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Title: A THEORETICAL INVESTIGATION OF RADIOLYTIC H2 GENERATION FROM SOLIDS

Abstract

Hydrogen generation from materials in nuclear materials storage is of critical interest due to the potential for pressurization and/or flammability issues. Studies have focused on aqueous systems or those with minor amounts of physisorbed water, since conventional knowledge identifies the radiolytic decomposition of water as the source of H{sub 2} gas. Furthermore, the approach to characterize gas generation is typically strictly empirical, relying on determination of G-values from which production in systems is estimated. Interestingly, exploratory work at SRNL1 on gamma exposure to fully-dried solids with chemically-bound water that are typical of those produced on aluminium-clad nuclear fuel in reactor and post-discharge storage has shown a profound production of hydrogen (as the sole gaseous species) from fully dried boehmite ({gamma}-AlOOH or Al{sub 2}O{sub 3} {center_dot} H{sub 2}O) powders and no observable hydrogen from gibbsite ({gamma}-Al(OH){sub 3} or Al{sub 2}O{sub 3} {center_dot} 3H{sub 2}O) under gamma irradiation from cobalt-60. This observation is significant in that gibbsite is known to thermally decompose at 80 C whereas boehmite is stable to 400 C. Radiation damage can have various effects on solids, including heating, bond breaking, and rearrangements in the bonding structure. For example, a molecule can be ionized resulting in the generation ofmore » free electrons which can, in turn, ionize another molecule. Alternately, reactive radical species such as {lg_bullet}OH or cation species may be formed, which can go on to change bonding structures.« less

Authors:
; ;
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1034528
Report Number(s):
SRNL-STI-2011-00630
TRN: US1200879
DOE Contract Number:  
DE-AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; BONDING; CATIONS; COBALT 60; ELECTRONS; FLAMMABILITY; GIBBSITE; HEATING; HYDROGEN; IRRADIATION; NUCLEAR FUELS; PRESSURIZATION; PRODUCTION; RADIATIONS; RADICALS; STORAGE; WATER

Citation Formats

Westbrook, M, Sindelar, R, and Fisher, D. A THEORETICAL INVESTIGATION OF RADIOLYTIC H2 GENERATION FROM SOLIDS. United States: N. p., 2012. Web. doi:10.2172/1034528.
Westbrook, M, Sindelar, R, & Fisher, D. A THEORETICAL INVESTIGATION OF RADIOLYTIC H2 GENERATION FROM SOLIDS. United States. https://doi.org/10.2172/1034528
Westbrook, M, Sindelar, R, and Fisher, D. 2012. "A THEORETICAL INVESTIGATION OF RADIOLYTIC H2 GENERATION FROM SOLIDS". United States. https://doi.org/10.2172/1034528. https://www.osti.gov/servlets/purl/1034528.
@article{osti_1034528,
title = {A THEORETICAL INVESTIGATION OF RADIOLYTIC H2 GENERATION FROM SOLIDS},
author = {Westbrook, M and Sindelar, R and Fisher, D},
abstractNote = {Hydrogen generation from materials in nuclear materials storage is of critical interest due to the potential for pressurization and/or flammability issues. Studies have focused on aqueous systems or those with minor amounts of physisorbed water, since conventional knowledge identifies the radiolytic decomposition of water as the source of H{sub 2} gas. Furthermore, the approach to characterize gas generation is typically strictly empirical, relying on determination of G-values from which production in systems is estimated. Interestingly, exploratory work at SRNL1 on gamma exposure to fully-dried solids with chemically-bound water that are typical of those produced on aluminium-clad nuclear fuel in reactor and post-discharge storage has shown a profound production of hydrogen (as the sole gaseous species) from fully dried boehmite ({gamma}-AlOOH or Al{sub 2}O{sub 3} {center_dot} H{sub 2}O) powders and no observable hydrogen from gibbsite ({gamma}-Al(OH){sub 3} or Al{sub 2}O{sub 3} {center_dot} 3H{sub 2}O) under gamma irradiation from cobalt-60. This observation is significant in that gibbsite is known to thermally decompose at 80 C whereas boehmite is stable to 400 C. Radiation damage can have various effects on solids, including heating, bond breaking, and rearrangements in the bonding structure. For example, a molecule can be ionized resulting in the generation of free electrons which can, in turn, ionize another molecule. Alternately, reactive radical species such as {lg_bullet}OH or cation species may be formed, which can go on to change bonding structures.},
doi = {10.2172/1034528},
url = {https://www.osti.gov/biblio/1034528}, journal = {},
number = ,
volume = ,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2012},
month = {Wed Feb 01 00:00:00 EST 2012}
}