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Title: Sorption Modeling and Verification for Off-Gas Treatment

The project has made progress toward developing a comprehensive modeling capability for the capture of target species in off gas evolved during the reprocessing of nuclear fuel. The effort has integrated experimentation, model development, and computer code development for adsorption and absorption processes. For adsorption, a modeling library has been initiated to include (a) equilibrium models for uptake of off-gas components by adsorbents, (b) mass transfer models to describe mass transfer to a particle, diffusion through the pores of the particle and adsorption on the active sites of the particle, and (c) interconnection of these models to fixed bed adsorption modeling which includes advection through the bed. For single-component equilibria, a Generalized Statistical Thermodynamic Adsorption (GSTA) code was developed to represent experimental data from a broad range of isotherm types; this is equivalent to a Langmuir isotherm in the two-parameter case, and was demonstrated for Kr on INL-engineered sorbent HZ PAN, water sorption on molecular sieve A sorbent material (MS3A), and Kr and Xe capture on metal-organic framework (MOF) materials. The GSTA isotherm was extended to multicomponent systems through application of a modified spreading pressure surface activity model and generalized predictive adsorbed solution theory; the result is the capability tomore » estimate multicomponent adsorption equilibria from single-component isotherms. This advance, which enhances the capability to simulate systems related to off-gas treatment, has been demonstrated for a range of real-gas systems in the literature and is ready for testing with data currently being collected for multicomponent systems of interest, including iodine and water on MS3A. A diffusion kinetic model for sorbent pellets involving pore and surface diffusion as well as external mass transfer has been established, and a methodology was developed for determining unknown diffusivity parameters from transient uptake data. Two parallel approaches have been explored for integrating the kernels described above into a mass-transport model for adsorption in fixed beds. In one, the GSTA isotherm kernel has been incorporated into the MOOSE framework; in the other approach, a focused finite-difference framework and PDE kernels have been developed. Issues, including oscillatory behavior in MOOSE solutions to advection-diffusion problems, and opportunities have been identified for each approach, and a path forward has been identified toward developing a stronger modeling platform. Experimental systems were established for collection of microscopic kinetics and equilibria data for single and multicomponent uptake of gaseous species on solid sorbents. The systems, which can operate at ambient temperature to 250°C and dew points from -69 to 17°C, are useful for collecting data needed for modeling performance of sorbents of interest. Experiments were conducted to determine applicable models and parameters for isotherms and mass transfer for water and/or iodine adsorption on MS3A. Validation experiments were also conducted for water adsorption on fixed beds of MS3A. For absorption, work involved modeling with supportive experimentation. A dynamic model was developed to simulate CO2 absorption with chemical reaction using high alkaline content water solutions. A computer code was developed to implement the model based upon transient mass and energy balances. Experiments were conducted in a laboratory-scale column to determine model parameters. The influence of geometric parameters and operating variables on CO2 absorption was studied over a wide range of conditions. This project has resulted in 7 publications, with 3 manuscripts in preparation. Also, 15 presentations were given at national meetings of ANS and AIChE and at Material Recovery and Waste Forms Campaign Working Group meetings.« less
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ;  [4]
  1. Syracuse Univ., NY (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
  3. Prairie View A & M Univ., Prairie View, TX (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
OSTI Identifier:
1179788
Report Number(s):
DOE/NEUP--11-3175
11-3175; TRN: US1600275
DOE Contract Number:
AC07-05ID14517
Resource Type:
Technical Report
Research Org:
Syracuse Univ., NY (United States); Georgia Inst. of Technology, Atlanta, GA (United States); Prairie View A & M Univ., Prairie View, TX (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Nuclear Energy (NE). Nuclear Energy University Programs (NEUP)
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; OFF-GAS SYSTEMS; AQUEOUS SOLUTIONS; ADSORPTION; ADVECTION; ABSORPTION; NUCLEAR FUELS; ISOTHERMS; MOLECULAR SIEVES; IODINE; WATER; VALIDATION; EQUILIBRIUM; PARTIAL DIFFERENTIAL EQUATIONS; DIFFUSION; PACKED BEDS; KERNELS; PARTICLES; COMPUTER CODES; MATHEMATICAL SOLUTIONS; ORGANOMETALLIC COMPOUNDS; CAPTURE; GEOMETRY; REPROCESSING; VERIFICATION; AMBIENT TEMPERATURE; ENERGY BALANCE; KINETICS; LIBRARIES; PELLETS; PERFORMANCE; GASEOUS WASTES; COMPUTERIZED SIMULATION; MATHEMATICAL MODELS; MASS TRANSFER; FINITE DIFFERENCE METHOD; CARBON DIOXIDE; KRYPTON; XENON; TEMPERATURE RANGE 0400-1000 K