Development of novel composite sorbents for the removal of actinides from environmental and analytical solutions

A novel approach to preparing granular sorbents for the separation of actinides has been developed, where the extractant is directly immobilized in an inert matrix. This allows substantially higher extractant loadings in the sorbent than for conventional extraction chromatography resins. This approach utilizes polyacrylonitrile (PAN) as the inert matrix material. The well-known actinide extractant octyl (phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) has been loaded into sorbent granules at extractant loadings from 20 to 33 wt.% CMPO. The porosity of the PAN matrix allows the active material to have rapid and complete access to the solution containing the impurities, resulting in improved kinetics and higher sorption capacities. Sorbents containing CMPO were prepared using PAN as a binding matrix, and tested against commercially available actinide extraction chromatography resins. Direct comparative batch contact tests performed with TRU-Resin^Ò and CMPO-PAN using an INEEL tank waste simulant, resulting in distribution coefficient (K _d) values for Am approximately 2-90 times higher for CMPO-PAN than for TRU-Resin. Batch distribution coefficient (K _d) values for Pu were approximately 60-150 times higher for CMPO-PAN than for the TRU-Resin. Acid dependency curves were generated for Am and Pu with CMPO-PAN over a concentration range of 1 mM to 5M HNO₃.     

Repulsive Casimir forces

We discuss repulsive Casimir forces between dielectric materials with nontrivial magnetic susceptibility. It is shown that considerations based on the naive pairwise summation of van der Waals and Casimir-Polder forces may not only give an incorrect estimate of the magnitude of the total Casimir force but even the wrong sign of the force when materials with high dielectric and magnetic responses are involved. Indeed repulsive Casimir forces may be found in a large range of parameters, and we suggest that the effect may be realized in known materials. The phenomenon of repulsive Casimir forces may be of importance both for experimental study and for nanomachinery applications.     

Final state interactions in deuteron breakup by protons at 585 and 800 MeV

Neutron-proton final state interactions (FSI) were observed in the deuteron breakup reaction ²H(p, 2p)n-via a kinematically complete experiment at incident proton energies of 585 and 800 MeV. Kinematic conditions were chosen which allowed the final state proton and neutron to have small relative energies; data were taken at four proton c.m. scattering angles at 800 MeV, ranging from 71° to 119° and at 94° and 106° at 585 MeV. The data are analyzed in terms of the Goldberger-Watson formalism for final state interactions, and the individual contributions of the ¹S₀ and ³S₁ np states are determined. The ${}^3\text{S}{}_1{}^1\text{S}{}_0$ ratio is large, as expected from some reaction models. The ratio of ³S₁ (almost elastic) to pd elastic cross sections is in good agreement with FSI analysis.     

Validity of wave-front reconstruction and propagation of ultrabroadband pulses measured with a Hartmann-Shack sensor

Wave-front reconstruction for ultrabroadband laser pulses is verified by use of a Hartmann-Shack sensor. We estimate the accuracy of numerical wave-front propagation by comparing numerical with experimental results and verify that wave fronts of ultrabroadband laser pulses from a hollow fiber can be propagated correctly by a single polychromatic wave-front measurement to a place where detection is not practicable, e.g., inside a vacuum chamber or laser focus.     

Hydrogenation of single-walled carbon nanotubes

Towards the development of a useful mechanism for hydrogen storage, we have studied the hydrogenation of single-walled carbon nanotubes with atomic hydrogen using core-level photoelectron spectroscopy and x-ray absorption spectroscopy. We find that atomic hydrogen creates C-H bonds with the carbon atoms in the nanotube walls, and such C-H bonds can be completely broken by heating to 600 degrees C. We demonstrate approximately 65 +/- 15 at % hydrogenation of carbon atoms in the single-walled carbon nanotubes, which is equivalent to 5.1 +/- 1.2 wt % hydrogen capacity. We also show that the hydrogenation is a reversible process.     

Negative differential conductance and hot phonons in suspended nanotube molecular wires

Freely suspended metallic single-walled carbon nanotubes (SWNTs) exhibit reduced current carrying ability compared to those lying on substrates, and striking negative differential conductance at low electric fields. Theoretical analysis reveals significant self-heating effects including electron scattering by hot nonequilibrium optical phonons. Electron transport characteristics under strong self-heating are exploited for the first time to probe the thermal conductivity of individual SWNTs (approximately 3600 W m-1 K-1 at T=300 K) up to approximately 700 K, and reveal a 1/T dependence expected for umklapp phonon scattering at high temperatures.     

Langmuir monolayers of bent-core molecules

A systematic study of five different, symmetric bent-core liquid crystals in Langmuir thin films at the air/water interface is presented. Both the end chains (siloxane vs hydrocarbon) and the core (more or less amphiphilic) are varied, to allow an exploration of different possible layer structures at the interface. The characterization includes systematic surface pressure isotherms, Brewster angle microscopy, and surface potential measurements. The properties of these layers are strongly dependent on the individual type of molecule: the molecules with amphiphilic end chains lie quite flat on the surface, while the molecules with hydrophobic end chains construct multilayer structures. In both cases, the three-dimensional collapse structure is reversible.