Silver-mordenite for radiologic gas capture from complex streams. Dual catalytic CH3I decomposition and I confinement
Abstract
The selective capture of radiological iodine (129I) is a persistent concern for safe nuclear energy. In these nuclear fuel reprocessing scenarios, the gas streams to be treated are extremely complex, containing several distinct iodine-containing molecules amongst a large variety of other species. Silver-containing mordenite (MOR) is a longstanding benchmark for radioiodine capture, reacting with molecular iodine (I2) to form AgI. However the mechanisms for organoiodine capture is not well understood. Here we investigate the capture of methyl iodide from complex mixed gas streams by combining chemical analysis of the effluent gas stream with in depth characterization of the recovered sorbent. Tools applied include infrared spectroscopy, thermogravimetric analysis with mass spectrometry, micro X-ray fluorescence, powder X-ray diffraction analysis, and pair distribution function analysis. Moreover, the MOR zeolite catalyzes decomposition of the methyl iodide through formation of surface methoxy species (SMS), which subsequently reacts with water in the mixed gas stream to form methanol, and with methanol to form dimethyl ether, which are both detected downstream in the effluent. The liberated iodine reacts with Ag in the MOR pore to the form subnanometer AgI clusters, smaller than the MOR pores, suggesting that the iodine is both physically and chemically confined within themore »
- Authors:
-
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Idaho National Lab. (INL), Idaho Falls, ID (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1140755
- Report Number(s):
- SAND-2014-1157J
Journal ID: ISSN 1387-1811; PII: S1387181114002273; TRN: US1600451
- Grant/Contract Number:
- AC04-94AL85000
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Microporous and Mesoporous Materials
- Additional Journal Information:
- Journal Volume: 200; Journal Issue: C; Journal ID: ISSN 1387-1811
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 07 ISOTOPE AND RADIATION SOURCES; mordenite; methyl iodide; synchrotron; pair distribution function (PDF); fission gas capture
Citation Formats
Nenoff, Tina M., Rodriguez, Mark A., Soelberg, Nick R., and Chapman, Karena W. Silver-mordenite for radiologic gas capture from complex streams. Dual catalytic CH3I decomposition and I confinement. United States: N. p., 2014.
Web. doi:10.1016/j.micromeso.2014.04.041.
Nenoff, Tina M., Rodriguez, Mark A., Soelberg, Nick R., & Chapman, Karena W. Silver-mordenite for radiologic gas capture from complex streams. Dual catalytic CH3I decomposition and I confinement. United States. https://doi.org/10.1016/j.micromeso.2014.04.041
Nenoff, Tina M., Rodriguez, Mark A., Soelberg, Nick R., and Chapman, Karena W. Fri .
"Silver-mordenite for radiologic gas capture from complex streams. Dual catalytic CH3I decomposition and I confinement". United States. https://doi.org/10.1016/j.micromeso.2014.04.041. https://www.osti.gov/servlets/purl/1140755.
@article{osti_1140755,
title = {Silver-mordenite for radiologic gas capture from complex streams. Dual catalytic CH3I decomposition and I confinement},
author = {Nenoff, Tina M. and Rodriguez, Mark A. and Soelberg, Nick R. and Chapman, Karena W.},
abstractNote = {The selective capture of radiological iodine (129I) is a persistent concern for safe nuclear energy. In these nuclear fuel reprocessing scenarios, the gas streams to be treated are extremely complex, containing several distinct iodine-containing molecules amongst a large variety of other species. Silver-containing mordenite (MOR) is a longstanding benchmark for radioiodine capture, reacting with molecular iodine (I2) to form AgI. However the mechanisms for organoiodine capture is not well understood. Here we investigate the capture of methyl iodide from complex mixed gas streams by combining chemical analysis of the effluent gas stream with in depth characterization of the recovered sorbent. Tools applied include infrared spectroscopy, thermogravimetric analysis with mass spectrometry, micro X-ray fluorescence, powder X-ray diffraction analysis, and pair distribution function analysis. Moreover, the MOR zeolite catalyzes decomposition of the methyl iodide through formation of surface methoxy species (SMS), which subsequently reacts with water in the mixed gas stream to form methanol, and with methanol to form dimethyl ether, which are both detected downstream in the effluent. The liberated iodine reacts with Ag in the MOR pore to the form subnanometer AgI clusters, smaller than the MOR pores, suggesting that the iodine is both physically and chemically confined within the zeolite.},
doi = {10.1016/j.micromeso.2014.04.041},
journal = {Microporous and Mesoporous Materials},
number = C,
volume = 200,
place = {United States},
year = {Fri May 09 00:00:00 EDT 2014},
month = {Fri May 09 00:00:00 EDT 2014}
}
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