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Auger decay mechanism in photon-stimulated desorption of ions from surfaces

Description: Photon-stimulated desorption (PSD) of positive ions was studied with synchrotron radiation using an angle-integrating time-of-flight mass spectrometer. Ion yields as functions of photon energy near core levels were measured from condensed gases, alkali fluorides, and other alkali and alkaline earth halides. These results are compared to bulk photoabsorption measurements with emphasis on understanding fundamental desorption mechanisms. The applicability of the Auger decay mechanism, in which ion desorption is strictly proportional to surface absorption, is discussed in detail. The Auger decay model is developed in detail to describe Na/sup +/ and F/sup +/ desorption from NaF following Na(1s) excitation. The major decay pathways of the Na(1s) hole leading to desorption are described and equations for the energetics of ion desorption are developed. Ion desorption spectra of H/sup +/, Li/sup +/, and F/sup +/ are compared to bulk photoabsorption near the F(2s) and Li(1s) edges of LiF. A strong photon beam exposure dependence of ion yields from alkali fluorides is revealed, which may indicate the predominance of metal ion desorption from defect sites. The large role of indirect mechanisms in ion desorption condensed N/sub 2/-O/sub 2/ multilayers is demonstrated and discussed. Ion desorption spectra from several alkali halides and alkaline earth halides are compared to bulk photoabsorption spectra. Relative ion yields from BaF/sub 2/ and a series of alkali halides are discussed in terms of desorption mechanisms.
Date: November 1, 1983
Creator: Parks, C.C.
Partner: UNT Libraries Government Documents Department

Status of radioiodine control for nuclear fuel reprocessing plants

Description: This report summarizes the status of radioiodine control in a nuclear fuel reprocessing plant with respect to capture, fixation, and disposal. Where possible, we refer the reader to a number of survey documents which have been published in the last four years. We provide updates where necessary. Also discussed are factors which must be considered in developing criteria for iodine control. For capture from gas streams, silver mordenite and a silver nitrate impregnated silica (AC-6120) are considered state-of-the-art and are recommended. Three aqueous scrubbing processes have been demonstrated: Caustic scrubbing is simple but probably will not give an adequate iodine retention by itself. Mercurex (mercuric nitrate-nitric acid scrubbing) has a number of disadvantages including the use of toxic mercury. Iodox (hyperazeotropic nitric acid scrubbing) is effective but employs a very corrosive and hazardous material. Other technologies have been tested but require extensive development. The waste forms recommended for long-term storage or disposal are silver iodide, the iodates of barium, strontium, or calcium, and silver loaded sorbents, all fixed in cement. Copper iodide in bitumen (asphalt) is a possibility but requires testing. The selection of a specific form will be influenced by the capture process used.
Date: July 1, 1983
Creator: Burger, L.L. & Scheele, R.D.
Partner: UNT Libraries Government Documents Department

Application of the carbon dioxide-barium hydroxide hydrate gas-solid reaction for the treatment of dilute carbon dioxide-bearing gas streams

Description: The removal of trace components from gas streams via irreversible gas-solid reactions in an area of interest to the chemical engineering profession. This research effort addresses the use of fixed beds of Ba(OH)/sub 2/ hydrate flakes for the removal of an acid gas, CO/sub 2/, from air that contains approx. 330 ppM/sub v/ CO/sub 2/. Areas of investigation encompassed: (1) an extensive literature review of Ba(OH)/sub 2/ hydrate chemistry, (2) microscale studies on 0.150-g samples to develop a better understanding of the reaction, (3) process studies at the macroscale level with 10.2-cm-ID fixed-bed reactors, and (4) the development of a model for predicting fixed-bed performance. Experimental studies indicated fixed beds of commercial Ba(OH)/sub 2/.8H/sub 2/O flakes at ambient temperatures to be capable of high CO/sub 2/-removal efficiencies (effluent concentrations <100 ppB), high reactant utilization (>99%), and an acceptable pressure drop (1.8 kPa/m at a superficial gas velocity of 13 cm/s). Ba(OH)/sub 2/.8H/sub 2/O was determined to be more reactive toward CO/sub 2/ than either Ba(OH)/sub 2/.3H/sub 2/O or Ba(OH)/sub 2/.1H/sub 2/O. A key variable in the development of this fixed-bed process was relative humidity. Operation at conditions with effluent relative humidities >60% resulted in significant recrystallization and restructuring of the flake and subsequent pressure-drop problems.
Date: September 1, 1983
Creator: Haag, G.L.
Partner: UNT Libraries Government Documents Department

Carbon-14 immobilization via the Ba(OH)/sub 2/. 8H/sub 2/O process

Description: The airborne release of /sup 4/C from varous nuclear facilities has been identified as a potential biohazard due to the long half-life of /sup 14/C (5730 y) and the ease with which it may be assimilated into the biosphere. At ORNL, technology has been developed for the removal and immobilization of this radionuclide. Prior studies have indicated that /sup 14/C will likely exist in the oxidized form as CO/sub 2/ and will contribute slightly to the bulk CO/sub 2/ concentration of the gas stream, which is airlike in nature (approx. 330 ppmv CO/sub 2/). The technology that has been developed utilizes the CO/sub 2/-Ba(OH)/sub 2/.8H/sub 2/O gas-solid reaction with the mode of gas-solid contacting being a fixed bed. The product, BaCO/sub 3/, possesses excellent thermal and chemical stability, prerequisites for the long-term disposal of nuclear wastes. For optimal process operation, studies have indicated that an operating window of adequate size does exist. When operating within the window, high CO/sub 2/ removal efficiency (effluent concentrations < 100 ppbv), high reactant utilization (> 99%), and an acceptable pressure drop across the bed (3 kPa/m at a superficial velocity of 13 cm/s) are possible. This paper addresses three areas of experimental investigation: (1) microscale studies on 150-mg samples to provide information concerning surface properties, kinetics, and equilibrium vapor pressures; (2) macroscale studies on large fixed beds (4.2 kg of reactant) to determine the effects of humidity, temperature, and gas flow rate upon bed pressure drop and CO/sub 2/ breakthrough; and (3) design, construction, and initial operation of a pilot unit capable of continuously processing a 34-m/sup 3//h (20-ft/sup 3//min) air-based gas stream.
Date: March 1, 1983
Creator: Haag, G.L.; Nehls, J.W. Jr. & Young, G.C.
Partner: UNT Libraries Government Documents Department

Improved spectrophotometric analysis of barium styphnate

Description: A spectrophotometric procedure to determine the purity of barium styphnate monohydrate based upon the absorbance of the styphnate ion at 326 and 413.3 nm has been developed. The purity is determined by comparing the absorbance of the styphnate ion in barium styphnate and in styphnic acid. Our investigation has shown that the molar absorptivity and lambda maxima of the styphnate ion are quite pH dependent; therefore, the pH is buffered to 6.8 to 7.0 with ammonium acetate. Under these conditions the molar absorptivity is 1.6 x 10/sup 4/ L/mol-cm. Analyses following the procedure in the Navy specification WS13444A using water were found to give low molar absorptivities (1.3 x 10/sup 4/ L/mol-cm) for the styphnic acid calibration resulting in erroneous values for barium styphnate purity.
Date: January 1, 1983
Creator: Brown, N E & Blasi, J A
Partner: UNT Libraries Government Documents Department

Stability of tetravalent actinides in perovskites

Description: This paper reports the first determination of the enthalpy of formation of a complex actinide(IV) oxide: ..delta..H/sup 0//sub f/ (BaUO/sub 3/, s, 298 K) = -1690 +- 10 kJ mol/sup -1/. The preparation and properties of this and other actinide(IV) complex oxides are described and are compared with other perovskites BaMO/sub 3/. The relative stabilities of tetravalent and hexavalent uranium in various environments are compared in terms of the oxidation-reduction behavior of uranium in geological nuclear waste storage media; in perovskite, uranium(IV) is very unstable in comparison with uranium(VI).
Date: January 1, 1983
Creator: Williams, C.W.; Morss, L.R. & Choi, I.K.
Partner: UNT Libraries Government Documents Department