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5 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Nuclear Data Sheets for A=170☆

Nuclear structure data pertaining to all nuclei with mass number A=170 have been evaluated, and incorporated into the ENSDF data file. This evaluation supersedes the previous evaluation (Coral M. Baglin), Nuclear Data Sheets 96, 611 (2002), (cutoff date 15 August 2002) and subsequent updates of the ENSDF file for Yb to Dy (cutoff 15 April 2010), Lu (cutoff 8 October 1998), Pt (cutoff 17 February 1999) and Ta, Os (cutoff 7 April 1998). Since the previous evaluation, {sup 170}Gd has been observed and the ground state T{sub 1/2} measured. New excited states have also been observed in the neutron rich {sup 170}Dy. The ground state T{sub 1/2} of {sup 170}Tb has been determined, however, there are currently still no excited states observed in this nucleus. There remains some uncertainty in the ground state and longer-lived isomer in {sup 170}Ir which could warrent further experimental investigation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1988

Geochemistry of K/T boundaries in India and contributions of Deccan volcanism

Three possible Cretaceous/Tertiary (K/T) boundary sections in the Indian subcontinent were studied for their geochemical and fossil characteristics. These include two marine sections of Meghalaya and Zanskar and one continental section of Nagpur. The Um Sohryngkew river section of Meghalaya shows a high iridium, osmium, iron, cobalt, nickel and chromium concentration in a 1.5 cm thick limonitic layer about 30 cm below the planktonic Cretaceous-Palaeocene boundary identified by the characteristic fossils. The Bottaccione and Contessa sections at Gubbio were also analyzed for these elements. The geochemical pattern at the boundary at the Um Sohryngkew river and Gubbio sections are similar but the peak concentrations and the enrichment factors are different. The biological boundary is not as sharp as the geochemical boundary and the extinction appears to be a prolonged process. The Zanskar section shows, in general, similar concentration of the siderophile, lithophile and rare earth elements but no evidence of enrichment of siderophiles has so far been observed. The Takli section is a shallow inter-trappean deposit within the Deccan province, sandwiched between flow 1 and flow 2. The geochemical stratigraphy of the inter-trappeans is presented. The various horizons of ash, clay and marl show concentration of Fe and Co, generally lower than the adjacent basalts. Two horizons of slight enrichment of iridium are found within the ash layers, one near the contact of flow 1 and other near the contact of flow 2, where iridium occurs at 170 and 260 pg/g. These levels are lower by a factor of 30 compared to Ir concentration in the K/T boundary in Meghalaya section. If the enhanced level of some elements in a few horizons of the ash layer are considered as volcanic contribution by some fractionation processes than the only elements for which it occurs are REE, Ir and possibly Cr.

Bhandari, N.↗
DOE OSTI2018

Rational Design of a Catalyst for the Selective Monoborylation of Methane

Combined computational and experimental studies elucidate the mechanism and suggest rational design and optimization strategies of a bis(phosphine)-supported iridium-catalyst for methane monoborylation. The activation of the C–H bond in methane via oxidative addition using tris(boryl) iridium(III) complexes bearing bis-chelating supporting ligands is modeled computationally. This model shows that the use of the soft Lewis base ligand such as 1,2-bis(dimethylphosphino)ethane (dmpe) lowers the activation barrier of the rate-determining step as it facilitates polarization of the metal-center, lowering the barrier of the oxidative addition to afford a seven-coordinate iridium(V) intermediate. The experimental optimization of this reaction using high-throughput methods shows that up to 170 turnovers can be achieved at 150 °C (500 psi) within 16 h using bis(pinacolato)diboron, a well-defined homogeneous and monomeric catalyst (dmpe)Ir(COD)Cl that is readily available from commercial precursors, with selectivity for the monoborylation product. High-boiling cyclic aliphatic solvents decalin and cyclooctane also prove suitable for this reaction, while being inert toward borylation. In accordance with the lower calculated activation barrier, catalytic turnover is also observed at 120 °C with up to 50 turnovers over the course of 4 days in cyclohexane solvent. Here, it was found that the borylation of methane is only achieved via one catalytic cycle, and buildup of pinacolborane, a side-product from methane borylation with bis(pinacolato)diboron, inhibits catalytic activity.

computational molecular modeling↗
DOE OSTI2022

Synthesis and Exploratory Catalysis of 3d Metals: Atom and Group-Transfer Reactions and the Activation and Functionalization of Small Molecules Including Greenhouse Gases

Determining ways to convert natural gas, with zero emissions, and to more value-added materials such as olefins is one of the main goals in my research group. Over this funding period, we explored the chemistry of early-transition metals with metal-nitrogen multiple bonds, specifically titanium and zirconium nitrides, and explored their redox properties, basicity and reactivity with small molecules including greenhouses gases such as carbon dioxide. Some of these work serve as inspiration for the chemistry of important materials such as uranium nitride along with its unprecedented basicity and ability to activate C-H bonds. Using robust chelating templates we also examined rare examples of trivalent group 4 transition metal ions, and studied these spectroscopically. Using early transition metal ions we also explored synthetic routes to new phosphide based products using the phosphaethynolate salt. In addition, we also explored the chemistry of ferrous systems, and redox active ligand that can allow us to reversibly break and make C-S as well as N-N bonds, activate dinitrogen forming unusual MNNM topologies. Our final component describes how we activate methane and dehydrocouple if with a carbene source to form ethylene. Using this information, we also discovered a simple to make iridium catalyst that activate and functionalize methane with 9:1 selectivity for mono-functionalization. We have established a pathway that leads to poisoning of the catalyst and have found optimal conditions for higher selectivity and with over 170 Turnovers.

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

Structure sensitivity of n -butane hydrogenolysis on supported Ir catalysts

Hydrogenolysis of alkanes has been widely reported as structure sensitive reaction on transition metal heterogeneous catalysts with metal particle sizes ranging between 1 and 20 nm. In this work, a series of Ir/MgAl 2 O 4 and Ir/SiO 2 catalysts with different Ir particle sizes ranging from subnanometer clusters (<1 nm) to nanoparticles (1–3 nm) were prepared and tested for n-butane hydrogenolysis. Our results show that the activity towards n-butane hydrogenolysis increases as Ir particle size increases in the lower particle size range, goes through a maximum at ~1.4–1.6 nm and then drops with a further increase in particle size. In this work, the product distribution at low temperature (170–190 °C) is dominated by central and terminal CAC bond cleavage of n-butane, and less by two CAC bond cleavage or further hydrogenolysis of the propane and ethane products. The selectivity to central CAC bond cleavage is highly dependent on the size of Ir and increases with a decrease in particle size down to ~1.4 nm but remains constant with further decrease in size. The results show that an Ir size of ~1.4 nm is optimum for n-butane hydrogenolysis activity and selectivity towards ethane.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗