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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 469 records · Page 26
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Discovery of the Azaserine Biosynthetic Pathway Uncovers a Biological Route for α‐Diazoester Production

Abstract Azaserine is a bacterial metabolite containing a biologically unusual and synthetically enabling α‐diazoester functional group. Herein, we report the discovery of the azaserine ( aza ) biosynthetic gene cluster from Glycomyces harbinensis . Discovery of related gene clusters reveals previously unappreciated azaserine producers, and heterologous expression of the aza gene cluster confirms its role in azaserine assembly. Notably, this gene cluster encodes homologues of hydrazonoacetic acid (HYAA)‐producing enzymes, implicating HYAA in α‐diazoester biosynthesis. Isotope feeding and biochemical experiments support this hypothesis. These discoveries indicate that a 2‐electron oxidation of a hydrazonoacetyl intermediate is required for α‐diazoester formation, constituting a distinct logic for diazo biosynthesis. Uncovering this biological route for α‐diazoester synthesis now enables the production of a highly versatile carbene precursor in cells, facilitating approaches for engineering complete carbene‐mediated biosynthetic transformations in vivo.

Van Cura, Devon↗
DOE OSTI2015

Divergent Mechanistic Routes for the Formation of gem-Dimethyl Groups in the Biosynthesis of Complex Polyketides

The gem-dimethyl groups in polyketide-derived natural products add steric bulk and, accordingly, lend increased stability to medicinal compounds, however, our ability to rationally incorporate this functional group in modified natural products is limited. In order to characterize the mechanism of gem-dimethyl group formation, with a goal toward engineering of novel compounds containing this moiety, the gem-dimethyl group producing polyketide synthase (PKS) modules of yersiniabactin and epothilone were characterized using mass spectrometry. The work demonstrated, contrary to the canonical understanding of reaction order in PKSs, that methylation can precede condensation in gem-dimethyl group producing PKS modules. Experiments showed that both PKSs are able to use dimethylmalonyl acyl carrier protein (ACP) as an extender unit. Interestingly, for epothilone module8, use of dimethylmalonyl-ACP appeared to be the sole route to form a gem-dimethylated product, while the yersiniabactin PKS could methylate before or after ketosynthase condensation.

Poust, S↗
DOE OSTI2022

A General Route to Flame Aerosol Synthesis and In Situ Functionalization of Mesoporous Silica

Mesoporous silica is a versatile material for energy, environmental, and medical applications. In this work, for the first time, we report a flame aerosol synthesis method for a class of mesoporous silica with hollow structure and specific surface area exceeding 1000 m 2 /g -1 . We show its superior performance in water purification, drug carrier, and thermal insulation. Moreover, we propose a general route to produce mesoporous nanoshell supported nanocatalysts by in situ decorating active nanoclusters, including noble metal (Pt/SiO 2 ), transition metal (Ni/SiO 2 ), metal oxide (CrO 3 /SiO 2 ), and alumina support (Co/Al 2 O 3 ). As a prototypical application, we perform dry reforming of methane using Ni/SiO 2 , achieving constant 97% CH 4 and CO 2 conversions for more than 200 hours, dramatically outperforming MCM-41 supported Ni catalyst. This work provides a scalable strategy to produce mesoporous nanoshells and proposes an in situ functionalization mechanism to flexible catalysts design for many reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Discovery of the Azaserine Biosynthetic Pathway Uncovers a Biological Route for α‐Diazoester Production

Abstract Azaserine is a bacterial metabolite containing a biologically unusual and synthetically enabling α‐diazoester functional group. Herein, we report the discovery of the azaserine ( aza ) biosynthetic gene cluster from Glycomyces harbinensis . Discovery of related gene clusters reveals previously unappreciated azaserine producers, and heterologous expression of the aza gene cluster confirms its role in azaserine assembly. Notably, this gene cluster encodes homologues of hydrazonoacetic acid (HYAA)‐producing enzymes, implicating HYAA in α‐diazoester biosynthesis. Isotope feeding and biochemical experiments support this hypothesis. These discoveries indicate that a 2‐electron oxidation of a hydrazonoacetyl intermediate is required for α‐diazoester formation, constituting a distinct logic for diazo biosynthesis. Uncovering this biological route for α‐diazoester synthesis now enables the production of a highly versatile carbene precursor in cells, facilitating approaches for engineering complete carbene‐mediated biosynthetic transformations in vivo.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Triplet Generation Through Singlet Fission in Metal-Organic Framework: An Alternative Route to Inefficient Singlet-Triplet Intersystem Crossing

High quantum yield triplets, populated by initially prepared excited singlets, are desired for various energy conversion schemes in solid working compositions like porous MOFs. However, a large disparity in the distribution of the excitonic center of mass, singlet-triplet intersystem crossing (ISC) in such assemblies is inhibited, so much so that a carboxy-coordinated zirconium heavy metal ion cannot effectively facilitate the ISC through spin-orbit coupling. Circumventing this sluggish ISC, singlet fission (SF) is explored as a viable route to generating triplets in solution-stable MOFs. Efficient SF is achieved through a high degree of interchromophoric coupling that facilitates electron super-exchange to generate triplet pairs. Here we show that a predesigned chromophoric linker with extremely poor ISC efficiency (k ISC ) but E S 1 ≥ 2E T 1 form triplets in MOF in contrast to the frameworks that are built from linkers with sizable k ISC but E S 1 ≤ 2E T 1 . Finally, this work opens a new photophysical and photochemical avenue in MOF chemistry and utility in energy conversion schemes.

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

Neighbor-directed histidine N(τ) alkylation. A route to imidazolium-containing phosphopeptide macrocycles

Our recently discovered, selective, on-resin route to N(τ)-alkylated imidazolium-containing histidine residues affords new strategies for peptide mimetic design. In this, we demonstrate the use of this chemistry to prepare a series of macrocyclic phosphopeptides, in which imidazolium groups serve as ring-forming junctions. These cationic moieties subsequently serve to charge-mask the phosphoamino acid group that directed their formation. Furthermore, neighbor-directed histidine N(τ)-alkylation opens the door to new families of phosphopeptidomimetics for use in a range of chemical biology contexts.

cationic dialkyl histidine↗
DOE OSTI2018

Synthetic Routes to Shaped AuPt Core-Shell Particles with Smooth Surfaces Based on Design Rules for Au Nanoparticle Growth

Widespread implementation of polymer electrolyte fuel cells is limited by the performance of Pt catalysts because of the high cost of Pt and the propensity for catalyst surfaces to lose activity as a result of surface poisoning. AuPt core–shell particles show potential to address these issues, yet provide new challenges because of the immiscibility of Au and Pt during particle growth. In this work, AuPt core–shell particles with distinct shapes are made using a one-pot synthesis under mild reaction conditions by exploiting the difference in reduction rate between Au and Pt ions. Employing this approach results in smooth, well-defined surfaces, rather than the more commonly observed dendritic or island-like Pt shells that generally form when presynthesized Au cores are used to template Au-core/Pt-shell particle growth. By using the established mechanisms of Au nanoparticle growth, facile modification of particle shape and size is achieved with no significant change to the Pt surface. As a result, this approach also offers a synthetic route to the preparation of more complex AuPt nanostructures, such as those with exotic shapes and high-energy surface facets.

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

Time-dependence of the holographic spectral function: diverse routes to thermalisation

Here, we develop a new method for computing the holographic retarded propagator in generic (non-) equilibrium states using the state/geometry map. We check that our method reproduces the thermal spectral function given by the Son-Starinets prescription. The time-dependence of the spectral function of a relevant scalar operator is studied in a class of non-equilibrium states. The latter are represented by AdS-Vaidya geometries with an arbitrary parameter characterising the timescale for the dual state to transit from an initial thermal equilibrium to another due to a homogeneous quench. For long quench duration, the spectral function indeed follows the thermal form at the instantaneous effective temperature adiabatically, although with a slight initial time delay and a bit premature thermalisation. At shorter quench durations, several new non-adiabatic features appear: (i) time-dependence of the spectral function is seen much before than that in the effective temperature (advanced time-dependence), (ii) a big transfer of spectral weight to frequencies greater than the initial temperature occurs at an intermediate time (kink formation) and (iii) new peaks with decreasing amplitudes but in greater numbers appear even after the effective temperature has stabilised (persistent oscillations). We find four broad routes to thermalisation for lower values of spatial momenta. At higher values of spatial momenta, kink formations and persistent oscillations are suppressed, and thermalisation time decreases. The general thermalisation pattern is globally top-down, but a closer look reveals complexities.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2015

Acute Superior Mesenteric Venous Thrombosis: Transcatheter Thrombolysis and Aspiration Thrombectomy Therapy by Combined Route of Superior Mesenteric Vein and Artery in Eight Patients

PurposeTo assess the feasibility, effectiveness, and safety of catheter-directed thrombolysis and aspiration thrombectomy therapy by combined route of superior mesenteric vein and artery (SMV+SMA) for acute superior mesenteric venous thrombosis (ASMVT).MethodsThis retrospective study reviewed eight ASMVT patients with transcatheter direct thrombolysis and aspiration thrombectomy therapy via SMV and indirect thrombolysis via SMA during a period of 14 months. The demographics, etiology, risk factors, therapeutic effect, complications, mortality, and follow-up of the study population were assessed. Anatomic and imaging classification of location and extent of thrombus at diagnosis and degree of thrombus lysis were described.ResultsTechnical success was achieved with substantial improvement in symptoms and thrombus resolution after thrombolytic therapy in all patients. The local urokinase infusion by SMA and SMV was performed for 5–7 (6.13 ± 0.83) and 7–15 (12 ± 2.51) days. Anticoagulation was performed catheter-directed and then orally throughout hospitalization and after discharge. Four patients required delayed localized bowel resection after thrombolytic therapy with no death. Thrombolytic therapy was not interrupted despite minor bleeding at the puncture site in two patients and sepsis in another two postoperatively. Nearly complete removal of thrombus was demonstrated by contrast-enhanced CT scan and portography before discharge. Patients were discharged in 10–27 (19.25 ± 4.89) days after admission. No recurrence developed during the follow-up of 10–13 (12.13 ± 0.99) months.ConclusionsCatheter-directed thrombolytic and aspiration therapy via SMV+SMA is beneficial for ASMVT in avoiding patient death, efficient resolving thrombus, rapid improving symptoms, reversing extensive intestinal ischemia, averting bowel resection, or localizing infarcted bowel segment and preventing short bowel syndrome.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2019

Nanocomposites Based on Poly(lactic acid) and Bacterial Cellulose Acetylated by an α-Hydroxyacid Catalyzed Route

Poly(lactic acid) (PLA) nanocomposite films reinforced with acetylated bacterial cellulose nanoribbons were prepared by solvent casting. Acetylation of bacterial cellulose (BC) was performed by an innovative and sustainable direct solvent-free route catalyzed by citric acid. The effect of derivatization and its extent on the morphological, optical, thermal and mechanical properties of the nanocomposites was analyzed. Data collected from the above studies showed that acetylation of BC nanoribbons clearly improved the nanofibers dispersion in the PLA matrix with respect to unmodified BC, which in turn resulted in increased transparency and mechanical properties of the nanocomposites produced.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Effect of NaOH Concentration and Adding Sequences on Structural and Magnetic Properties of Ni{sub 0.4}Co{sub 0.6}Fe{sub 2}O{sub 4} Nanopowders Prepared Via Co-precipitation Route

Ni{sub 0.4}Co{sub 0.6}Fe{sub 2}O{sub 4} nanopowders were prepared via the co-precipitation route followed by annealing treatment. The structural and magnetic properties of the as-synthesized samples were determined by XRD, FT-IR, TG-DSC, and PPMS measurements, respectively. The XRD patterns indicated a single-phase cubic spinel structure for all the Ni-Co ferrite samples, regardless of adding sequences of the reactants or NaOH concentration. The analysis of the XRD patterns revealed that the enhancement in lattice constant with increasing NaOH concentration is related to the prevention of oxidization of Co{sup 2+} ions in the Ni-Co ferrite lattice. The FT-IR spectra indicated that samples prepared in the B process have fewer impurities than those prepared in the A process. The enhancement in saturation magnetization with the increase in sodium hydroxide concentration could be attributed to the strengthening of super-exchange interaction between A and B sublattices, due to replacements of Co{sup 3+} ions (magnetic moment of 0 μ{sub B}) by Co{sup 2+} ions (magnetic moment of 3 μ{sub B}) at B sublattices. The obvious increase in the coercivity field with the increase in concentration of NaOH solutions can be interpreted in terms of enhancement of magneto-crystalline anisotropy that originated from gradual substitutions of Co{sup 3+} ions with Co{sup 2+} ions at the octahedral sites.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

A Novel Wet-Chemical Route for Synthesis of Multiferroic AMnO{sub 3} (A = Gd, Tb, Dy) Particles and Its Structural, Optical and Magnetic Properties

Several multiferroic AMnO{sub 3} (A = Gd, Tb, Dy) particles were synthesized by microwave-assisted acrylamide gel route. The influence of A-site cation on the phase purity, surface morphologies, and optical and magnetic properties of the as-prepared multiferroic AMnO{sub 3} (A = Gd, Tb, Dy) particles was investigated. X-ray diffraction pattern, Fourier transform infrared spectroscopy, and Raman spectroscopy confirm the pure phase of the AMnO{sub 3} (A = Gd, Tb, Dy) particles exhibits an orthorhombic perovskite structure. Scanning electron microscopy (SEM) observation indicates that the surface morphology of AMnO{sub 3} (A = Gd, Tb, Dy) particles is significantly dependent on the A-site cation. The particle size of AMnO{sub 3} (A = Gd, Tb, Dy) particles increases with the increasing atomic number of A-site cation The optical band gap values of AMnO{sub 3} (A = Gd, Tb, Dy) particles decrease with an increase in the atomic number of A-site cation. Magnetization measurements show that these AMnO{sub 3} (A = Gd, Tb, Dy) particles exhibit magnetic ordering at low temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

An Electro-Assisted Powder Metallurgical Route for the Preparation of Porous Ti and NiTi in Molten CaCl{sub 2}

Molten salts can provide a high-temperature and oxygen-water-free environment, and the electrochemical polarization is able to reduce the oxide scale on the surface of Ti and Ni particles in molten salts and, thereby, enhance the sintering and accelerating atom diffusion between Ti and Ni. Thus, an electro-assisted powder metallurgical (EPM) approach was developed to prepare porous Ti and NiTi from metal powders in molten salts, where the porous pellet cathode made of the mixture of Ni and Ti powders is electrochemically polarized to facilitate the generation of the porous Ti and NiTi at a temperature lower than 1000 °C. The electrolytic product obtained under a cell voltage of 3 V for 12 hours is nearly pure NiTi with a tiny amount of undesired Ni{sub 3}Ti and NiTi{sub 2} phases. Overall, the EPM route could be a straightforward and general way to prepare porous Ti and Ti-alloys for implants and other applications.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Abnormal Transient Liquid Phase Bondability of High-Volume Fraction SiC Particle-Reinforced A356 Composite for Cu Interlayer and the Interlayer Improvement Routes

Features of transient liquid phase (TLP) bondability of high-volume fraction (70 vol.%) SiC particle-reinforced A356 composite for popular Cu interlayer were investigated. Although Cu foil was melted, molten Cu was completely expulsed, indicating that the numerous SiC particles significantly deteriorated wettability not only at particle/braze metal (P/M) interface, but also at the matrix/braze metal (M/M) interface. For the reason of poor wettability at P/M interface, a model showing there is a “window period” for actual wetting reaction (allowing liquid phase to be in contact with surficial SiC particles) much shorter than nominal isothermal solidification time during TLP bonding of the composite containing sintered ceramic preform was proposed. For the poor wettability at M/M interface, both size effect of too small matrix unit (2 ~ 20 μm) and restraint effect of the rigid porous ceramic preform on suppressing oxide film crack on the small matrix unit surface were proposed. Thus, chemical route to disrupt oxide film on the small matrix unit surface should be preferred in braze composition design. For example, Al-27Cu-5Si-2Mg-1Ti braze was developed by co-addition of Mg and Ti to improve wettability and to in situ reinforce bond seam, respectively; Ti also could remedy Mg loss for improving wettability.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Compressive Deformation Behavior of Open-Cell Cu-Zn-Al Alloy Foam Made Through P/M Route Using Mechanically Alloyed Powder

Cu-Zn-Al foams of varying porosity fractions using mechanical alloyed powder have been made through powder metallurgy route. Here, NH{sub 4} (HCO{sub 3}) was used as a space holder. Mechanically alloyed Cu-Zn-Al is made using a planetary ball mill taking the ratio of Cu/Zn/Al = 70:25:5 (by weight ratio). The ball/powder ratios were varied in the four ranges 10:1, 15:1, 20:1, and 25:1. Green compacts of milled powder and space holder samples were sintered at three stages at three different temperatures 350, 550, and 850 °C for 1 h at each stage. The crystalline size and particle size as a function of ball/powder ratios were examined. The compressive deformation responses of foams are varied with relative density and the ball/powder ratio. The plateau stress and energy absorption of these foams increase with an increase in relative density but decreases with increase in ball/powder ratio, even though crystalline size decreases. This has further been explained on the basis of particle morphology as a function of ball/powder ratio.

36 MATERIALS SCIENCE↗
DOE OSTI2019

A New Approach for Consolidation of Pure Magnesium Powder Using an Integrated Severe Plastic Deformation Route

In this paper, a new approach using a novel severe plastic deformation route is presented for consolidation and processing of a high-density and ultrafine-grained pure magnesium. Pure magnesium particles were successfully consolidated at 400 °C into a sufficiently dense bulk material using a new combined method including cyclic extrusion compression, equal channel angular pressing (ECAP) and conventional extrusion. The grain refinement, consolidation behavior and mechanical properties were deeply investigated. Results showed that the as-consolidated material had a fine grain structure with excellent tensile strength and ductility compared to as-cast and as-ECAPed specimens. Vickers microhardness increased from 38.75 to 52.58 during the process. Porosity also reduced considerably from 12.55 to 1.2% during the process which led to a dense bulk material. Results indicate that the introduced method is a promising and effective process for producing strong bulk materials from metal powders.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Wear Resistance and Tribological Features of Ultra-Fine-Grained Al-Mg Alloys Processed by Constrained Groove Pressing-Cross Route

In the present study, the wear behavior of ultra-fine grained (UFG) Al-Mg alloys produced by a severe plastic deformation (SPD) method was assessed and compared against the annealed coarse-grained alloy. To this end, weight loss, wear resistance, friction coefficient, and morphology of the worn surfaces was investigated. Constrained groove pressing-cross route (CGP-CR) process, an SPD technique, was implemented at ambient temperature up to two passes to impose an equivalent plastic strain of about 4.64. Formation of a UFG structure with an average sub-grain size of ~ 350 nm with an enhanced tensile strength of up to ~ 225 MPa and indentation hardness of up to ~ 95 HV were achieved upon two passes of CGP-CR process. The pin-on-disk dry wear sliding testing was conducted up to a distance of 1000 m under normal loads of 5, 7, and 9 N at a constant sliding speed of 0.5 m/s. The trends measured for the evaluation of wear properties/mechanisms are discussed based on the microstructural features and mechanical property of UFGed alloys. The results showed that by employing the CGP-CR process and through the formation of UFG structure, the wear resistance was considerably increased. This was even beyond two times (~ 100%) larger depending on the normal loading with the lowest coefficient of friction around 0.6. Observation and study of the morphology of the worn surfaces under field emission-scanning electron microscopy (FE-SEM) revealed a change in the wear mechanism from sticking followed by formation of plastic deformation bands and delamination in the coarse-grained annealed alloy into a combined abrasive-adhesive behavior in the UFG material.

36 MATERIALS SCIENCE↗
DOE OSTI2018

A new bi-objective periodic vehicle routing problem with maximization market share in an uncertain competitive environment

This paper presents a new variant of periodic vehicle routing problem in which the reaching time to the customers affects market share. Thus, there is a competition between distributors to achieve more market share by reaching the customers earlier than others; moreover, travel time between each two pairs of customers is uncertain. This situation is called an uncertain competitive environment. For the given problem, a new bi-objective mathematical model including minimization of total traveled time and maximization of the market share is presented. In order to solve this model, a multi-objective particle swarm (MOPSO) and local MOPSO algorithms are applied; and to evaluate the algorithm performance, some samples are generated; and the results of algorithms are compared based on some comparison metrics. The results demonstrate that the proposed LMOPSO algorithm leads to a better performance compared to the MOPSO in most comparison metrics.

97 MATHEMATICS AND COMPUTING↗