Metal-Organic Frameworks for Removal of Xe and Kr from Nuclear Fuel Reprocessing Plants

被引:169
作者
Liu, Jian [1 ]
Thallapally, Praveen K. [1 ]
Strachan, Denis [1 ]
机构
[1] Pacific NW Natl Lab, Energy & Environm Directorate, Richland, WA 99352 USA
关键词
MONTE-CARLO SIMULATIONS; ACTIVATED-CHARCOAL; ROOM-TEMPERATURE; NOBLE-GASES; ADSORPTION; SEPARATION; XENON; CO2; CAPTURE; KRYPTON;
D O I
10.1021/la301870n
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Removal of xenon (Xe) and krypton (Kr) from process off-gases containing 400 ppm Xe, 40 ppm Kr, 78% N-2, 21% O-2, 0.9% Ar, 0.03% CO2, and so forth using adsorption was demonstrated for the first time. Two well-known metal-organic frameworks (MOFs), HKUST-1 and Ni/DOBDC, which both have unsaturated metal centers but different pore morphologies, were selected as novel adsorbents. Results of an activated carbon were also included for comparison. The Ni/DOBDC has higher Xe/Kr selectivities than those of the activated carbon and the HKUST-1. In addition, results show that the Ni/DOBDC and HKUST-1 can adsorb substantial amounts of Xe and Kr even when they are mixed in air. Moreover, the Ni/DOBDC can successfully separate 400 ppm Xe from 40 ppm Kr and air containing O-2, N-2, and CO2 with a Xe/Ke selectivity of 7.3 as indicated by our breakthrough results. This shows a promising future for MOFs in radioactive nuclide separations from spent fuels.
引用
收藏
页码:11584 / 11589
页数:6
相关论文
共 27 条
  • [1] High Propene/Propane Selectivity in Isostructural Metal-Organic Frameworks with High Densities of Open Metal Sites
    Bae, Youn-Sang
    Lee, Chang Yeon
    Kim, Ki Chul
    Farha, Omar K.
    Nickias, Peter
    Hupp, Joseph T.
    Nguyen, SonBinh T.
    Snurr, Randall Q.
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (08) : 1857 - 1860
  • [2] Adsorption equilibria of O2, Ar, Kr and Xe on activated carbon and zeolites: single component and mixture data
    Bazan, R. E.
    Bastos-Neto, M.
    Moeller, A.
    Dreisbach, F.
    Staudt, R.
    [J]. ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY, 2011, 17 (02): : 371 - 383
  • [3] Application of metal-organic frameworks with coordinatively unsaturated metal sites in storage and separation of methane and carbon dioxide
    Dietzel, Pascal D. C.
    Besikiotis, Vasileios
    Blom, Richard
    [J]. JOURNAL OF MATERIALS CHEMISTRY, 2009, 19 (39) : 7362 - 7370
  • [4] Farha OK, 2010, NAT CHEM, V2, P944, DOI [10.1038/NCHEM.834, 10.1038/nchem.834]
  • [5] FEREY G, 2011, CHEM SOC REV, V40, P550, DOI DOI 10.1039/c0cs00040j
  • [6] Switching Kr/Xe Selectivity with Temperature in a Metal-Organic Framework
    Fernandez, Carlos A.
    Liu, Jian
    Thallapally, Praveen K.
    Strachan, Denis M.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (22) : 9046 - 9049
  • [7] Ultrahigh Porosity in Metal-Organic Frameworks
    Furukawa, Hiroyasu
    Ko, Nakeun
    Go, Yong Bok
    Aratani, Naoki
    Choi, Sang Beom
    Choi, Eunwoo
    Yazaydin, A. Oezguer
    Snurr, Randall Q.
    O'Keeffe, Michael
    Kim, Jaheon
    Yaghi, Omar M.
    [J]. SCIENCE, 2010, 329 (5990) : 424 - 428
  • [8] Adsorption and Separation of Noble Gases by IRMOF-1: Grand Canonical Monte Carlo Simulations
    Greathouse, Jeffery A.
    Kinnibrugh, Tiffany L.
    Allendorf, Mark D.
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2009, 48 (07) : 3425 - 3431
  • [9] Atomically Detailed Modeling of Metal Organic Frameworks for Adsorption, Diffusion, and Separation of Noble Gas Mixtures
    Gurdal, Yeliz
    Keskin, Seda
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2012, 51 (21) : 7373 - 7382
  • [10] CO2 and CH4 Separation by Adsorption Using Cu-BTC Metal-Organic Framework
    Hamon, Lomig
    Jolimaitre, Elsa
    Pirngruber, Gerhard D.
    [J]. INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (16) : 7497 - 7503