Silver-Exchanged Mordenite for Capture of Water Vapor in Off-Gas Streams: A Study of Adsorption Kinetics

被引:12
作者
Nan, Yue [1 ]
Liu, Jiuxu [1 ]
Tang, Siqi [1 ]
Lin, Ronghong [1 ,2 ]
Tavlarides, Lawrence L. [1 ]
机构
[1] Syracuse Univ, Dept Biomed & Chem Engn, 329 Link Hall, Syracuse, NY 13244 USA
[2] US DOE, Natl Energy Technol Lab, 626 Cochrans Mill Rd, Pittsburgh, PA 15236 USA
关键词
IODINE CAPTURE; RADIOIODINE; HYDROGEN;
D O I
10.1021/acs.iecr.7b04420
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Reduced silver-exchanged mordenite (Ag(0)Z) has been recognized as the benchmark adsorbent for radioactive iodine removal from the nuclear fuel reprocessing off-gases. It has also been shown to have a considerable adsorption capacity for water vapor, which is a major component (tritiated water) in the off-gases of spent nuclear fuel reprocessing facilities. Therefore, understanding the kinetics of water vapor adsorption on Ag(0)Z is necessary for a better design of off-gas treatment systems. The adsorption kinetics were studied through adsorption experiments of water vapor on Ag(0)Z pellets and analyses of the kinetic data with adsorption models that describe processes of mass transfer and inter/intracrystalline diffusion. Uptake curves of water vapor on Ag(0)Z pellets were obtained with a continuous-flow adsorption system at temperatures of 25, 40, 60, 100, 150, and 200 degrees C and dew points from -53.6 degrees C to 12.1 degrees C. The diffusion-controlling factors were determined experimentally and analytically. It was found that the diffusion process of water vapor in Ag(0)Z pellets was controlled by macropore diffusion. Gas film mass-transfer resistance also contributed to the adsorption process of the 0.9 mm Ag(0)Z pellets, but it could be minimized with a high gas velocity and small pellet radius. Kinetic models including macropore diffusion (MD), linear driving force (LDF) and shrinking core (SC) were used to fit the uptake curves. The macropore diffusivity for water vapor adsorption on Ag(0)Z pellets was determined using the three models. It was found that the LDF and SC models could well describe the kinetic process, while the fitting with the MD model was not quite as good due to the existence of external mass-transfer resistance for the 0.9 mm Ag(0)Z pellets.
引用
收藏
页码:1048 / 1058
页数:11
相关论文
共 39 条
[1]   NON-ISOTHERMAL ADSORPTION OF WATER BY SYNTHETIC NAX ZEOLITE PELLETS [J].
ABDALLAH, K ;
GRENIER, P ;
SUN, LM ;
MEUNIER, F .
CHEMICAL ENGINEERING SCIENCE, 1988, 43 (10) :2633-2643
[2]   X-ray Absorption Spectroscopy Investigation of Iodine Capture by Silver-Exchanged Mordenite [J].
Abney, Carter W. ;
Nan, Yue ;
Tavlarides, Lawrence L. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2017, 56 (16) :4837-4846
[3]  
[Anonymous], 1952, CHEM ENG PROG
[4]  
[Anonymous], 1998, ADSORPTION ANAL EQUI
[5]   Capture of elemental and organic iodine from dilute gas streams by silver-exchanged mordenite [J].
Bruffey, S. H. ;
Jubin, R. T. ;
Jordan, J. A. .
ATALANTE 2016 INTERNATIONAL CONFERENCE ON NUCLEAR CHEMISTRY FOR SUSTAINABLE FUEL CYCLES, 2016, 21 :293-299
[6]   Radioactive Iodine Capture in Silver-Containing Mordenites through Nanoscale Silver Iodide Formation [J].
Chapman, Karena W. ;
Chupas, Peter J. ;
Nenoff, Tina M. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (26) :8897-+
[7]   Performance of CuII-, PbII-, and HgII-Exchanged Mordenite in the Adsorption of I2, ICH3, H2O, CO, ClCH3, and Cl2: A Density Functional Study [J].
Chibani, Siwar ;
Medlej, Israa ;
Lebegue, Sebastien ;
Angyan, Janos G. ;
Cantrel, Laurent ;
Badawi, Michael .
CHEMPHYSCHEM, 2017, 18 (12) :1642-1652
[8]   A DFT investigation of the adsorption of iodine compounds and water in H-, Na-, Ag-, and Cu- mordenite [J].
Chibani, Siwar ;
Chebbi, Mouheb ;
Lebegue, Sebastien ;
Bucko, Tomas ;
Badawi, Michael .
JOURNAL OF CHEMICAL PHYSICS, 2016, 144 (24)
[9]   Localization of water molecules and sodium ions in Na-mordenite, by thermally stimulated current measurement [J].
Devautour, S ;
Abdoulaye, A ;
Giuntini, JC ;
Henn, F .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (38) :9297-9301
[10]   Effect of Water Adsorption on Cation-Surface Interaction Energy in the Na-Mordenite of 5.5: 1 Si/Al Ratio [J].
Diaby, Sekou .
JOURNAL OF CHEMISTRY, 2016, 2016