catalysts. The sum selectivity of aldehydes and alcohols is usually >50 wt% whereof up to ~97% can be n-aldehydes. While the product slate contains ~60% n-aldehydes at /p CO =0.5, a 65/35% slate of paraffins/alcohols is obtained at a ratio of 9. A linear Anderson–Schulz–Flory behaviour, independent of the /p CO ratio, is found for the sum of C 4+ products. We advocate a synergistic interaction between a Mn 5 O 8 oxide and a bulk Co 2 C phase, promoted by the presence of potassium, to be responsible for the unique product spectra in our studies.

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

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the band edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. As a result, we expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Community-integrated omics links dominance of a microbial generalist to fine-tuned resource usage

Microbial communities are complex and dynamic systems that are primarily structured according to their members’ ecological niches. To investigate how niche breadth (generalist versus specialist lifestyle strategies) relates to ecological success, we develop and apply an integrative workflow for the multi-omic analysis of oleaginous mixed microbial communities from a biological wastewater treatment plant. Time- and space-resolved coupled metabolomic and taxonomic analyses demonstrate that the community-wide lipid accumulation phenotype is associated with the dominance of the generalist bacterium Candidatus Microthrix spp. By integrating population-level genomic reconstructions (reflecting fundamental niches) with transcriptomic and proteomic data (realised niches), we identify finely tuned gene expression governing resource usage by Candidatus Microthrix parvicella over time. Moreover, our results indicate that the fluctuating environmental conditions constrain the accumulation of genetic variation in Candidatus Microthrix parvicella likely due to fitness trade-offs. Based on our observations, niche breadth has to be considered as an important factor for understanding the evolutionary processes governing (microbial) population sizes and structures in situ.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces

Optical metasurfaces are regular quasi-planar nanopatterns that can apply diverse spatial and spectral transformations to light waves. But, metasurfaces are no longer adjustable after fabrication, and a critical challenge is to realise a technique of tuning their optical properties that is both fast and efficient. Here, we experimentally realise an ultrafast tunable metasurface consisting of subwavelength gallium arsenide nanoparticles supporting Mie-type resonances in the near infrared. In using transient reflectance spectroscopy, we demonstrate a picosecond-scale absolute reflectance modulation of up to 0.35 at the magnetic dipole resonance of the metasurfaces and a spectral shift of the resonance by 30 nm, both achieved at unprecedentedly low pump fluences of less than 400 μJ cm –2 . Our findings thereby enable a versatile tool for ultrafast and efficient control of light using light.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Giant magnetoelectric effects achieved by tuning spin cone symmetry in Y-type hexaferrites

Multiferroics materials, which exhibit coupled magnetic and ferroelectric properties, have attracted tremendous research interest because of their potential in constructing next-generation multifunctional devices. The application of single-phase multiferroics is currently limited by their usually small magnetoelectric effects. Here, we report the realization of giant magnetoelectric effects in a Y-type hexaferrite Ba 0.4 Sr 1.6 Mg 2 Fe 12 O 22 single crystal, which exhibits record-breaking direct and converse magnetoelectric coefficients and a large electric-field-reversed magnetization. We have uncovered the origin of the giant magnetoelectric effects by a systematic study in the Ba 2-x Sr x Mg 2 Fe 12 O 22 family with magnetization, ferroelectricity and neutron diffraction measurements. With the transverse spin cone symmetry restricted to be two-fold, the one-step sharp magnetization reversal is realized and giant magnetoelectric coefficients are achieved. Our study reveals that tuning magnetic symmetry is an effective route to enhance the magnetoelectric effects also in multiferroic hexaferrites.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Carrier density and disorder tuned superconductor-metal transition in a two-dimensional electron system

Quantum ground states that arise at atomically controlled oxide interfaces provide an opportunity to address key questions in condensed matter physics, including the nature of two-dimensional metallic behaviour often observed adjacent to superconductivity. At the superconducting LaAlO 3 /SrTiO 3 interface, a metallic ground state emerges upon the collapse of superconductivity with field-effect gating and is accompanied with a pseudogap. Here we utilize independent control of carrier density and disorder of the interfacial superconductor using dual electrostatic gates, which enables the comprehensive examination of the electronic phase diagram approaching zero temperature. We find that the pseudogap corresponds to precursor pairing, and the onset of long-range phase coherence forms a two-dimensional superconducting dome as a function of the dual-gate voltages. In conclusion, the gate-tuned superconductor–metal transitions are driven by macroscopic phase fluctuations of Josephson coupled superconducting puddles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Two-dimensional transition metal carbides as supports for tuning the chemistry of catalytic nanoparticles

Supported nanoparticles are broadly employed in industrial catalytic processes, where the active sites can be tuned by metal-support interactions (MSIs). Although it is well accepted that supports can modify the chemistry of metal nanoparticles, systematic utilization of MSIs for achieving desired catalytic performance is still challenging. The developments of supports with appropriate chemical properties and identification of the resulting active sites are the main barriers. Here, we develop two-dimensional transition metal carbides (MXenes) supported platinum as efficient catalysts for light alkane dehydrogenations. Ordered Pt 3 Ti and surface Pt 3 Nb intermetallic compound nanoparticles are formed via reactive metal-support interactions on Pt/Ti 3 C 2 T x and Pt/Nb 2 CT x catalysts, respectively. MXene supports modulate the nature of the active sites, making them highly selective toward C–H activation. Such exploitation of the MSIs makes MXenes promising platforms with versatile chemical reactivity and tunability for facile design of supported intermetallic nanoparticles over a wide range of compositions and structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Tuning high- Q nonlinear dynamics in a disordered quantum magnet

Quantum states cohere and interfere. Atoms arranged imperfectly in a solid rarely display these properties. Here we demonstrate an exception in a disordered quantum magnet that divides itself into nearly isolated subsystems. We probe these coherent spin clusters by driving the system nonlinearly and measuring the resulting hole in the linear spectral response. The Fano shape of the hole encodes the incoherent lifetime as well as coherent mixing of the localized excitations. For the Ising magnet LiHo 0.045 Y 0.955 F 4 , the quality factor Q for spectral holes can be as high as 100,000. We tune the dynamics by sweeping the Fano mixing parameter q through zero via the ac pump amplitude as well as a dc transverse field. The zero crossing of q is associated with a dissipationless response at the drive frequency. Identifying localized two-level systems in a dense and disordered magnet advances the search for qubit platforms emerging from strongly interacting, many-body systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗