Noble metal-catalyzed homogeneous and heterogeneous processes in treating simulated nuclear waste media with formic acid

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Simulants for the Hanford Waste Vitrification Plant feed containing the major non-radioactive components Al, Cd, Fe, Mn, Nd, Ni, Si, Zr, Na, CO{sub 3}{sup 2}-, NO{sub 3}-, and NO{sub 2}- were used to study reactions of formic acid at 90{degrees}C catalyzed by the noble metals Ru, Rh, and/or Pd found in significant quantities in uranium fission products. Such reactions were monitored using gas chromatography to analyze the CO{sub 2}, H{sub 2}, NO, and N{sub 2}O in the gas phase and a microammonia electrode to analyze the NH{sub 4}+/NH{sub 3} in the liquid phase as a function of time. The following ... continued below

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12 p.

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King, R.B.; Bhattacharyya, N.K. & Smith, H.D. September 1, 1995.

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  • Pacific Northwest Laboratory
    Publisher Info: Pacific Northwest Lab., Richland, WA (United States)
    Place of Publication: Richland, Washington

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Simulants for the Hanford Waste Vitrification Plant feed containing the major non-radioactive components Al, Cd, Fe, Mn, Nd, Ni, Si, Zr, Na, CO{sub 3}{sup 2}-, NO{sub 3}-, and NO{sub 2}- were used to study reactions of formic acid at 90{degrees}C catalyzed by the noble metals Ru, Rh, and/or Pd found in significant quantities in uranium fission products. Such reactions were monitored using gas chromatography to analyze the CO{sub 2}, H{sub 2}, NO, and N{sub 2}O in the gas phase and a microammonia electrode to analyze the NH{sub 4}+/NH{sub 3} in the liquid phase as a function of time. The following reactions have been studied in these systems since they are undesirable side reactions in nuclear waste processing: (1) Decomposition of formic acid to CO{sub 2} + H{sub 2} is undesirable because of the potential fire and explosion hazard of H{sub 2}. Rhodium, which was introduced as soluble RhCl{sub 3}-3H{sub 2}O, was found to be the most active catalyst for H{sub 2} generation from formic acid above {approximately} 80{degrees}C in the presence of nitrite ion. The H{sub 2} production rate has an approximate pseudo first-order dependence on the Rh concentration, (2) Generation of NH{sub 3} from the formic acid reduction of nitrate and/or nitrite is undesirable because of a possible explosion hazard from NH{sub 4}NO{sub 3} accumulation in a waste processing plant off-gas system. The Rh-catalyzed reduction of nitrogen-oxygen compounds to ammonia by formic acid was found to exhibit the following features: (a) Nitrate rather than nitrite is the principal source of NH{sub 3}. (b) Ammonia production occurs at the expense of hydrogen production. (c) Supported rhodium metal catalysts are more active than rhodium in any other form, suggesting that ammonia production involves heterogeneous rather than homogeneous catalysis.

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12 p.

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INIS; OSTI as DE96002718

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  • 8. international symposium on relations between homogeneous and heterogeneous catalysis, Balatonfuered (Hungary), 10-14 Sep 1995

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  • Other: DE96002718
  • Report No.: PNL-SA--25954
  • Report No.: CONF-9509175--1
  • Grant Number: AC06-76RL01830
  • Office of Scientific & Technical Information Report Number: 135035
  • Archival Resource Key: ark:/67531/metadc626036

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  • September 1, 1995

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  • June 16, 2015, 7:43 a.m.

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  • April 7, 2016, 4:45 p.m.

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King, R.B.; Bhattacharyya, N.K. & Smith, H.D. Noble metal-catalyzed homogeneous and heterogeneous processes in treating simulated nuclear waste media with formic acid, article, September 1, 1995; Richland, Washington. (digital.library.unt.edu/ark:/67531/metadc626036/: accessed August 18, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.