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Title: 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 Ag 0 nanoparticles upon treatment with H 2, 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:
ORCiD logo [1];  [2];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Syracuse Univ., NY (United States). Dept. of Biomedical and Chemical Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (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:
Journal Article: 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. doi: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. doi: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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