Summary report on the geochemistry of Yucca Mountain and environs

This report gives a detailed description of work at Los Alamos that will help resolve geochemical issues pertinent to siting a high-level nuclear waste repository in tuff at Yucca Mountain, Nevada. It is necessary to understand the properties and setting of the host tuff because this rock provides the first natural barrier to migration of waste elements from a repository. The geochemistry of tuff is being investigated with particular emphasis on retardation processes. This report addresses the various aspects of sorption by tuff, physical and chemical makeup of tuff, diffusion processes, tuff/groundwater chemistry, waste element chemistry under expected repository conditions, transport processes involved in porous and fracture flow, and geochemical and transport modeling

Measurement and Modelling of Pm Sorption onto TiO2 and goethite

The sorption of Pm (1 x 10(-9) M) onto TiO2 and goethite has been studied as a function of pH and Ionic strength (0.01, 0.1 M NaClO4) at ambient temperature under N-2 atmosphere. For both minerals studied there is no effect of the different ionic strengths and the sorption (log K-a vs. pH) increases with a slope of similar to2. At the same pH sorption is lower on the more positively (or less negatively) charged goethite (pH(pzc) = 8.4) than on the TiO2 (pH(pzc) = 6.2). A comparison to other trivalent cations sorbed on different substrates (made by extracting values from %-sorbed curves and calculating these to K-a) indicate a similar pH-dependence. The results have been fitted using a 1-pK basic Stern model with FITEQL [1]. An a priori restriction was that only one sorption reaction stoichiometry at a time was to be used to keep the number of parameters as small as possible. Outersphere and mono-, bi- and tri-dentate inner-sphere complexes were fitted. For each fit the value of the capacitance was varied to find the value that provided the best fit. Two different site densities were used: 1 site/nm(2) and 2.31 sites/nm(2). For the low site density the reaction which provides the best tit was: drop SOH0.5- + Pm+3 drop SOHPm2.5+for both minerals. At the high site density the same reaction fits for TiO2 while there are several reactions that are equivalent in the fit for goethite

Measurement and Modelling of Pm Sorption onto TiO2 and goethite

The sorption of Pm (1 x 10(-9) M) onto TiO2 and goethite has been studied as a function of pH and Ionic strength (0.01, 0.1 M NaClO4) at ambient temperature under N-2 atmosphere. For both minerals studied there is no effect of the different ionic strengths and the sorption (log K-a vs. pH) increases with a slope of similar to2. At the same pH sorption is lower on the more positively (or less negatively) charged goethite (pH(pzc) = 8.4) than on the TiO2 (pH(pzc) = 6.2). A comparison to other trivalent cations sorbed on different substrates (made by extracting values from %-sorbed curves and calculating these to K-a) indicate a similar pH-dependence. The results have been fitted using a 1-pK basic Stern model with FITEQL [1]. An a priori restriction was that only one sorption reaction stoichiometry at a time was to be used to keep the number of parameters as small as possible. Outersphere and mono-, bi- and tri-dentate inner-sphere complexes were fitted. For each fit the value of the capacitance was varied to find the value that provided the best fit. Two different site densities were used: 1 site/nm(2) and 2.31 sites/nm(2). For the low site density the reaction which provides the best tit was: drop SOH0.5- + Pm+3 drop SOHPm2.5+for both minerals. At the high site density the same reaction fits for TiO2 while there are several reactions that are equivalent in the fit for goethite

Update report on fracture flow in saturated tuff: Dynamic transport task for the Nevada Nuclear Waste Investigations

This report summarizes the results of continuing experiments on the behavior of tracers during fracture flow in saturated, welded tuff. These experiments were completed during the past year as part of the Dynamic Transport Task of geochemical investigations for the Yucca Mountain Project sponsored by the US Department of Energy. These experiments are designed to investigate the effects of fluid movement in fractures when coupled with matrix diffusion and sorption but isolated from the effects of capillary suction and two-phase flow characteristic of unsaturated conditions. The experiments reported here are continuations of experimental efforts reported previously. The behavior of three tracers [HTO (tritiated water), TcO{sub 4}{sup {minus}} (pertechnetate), and sulforhodamine B dye] have been investigated during flow through a saturated column of densely welded tuff from the Topopah Spring Member of the Paintbrush Tuff, Yucca Mountain, Nye County, southern Nevada. 31 refs., 26 figs., 2 tabs

Neutron capture measurements on Tl-isotopes at DANCE

The thallium isotopes play an important role in the s-process nucleosynthesis at the s-process endpoint. Furthermore, 204Tl is one of few branch point isotopes in the endpoint region. The understanding of branch point isotopes provides modeling constraints on the temperatures and neutron densities during which the process takes place. The production of s-only 204Pb is controlled almost entirely by 204Tl. Measurements of the capture cross-sections of the stable Tl isotopes have recently been made using the DANCE 4π array at LANSCE. This provides needed resonance information in the region as well as preparing the way for measurements of as yet unmeasured capture cross-section of the unstable 204Tl

Isomeric ratio measurements for the radiative neutron capture

The isomeric ratio for the neutron capture reaction 176Lu(n,γ) on the Jπ= 5/2−, 761.7 keV, T1/2=32.8 ns level of 177mLu, has been determined in the neutron energy range 8.5 eV-100 keV for the first time using the DANCE array at the Los Alamos National Laboratory

Isomeric ratio measurements for the radiative neutron capture 176Lu(n,γ) at DANCE

The isomeric ratio for the neutron capture reaction 176Lu(n,γ) on the Jπ= 5/2−, 761.7 keV, T1/2=32.8 ns level of 177mLu, has been determined in the neutron energy range 8.5 eV-100 keV for the first time using the DANCE array at the Los Alamos National Laboratory

Scissors Mode of 162Dy Studied from Resonance Neutron Capture

Multi-step cascade γ-ray spectra from the neutron capture at isolated resonances of 161Dy nucleus were measured at the LANSCE/DANCE time-of-flight facility in Los Alamos National Laboratory. The objectives of this experiment were to confirm and possibly extend the spin assignment of s-wave neutron resonances and get new information on photon strength functions with emphasis on the role of the M1 scissors mode vibration. The preliminary results show that the scissors mode plays a significant role in all transitions between accessible states of the studied nucleus. The photon strength functions describing well our data are compared to results from 3He-induced reactions, (n,γ) experiments on Gd isotopes, and (γ,γ’) reactions

Scissors Mode of

Multi-step cascade γ-ray spectra from the neutron capture at isolated resonances of 161Dy nucleus were measured at the LANSCE/DANCE time-of-flight facility in Los Alamos National Laboratory. The objectives of this experiment were to confirm and possibly extend the spin assignment of s-wave neutron resonances and get new information on photon strength functions with emphasis on the role of the M1 scissors mode vibration. The preliminary results show that the scissors mode plays a significant role in all transitions between accessible states of the studied nucleus. The photon strength functions describing well our data are compared to results from 3He-induced reactions, (n,γ) experiments on Gd isotopes, and (γ,γ’) reactions

Neutron capture experiments with 4π DANCE Calorimeter

In recent years we have performed a series of neutron capture experiments with the DANCE detector array located at the Los Alamos Neutron Science Center. The radiative decay spectrum from the compound nucleus contains important information about nuclear structure and the reaction mechanism. The primary goals of the measurements are to obtain improved capture cross sections, to determine properties of the photon strength function, to improve neutron level densities and strength functions by determining the spin and parity of the capturing states. We shall present examples of our recent results