56 research outputs found
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Phase Chemistry of Tank Sludge Residual Components
About four or five distinct reprocessing technologies were used at various times in Hanford's history. After removing U and Pu (or later 137Cs and 90Sr), the strongly acidic HLW was ''neutralized'' to high pH (>13) and stored in steel-lined tanks. High pH was necessary to prevent tank corrosion. While each technology produced chemically distinct waste, all wastes were similar in that they were high pH, concentrated, aqueous solutions. Dominant dissolved metals were Fe and/or Al, usually followed by Ni, Mn, or Cr. In an effort to reduce waste volume, many of the wastes were placed in evaporators or allowed to ''self-boil'' from the heat produced by their own radioactive decay. Consequently, today's HLW has been aging at temperatures ranging from 20 to 160 C. Previous studies of synthetic HLW sludge analogues have varied in their exact synthesis procedures and recipes, although each involved ''neutralization'' of acidic nitrate salt solutions by concentrated NaOH. Some recipes included small amounts of Si, SO4 2-, CO3 2-, and other minor chemical components in the Hanford sludges. The work being conducted at the University of Colorado differs from previous studies and from parallel current investigations at Sandia National Laboratories in the simplicity of the synthetic sludge we are investigating. We are emphasizing the dominant role of Fe and Al, and secondarily, the effects of Ni and Si on the aging kinetics of the solid phases in the sludge
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Phase Chemistry of Tank Sludge Residual Components
Experiments began with ''neutralization'' of iron (III)-aluminum nitrate solutions by addition of sodium hydroxide at room temperature. The final pH of most experiments was approximately 13.7. The samples were neutralized in PP or HDPE bottles that were then submerged in a water bath and aged at 90 C for up to 120 h. (In the low-Al systems, X-ray diffraction (XRD) results suggest that transformation of the initial amorphous precipitate to crystalline phases was complete after this time.) Experiments were run either as a single 250 mL sample (''single age experiments'') or as 2 L batches, from which 250 mL aliquots were drawn (''batch experiments''). Both solid phase chemistry and solution composition were monitored throughout the aging process. Samples were centrifuged and the experimental supernatant solutions were decanted and passed through a 0.4 mm syringe filter prior to analysis. Solids were dialyzed to removed excess salts. Aqueous Al and Fe were measured by the catechol violet (Dougan and Wilson, 1974) and Ferrozine (Dawson and Lyle, 1990) techniques, respectively. X-ray diffraction data were taken with a Scintag powder diffractometer scanning at 1{sup o} 2Q per minute using Cu K-a radiation and a graphite beam monochromator
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A Comprehensive Study of the Solubility, Thermochemistry, Ion Exchange, and Precipitation Kinetics of NO3 Cancrinite and NO3 Sodalite
NO3 cancrinite and NO3 sodalite haves been found as a common sodium alumino-silicate forming in strongly caustic alkaline aqueous solutions associated with radioactive High Level Waste (HLW) stored in many underground tanks and also in nuclear waste treatment facilities such as the Savannah River Site (SRS). The appearance of these phases have created very expensive problems in waste treatment plants by fouling process evaporators in the SRS waste processing facility. Therefore, in order to prevent their formation an assessment of the relative stability, formation kinetics, and the ion-exchange characteristics of these two phases in HLW solutions needs to be investigated. The goals of this project are to: (1) Develop a robust equilibrium thermodynamic framework to accurately describe and predict the formation of NO3 cancrinite and NO3 sodalite. (2) Provide a comprehensive characterization of the solid precipitation rates and mechanisms using novel spectroscopic (e.g., NMR) and thermochemical techniques in conditions encountered in HLW waste solutions. (3) Investigate the ion exchange capacity of these zeolitic phases with respect to radionuclides and RCRA metal species
Tweed in Martensites: A Potential New Spin Glass
We've been studying the ``tweed'' precursors above the martensitic transition
in shape--memory alloys. These characteristic cross--hatched modulations occur
for hundreds of degrees above the first--order shape--changing transition. Our
two--dimensional model for this transition, in the limit of infinite elastic
anisotropy, can be mapped onto a spin--glass Hamiltonian in a random field. We
suggest that the tweed precursors are a direct analogy of the spin--glass
phase. The tweed is intermediate between the high--temperature cubic phase and
the low--temperature martensitic phase in the same way as the spin--glass phase
can be intermediate between ferromagnet and antiferromagnet.Comment: 18 pages and four figures (included
Disorder-Driven Pretransitional Tweed in Martensitic Transformations
Defying the conventional wisdom regarding first--order transitions, {\it
solid--solid displacive transformations} are often accompanied by pronounced
pretransitional phenomena. Generally, these phenomena are indicative of some
mesoscopic lattice deformation that ``anticipates'' the upcoming phase
transition. Among these precursive effects is the observation of the so-called
``tweed'' pattern in transmission electron microscopy in a wide variety of
materials. We have investigated the tweed deformation in a two dimensional
model system, and found that it arises because the compositional disorder
intrinsic to any alloy conspires with the natural geometric constraints of the
lattice to produce a frustrated, glassy phase. The predicted phase diagram and
glassy behavior have been verified by numerical simulations, and diffraction
patterns of simulated systems are found to compare well with experimental data.
Analytically comparing to alternative models of strain-disorder coupling, we
show that the present model best accounts for experimental observations.Comment: 43 pages in TeX, plus figures. Most figures supplied separately in
uuencoded format. Three other figures available via anonymous ftp
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Desalination of brackish ground waters and produced waters using in-situ precipitation.
The need for fresh water has increased exponentially during the last several decades due to the continuous growth of human population and industrial and agricultural activities. Yet existing resources are limited often because of their high salinity. This unfavorable situation requires the development of new, long-term strategies and alternative technologies for desalination of saline waters presently not being used to supply the population growth occurring in arid regions. We have developed a novel environmentally friendly method for desalinating inland brackish waters. This process can be applied to either brackish ground water or produced waters (i.e., coal-bed methane or oil and gas produced waters). Using a set of ion exchange and sorption materials, our process effectively removes anions and cations in separate steps. The ion exchange materials were chosen because of their specific selectivity for ions of interest, and for their ability to work in the temperature and pH regions necessary for cost and energy effectiveness. For anion exchange, we have focused on hydrotalcite (HTC), a layered hydroxide similar to clay in structure. For cation exchange, we have developed an amorphous silica material that has enhanced cation (in particular Na{sup +}) selectivity. In the case of produced waters with high concentrations of Ca{sup 2+}, a lime softening step is included
Hysteresis and hierarchies: dynamics of disorder-driven first-order phase transformations
We use the zero-temperature random-field Ising model to study hysteretic
behavior at first-order phase transitions. Sweeping the external field through
zero, the model exhibits hysteresis, the return-point memory effect, and
avalanche fluctuations. There is a critical value of disorder at which a jump
in the magnetization (corresponding to an infinite avalanche) first occurs. We
study the universal behavior at this critical point using mean-field theory,
and also present preliminary results of numerical simulations in three
dimensions.Comment: 12 pages plus 2 appended figures, plain TeX, CU-MSC-747
A process model of natural attenuation in drainage from a historic mining district
A process model was used to better understand the controls on the chemical evolution of drainage in a historic mining district. At the Pecos Mine Operable Unit, New Mexico, drainage near the waste rock pile is acidic (pH varies from 3.0--5.0) and carries high concentrations of Zn, Al, Cu and Pb. As drainage flows toward the Pecos River, pH increases to greater than 7 and heavy metal content decreases. A process model of natural attenuation in this drainage shows the main controls on pH are reaction with a local bedrock that contains limestone, and concurrent mixing with tributary streams. Models that account for both calcite dissolution and mixing reproduce the observed decrease in aqueous metal concentrations with increasing pH. Contaminant concentrations attenuate primarily via two distinct pathways: Al, Cu, Fe and Pb precipitate directly from solution, whereas Zn, Mg, Mn and SO{sub 4} concentrations decrease primarily through dilution. Additionally, Pb adsorbs to precipitating hydroxide surfaces
Spatial Representations Are Specific to Different Domains of Knowledge
There is evidence that many abstract concepts are represented cognitively in a spatial format. However, it is unknown whether similar spatial processes are employed in different knowledge domains, or whether individuals exhibit similar spatial profiles within and across domains. This research investigated similarities in spatial representation in two knowledge domains â mathematics and music. Sixty-one adults completed analogous number magnitude and pitch discrimination tasks: the Spatial-Numerical Association of Response Codes and Spatial-Musical Association of Response Codes tasks. Subgroups of individuals with different response patterns were identified through cluster analyses. For both the mathematical and musical tasks, approximately half of the participants showed the expected spatial judgment effect when explicitly cued to focus on the spatial properties of the stimuli. Despite this, performances on the two tasks were largely independent. Consistent with previous research, the study provides evidence for the spatial representation of number and pitch in the majority of individuals. However, there was little evidence to support the claim that the same spatial representation processes underpin mathematical and musical judgments
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Abnormal neural responses to harmonic syntactic structures in congenital amusia
Harmonic syntactic structures are organized hierarchically through local and long-distance dependencies. The present study investigated whether the processing of harmonic syntactic structures is impaired in congenital amusia, a neurodevelopmental disorder of pitch perception. Harmonic sequences containing two phrases were used as stimuli, in which the first phrase ended with a half cadence and the second with an authentic cadence. In Experiment 1, we manipulated the ending chord in the authentic cadence to be either syntactically regular or irregular. Sixteen amusics and 16 controls judged the expectedness of these chords while their EEG waveforms were recorded. In comparison to the regular endings, irregular endings elicited an ERAN, an N5 and a late positive component in controls but not in amusics, indicating that amusics were impaired in perceiving harmonic syntactic structures induced by local dependencies. In Experiment 2, we manipulated the half cadence of the harmonic sequences to examine the processing of harmonic syntactic structures induced by long-distance dependencies. An ERAN-like response and an N5 were elicited in controls but not in amusics, suggesting that amusics were impaired in processing long-distance syntactic dependencies. Furthermore, for controls, the neural processing of local and long-distance syntactic dependencies was correlated in the late (as indexed by the N5) but not in the early stage. These findings indicate that amusics are impaired in the detection of syntactic violations and subsequent harmonic integration. The implications of these findings in terms of hierarchical music-syntactic processing are discussed
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