Acid-base behavior in hydrothermal processing of wastes. 1998 annual progress report

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'A new technology, hydrothermal oxidation (also called supercritical water oxidation), is being developed to treat high level nuclear wastes. Nitrates are reduced to nitrogen; furthermore, phosphates, alumina sludge, and chromium are solubilized, and the sludge is reconstituted as fine oxide particles. A major obstacle to development of this technology has been a lack of scientific knowledge of chemistry in hydrothermal solution above 350 C, particularly acid-base behavior, and transport phenomena, which is needed to understand corrosion, metal-ion complexation, and salt precipitation and recovery. The objective is to provide this knowledge with in-situ UV-vis spectroscopic measurements and fully molecular computer simulation. ... continued below

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3 pages

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Johnson, K.P. & Rossky, P.J. June 1, 1998.

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'A new technology, hydrothermal oxidation (also called supercritical water oxidation), is being developed to treat high level nuclear wastes. Nitrates are reduced to nitrogen; furthermore, phosphates, alumina sludge, and chromium are solubilized, and the sludge is reconstituted as fine oxide particles. A major obstacle to development of this technology has been a lack of scientific knowledge of chemistry in hydrothermal solution above 350 C, particularly acid-base behavior, and transport phenomena, which is needed to understand corrosion, metal-ion complexation, and salt precipitation and recovery. The objective is to provide this knowledge with in-situ UV-vis spectroscopic measurements and fully molecular computer simulation. A major objective of the experimental studies has been to determine the equilibria for Cr(VI) up to 420 C as this is a key species to be removed from nuclear wastes. A wide range of concentrations of KOH and perchloric acid were utilized to manipulate the acid-base equilibria and to understand the effects of ion solvation and ion pairing. The second system is the equilibria between nitric acid, nitrous acid, nitrogen dioxide, nitrite and nitrate ions and oxygen. For both of these systems, chemical equilibria has not been measured previously in hydrothermal solution at these temperatures. On the theoretical side, the authors have focused on the study of the transport properties of aqueous ions in supercritical water. The motivation for these studies is two fold. First, although transport coefficients are fundamental to solution chemistry reaction rates, the behavior of such transport properties over wide ranges of density and temperature are not well established experimentally, particularly at the densities typically of interest (< 0.5 g/cc). Second, due to practical challenges, ionic association equilibria in SCW is typically accessed via measurements of conductivity followed by analysis through a theoretical model that incorporates ion pairing. The results of these analyses in the interesting low density region have yielded results for the limiting infinite dilution conductivity of alkali halides which are not consistent among labs. However, the most common result suggests a nearly constant ionic diffusion constant with decreasing density, which is further rather insensitive to temperature. This is in contrast to the typical behavior at higher densities, where there is agreement on a linear increase with decreasing density. Either this surprising behavior is a physical result of a balance of forces that is different at the lower densities, or the model used to extrapolate to infinite dilution, and to extract the association constants, is not accurate for these cases. The goal is to determine independently via computer simulation what one should expect of these transport coefficients.'

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3 pages

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  • Other: DE00013627
  • Report No.: EMSP-54506--98
  • Grant Number: NONE
  • DOI: 10.2172/13627 | External Link
  • Office of Scientific & Technical Information Report Number: 13627
  • Archival Resource Key: ark:/67531/metadc623004

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  • June 1, 1998

Added to The UNT Digital Library

  • June 16, 2015, 7:43 a.m.

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  • June 13, 2016, 4:22 p.m.

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Johnson, K.P. & Rossky, P.J. Acid-base behavior in hydrothermal processing of wastes. 1998 annual progress report, report, June 1, 1998; United States. (digital.library.unt.edu/ark:/67531/metadc623004/: accessed August 18, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.