X-ray Absorption Spectroscopy Investigation of Iodine Capture by Silver-Exchanged Mordenite
Abstract
Capture of radioactive iodine is a significant consideration during reprocessing of spent nuclear fuel and disposal of legacy wastes. While silver-exchanged mordenite (AgZ) is widely regarded as a benchmark material for assessing iodine adsorption performance, previous research efforts have largely focused on bulk material properties rather than the underpinning molecular interactions that achieve effective iodine capture. As a result, the fundamental understanding necessary to identify and mitigate deactivation pathways for the recycle of AgZ is not available. In this paper, we applied X-ray Absorption Fine Structure (XAFS) spectroscopy to investigate AgZ following activation, adsorption of iodine, regeneration, and recycle, observing no appreciable degradation in performance due to the highly controlled conditions under which the AgZ was maintained. Fits of the extended XAFS (EXAFS) data reveal complete formation of Ag0 nanoparticles upon treatment with H2, and confirm the formation of α-AgI within the mordenite channels in addition to surface γ/β-AgI nanoparticles following iodine exposure. Analysis of the nanoparticle size and fractional composition of α-AgI to γ/β-AgI supports ripening of surface nanoparticles as a function of recycle. Finally, this work provides a foundation for future investigation of AgZ deactivation under conditions relevant to spent nuclear fuel reprocessing.
- Authors:
-
[1];
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Syracuse Univ., NY (United States). Dept. of Biomedical and Chemical Engineering
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Syracuse Univ., NY (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Nuclear Energy (NE), Nuclear Reactor Technologies (NE-7). Nuclear Energy University Program (NEUP); USDOE Office of Science (SC)
- OSTI Identifier:
- 1376447
- Grant/Contract Number:
- AC05-00OR22725; AC02-06CH11357; NE0008275
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Industrial and Engineering Chemistry Research
- Additional Journal Information:
- Journal Volume: 56; Journal Issue: 16; Journal ID: ISSN 0888-5885
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Citation Formats
Abney, Carter W., Nan, Yue, and Tavlarides, Lawrence L. X-ray Absorption Spectroscopy Investigation of Iodine Capture by Silver-Exchanged Mordenite. United States: N. p., 2017.
Web. doi:10.1021/acs.iecr.7b00233.
Abney, Carter W., Nan, Yue, & Tavlarides, Lawrence L. X-ray Absorption Spectroscopy Investigation of Iodine Capture by Silver-Exchanged Mordenite. United States. https://doi.org/10.1021/acs.iecr.7b00233
Abney, Carter W., Nan, Yue, and Tavlarides, Lawrence L. Wed .
"X-ray Absorption Spectroscopy Investigation of Iodine Capture by Silver-Exchanged Mordenite". United States. https://doi.org/10.1021/acs.iecr.7b00233. https://www.osti.gov/servlets/purl/1376447.
@article{osti_1376447,
title = {X-ray Absorption Spectroscopy Investigation of Iodine Capture by Silver-Exchanged Mordenite},
author = {Abney, Carter W. and Nan, Yue and Tavlarides, Lawrence L.},
abstractNote = {Capture of radioactive iodine is a significant consideration during reprocessing of spent nuclear fuel and disposal of legacy wastes. While silver-exchanged mordenite (AgZ) is widely regarded as a benchmark material for assessing iodine adsorption performance, previous research efforts have largely focused on bulk material properties rather than the underpinning molecular interactions that achieve effective iodine capture. As a result, the fundamental understanding necessary to identify and mitigate deactivation pathways for the recycle of AgZ is not available. In this paper, we applied X-ray Absorption Fine Structure (XAFS) spectroscopy to investigate AgZ following activation, adsorption of iodine, regeneration, and recycle, observing no appreciable degradation in performance due to the highly controlled conditions under which the AgZ was maintained. Fits of the extended XAFS (EXAFS) data reveal complete formation of Ag0 nanoparticles upon treatment with H2, and confirm the formation of α-AgI within the mordenite channels in addition to surface γ/β-AgI nanoparticles following iodine exposure. Analysis of the nanoparticle size and fractional composition of α-AgI to γ/β-AgI supports ripening of surface nanoparticles as a function of recycle. Finally, this work provides a foundation for future investigation of AgZ deactivation under conditions relevant to spent nuclear fuel reprocessing.},
doi = {10.1021/acs.iecr.7b00233},
journal = {Industrial and Engineering Chemistry Research},
number = 16,
volume = 56,
place = {United States},
year = {Wed Mar 29 00:00:00 EDT 2017},
month = {Wed Mar 29 00:00:00 EDT 2017}
}
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Works referenced in this record:
Life Cycle Greenhouse Gas Emissions of Coal-Fired Electricity Generation: Systematic Review and Harmonization
journal, April 2012
- Whitaker, Michael; Heath, Garvin A.; O’Donoughue, Patrick
- Journal of Industrial Ecology, Vol. 16
Why nuclear energy is sustainable and has to be part of the energy mix
journal, December 2014
- Brook, Barry W.; Alonso, Agustin; Meneley, Daniel A.
- Sustainable Materials and Technologies, Vol. 1-2
The energetic implications of curtailing versus storing solar- and wind-generated electricity
journal, January 2013
- Barnhart, Charles J.; Dale, Michael; Brandt, Adam R.
- Energy & Environmental Science, Vol. 6, Issue 10
Life Cycle Greenhouse Gas Emissions of Nuclear Electricity Generation: Systematic Review and Harmonization
journal, April 2012
- Warner, Ethan S.; Heath, Garvin A.
- Journal of Industrial Ecology, Vol. 16
Life Cycle Greenhouse Gas Emissions of Utility-Scale Wind Power: Systematic Review and Harmonization
journal, March 2012
- Dolan, Stacey L.; Heath, Garvin A.
- Journal of Industrial Ecology, Vol. 16
Life Cycle Greenhouse Gas Emissions of Trough and Tower Concentrating Solar Power Electricity Generation: Systematic Review and Harmonization
journal, April 2012
- Burkhardt, John J.; Heath, Garvin; Cohen, Elliot
- Journal of Industrial Ecology, Vol. 16
Life Cycle Greenhouse Gas Emissions of Crystalline Silicon Photovoltaic Electricity Generation: Systematic Review and Harmonization
journal, March 2012
- Hsu, David D.; O’Donoughue, Patrick; Fthenakis, Vasilis
- Journal of Industrial Ecology, Vol. 16
Capture of harmful radioactive contaminants from off-gas stream using porous solid sorbents for clean environment – A review
journal, December 2016
- Nandanwar, Sachin U.; Coldsnow, Kai; Utgikar, Vivek
- Chemical Engineering Journal, Vol. 306
The mass transfer dynamics of gaseous methyl-iodide adsorption by silver-exchanged sodium mordenite
report, December 1994
- Jubin, R. T.
Radioactive Iodine and Krypton Control for Nuclear Fuel Reprocessing Facilities
journal, January 2013
- Soelberg, Nick R.; Garn, Troy G.; Greenhalgh, Mitchell R.
- Science and Technology of Nuclear Installations, Vol. 2013
Materials and processes for the effective capture and immobilization of radioiodine: A review
journal, March 2016
- Riley, Brian J.; Vienna, John D.; Strachan, Denis M.
- Journal of Nuclear Materials, Vol. 470
Chalcogen-Based Aerogels As Sorbents for Radionuclide Remediation
journal, June 2013
- Riley, Brian J.; Chun, Jaehun; Um, Wooyong
- Environmental Science & Technology, Vol. 47, Issue 13
Polyacrylonitrile-Chalcogel Hybrid Sorbents for Radioiodine Capture
journal, April 2014
- Riley, Brian J.; Pierce, David A.; Chun, Jaehun
- Environmental Science & Technology, Vol. 48, Issue 10
Chalcogenide Aerogels as Sorbents for Radioactive Iodine
journal, March 2015
- Subrahmanyam, K. S.; Sarma, Debajit; Malliakas, Christos D.
- Chemistry of Materials, Vol. 27, Issue 7
Capture of Volatile Iodine, a Gaseous Fission Product, by Zeolitic Imidazolate Framework-8
journal, August 2011
- Sava, Dorina F.; Rodriguez, Mark A.; Chapman, Karena W.
- Journal of the American Chemical Society, Vol. 133, Issue 32
Competitive I 2 Sorption by Cu-BTC from Humid Gas Streams
journal, June 2013
- Sava, Dorina F.; Chapman, Karena W.; Rodriguez, Mark A.
- Chemistry of Materials, Vol. 25, Issue 13
Trapping Guests within a Nanoporous Metal–Organic Framework through Pressure-Induced Amorphization
journal, November 2011
- Chapman, Karena W.; Sava, Dorina F.; Halder, Gregory J.
- Journal of the American Chemical Society, Vol. 133, Issue 46
Thermochemical Evidence for Strong Iodine Chemisorption by ZIF-8
journal, October 2013
- Hughes, James T.; Sava, Dorina F.; Nenoff, Tina M.
- Journal of the American Chemical Society, Vol. 135, Issue 44
Iodine Confinement into Metal–Organic Frameworks (MOFs): Low-Temperature Sintering Glasses To Form Novel Glass Composite Material (GCM) Alternative Waste Forms
journal, May 2011
- Sava, Dorina F.; Garino, Terry J.; Nenoff, Tina M.
- Industrial & Engineering Chemistry Research, Vol. 51, Issue 2
In silico screening of metal organic framework for iodine capture and storage
journal, August 2014
- Assfour, Bassem; Assaad, Thaer; Odeh, Adnan
- Chemical Physics Letters, Vol. 610-611
Synthesis and characterization of ETS-10: supported hollow carbon nano-polyhedrons nanosorbent for adsorption of krypton at near ambient temperatures
journal, October 2015
- Nandanwar, Sachin U.; Coldsnow, Kai; Utgikar, Vivek
- Adsorption, Vol. 22, Issue 2
XPS Characterization of Silver Exchanged ETS-10 and Mordenite Molecular Sieves
journal, May 2009
- Anson, A.; Maham, Y.; Lin, C. C. H.
- Journal of Nanoscience and Nanotechnology, Vol. 9, Issue 5
A Study of Silver Species on Silver-Exchanged ETS-10 and Mordenite by XRD, SEM and Solid-State 109 Ag, 29 Si and 27 Al NMR Spectroscopy
journal, August 2012
- Liu, Yan; Chen, Fu; Wasylishen, Roderick E.
- Journal of Nanoscience and Nanotechnology, Vol. 12, Issue 8
Iodine adsorption on silver-exchanged titania-derived adsorbents
journal, June 2014
- Wu, Lan; Sawada, James A.; Kuznicki, Daniel B.
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 302, Issue 1
Novel synthesis of bismuth-based adsorbents for the removal of 129I in off-gas
journal, February 2015
- Yang, Jae Hwan; Shin, Jin Myeong; Park, Jang Jin
- Journal of Nuclear Materials, Vol. 457
Bismuth-embedded SBA-15 mesoporous silica for radioactive iodine capture and stable storage
journal, October 2015
- Yang, Jae Hwan; Cho, Yong-Jun; Shin, Jin Myeong
- Journal of Nuclear Materials, Vol. 465
Comparative Study on Adsorption of Iodine Vapor by Silica-Supported Cu Nanoparticles and Micronized Copper
journal, November 2012
- Outokesh, Mohammad; Saket, Arezoo; Ahmadi, Seyed Javad
- Industrial & Engineering Chemistry Research, Vol. 51, Issue 47
Airborne elemental iodine loading capacities of metal zeolites and a method for recycling silver zeolite
report, July 1977
- Thomas, T. R.; Staples, B. A.; Murphy, L. P.
Methyl iodide sorption by reduced silver mordenite
report, June 1983
- Scheele, R. D.; Burger, L. L.; Matsuzaki, C. L.
Adsorption of iodine on hydrogen-reduced silver-exchanged mordenite: Experiments and modeling
journal, August 2016
- Nan, Yue; Tavlarides, Lawrence L.; DePaoli, David W.
- AIChE Journal, Vol. 63, Issue 3
Radioactive Iodine Capture in Silver-Containing Mordenites through Nanoscale Silver Iodide Formation
journal, July 2010
- Chapman, Karena W.; Chupas, Peter J.; Nenoff, Tina M.
- Journal of the American Chemical Society, Vol. 132, Issue 26
Selective Recovery of Dynamic Guest Structure in a Nanoporous Prussian Blue through in Situ X-ray Diffraction: A Differential Pair Distribution Function Analysis
journal, August 2005
- Chapman, Karena W.; Chupas, Peter J.; Kepert, Cameron J.
- Journal of the American Chemical Society, Vol. 127, Issue 32
Determining Quantitative Kinetics and the Structural Mechanism for Particle Growth in Porous Templates
journal, October 2011
- Zhao, Haiyan; Nenoff, Tina M.; Jennings, Guy
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 21
Silver-mordenite for radiologic gas capture from complex streams: Dual catalytic CH3I decomposition and I confinement
journal, December 2014
- Nenoff, Tina M.; Rodriguez, Mark A.; Soelberg, Nick R.
- Microporous and Mesoporous Materials, Vol. 200
EXAFS: Basic Principles and Data Analysis
book, January 1986
- Teo, Boon K.
- Inorganic Chemistry Concepts
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005
- Ravel, B.; Newville, M.
- Journal of Synchrotron Radiation, Vol. 12, Issue 4
Theoretical approaches to x-ray absorption fine structure
journal, July 2000
- Rehr, J. J.; Albers, R. C.
- Reviews of Modern Physics, Vol. 72, Issue 3
High-temperature X-ray diffractometer
journal, March 1959
- Spreadborough, J.; Christian, J. W.
- Journal of Scientific Instruments, Vol. 36, Issue 3
The crystal structure of silver oxide (Ag 2 O)
journal, March 1922
- Wyckoff, R. W. G.
- American Journal of Science, Vol. s5-3, Issue 15
The Crystal Structure of Hexagonal Silver Iodide
journal, November 1935
- Helmholz, Lindsay
- The Journal of Chemical Physics, Vol. 3, Issue 11
The structure of superionic compounds by powder neutron diffraction. I. Cation distribution in α-AgI
journal, July 1977
- Wright, A. F.; Fender, B. E. F.
- Journal of Physics C: Solid State Physics, Vol. 10, Issue 13
Estimation of mean size and shape of small metal particles by EXAFS
journal, January 1999
- Jentys, Andreas
- Physical Chemistry Chemical Physics, Vol. 1, Issue 17
Modeling the Structure and Composition of Nanoparticles by Extended X-Ray Absorption Fine-Structure Spectroscopy
journal, July 2011
- Frenkel, Anatoly I.; Yevick, Aaron; Cooper, Chana
- Annual Review of Analytical Chemistry, Vol. 4, Issue 1
A Novel Method to Control the Size of Silver Nanoparticles Formed on Chabazite
journal, April 2009
- Liu, Yan; Chen, Fu; Kuznicki, Steven M.
- Journal of Nanoscience and Nanotechnology, Vol. 9, Issue 4
Local Structure of Thermally Stable Super Ionic Conducting AgI Confined in Mesopores
journal, October 2014
- Yamada, Hirotoshi; Saruwatari, Isamu; Kuwata, Naoaki
- The Journal of Physical Chemistry C, Vol. 118, Issue 41
Position and Dynamics of Ag Ions in Superionic AgI Using Extended X-Ray Absorption Fine Structure
journal, June 1977
- Boyce, J. B.; Hayes, T. M.; Stutius, W.
- Physical Review Letters, Vol. 38, Issue 23
Superionics: crystal structures and conduction processes
journal, June 2004
- Hull, Stephen
- Reports on Progress in Physics, Vol. 67, Issue 7