Effects of moisture and aging upon decomposition of methyl iodide by reduced silver mordenite
Reduced silver mordenite has been considered as a sorbent for the capture of organic iodides, especially methyl iodide, from off-gases produced by aqueous used nuclear fuel reprocessing operations. The adsorption capacity of this material has been unpredictable especially when NO x and water are pre...
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Veröffentlicht in: | Adsorption : journal of the International Adsorption Society 2024, Vol.30 (6), p.915-924 |
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description | Reduced silver mordenite has been considered as a sorbent for the capture of organic iodides, especially methyl iodide, from off-gases produced by aqueous used nuclear fuel reprocessing operations. The adsorption capacity of this material has been unpredictable especially when NO
x
and water are present. Previous work has found that a catalytic decomposition reaction is occurring on the surface but few determinations have been made of the kinetics of this reaction. The work presented tested the adsorption behavior and apparent catalytic reaction rate in humid conditions and compared those to dry conditions testing. Both experiments observed a first order reaction with rate constants of 0.0847 L/g sorbent/s and 0.1202 L/g sorbent/s respectively. Such a reduction in apparent rate constant is possibly due to either water obstructing methyl iodide adsorption or product desorption limitation. Changes in the adsorption profile were also apparent between these two, with the humid conditions experiment reaching saturation sooner than the dry conditions experiment. Additionally, an experiment into the effects of sorbent storage in a controlled laboratory environment was performed. The performance of the sorbent materials that were stored with silver in the zerovalent state was slightly inferior to those materials that were stored in ionic form (Ag
+
) and reduced to zerovalent silver immediately prior to subjecting them to sorption test. The materials stored with silver in the ionic form (and reduced just prior to application) behaved essentially similarly to the freshly synthesized (and reduced) sorbents in the sorption tests. This suggests that zerovalent silver experiences some oxidation resulting in deactivation of some sites. |
doi_str_mv | 10.1007/s10450-024-00473-8 |
format | Article |
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x
and water are present. Previous work has found that a catalytic decomposition reaction is occurring on the surface but few determinations have been made of the kinetics of this reaction. The work presented tested the adsorption behavior and apparent catalytic reaction rate in humid conditions and compared those to dry conditions testing. Both experiments observed a first order reaction with rate constants of 0.0847 L/g sorbent/s and 0.1202 L/g sorbent/s respectively. Such a reduction in apparent rate constant is possibly due to either water obstructing methyl iodide adsorption or product desorption limitation. Changes in the adsorption profile were also apparent between these two, with the humid conditions experiment reaching saturation sooner than the dry conditions experiment. Additionally, an experiment into the effects of sorbent storage in a controlled laboratory environment was performed. The performance of the sorbent materials that were stored with silver in the zerovalent state was slightly inferior to those materials that were stored in ionic form (Ag
+
) and reduced to zerovalent silver immediately prior to subjecting them to sorption test. The materials stored with silver in the ionic form (and reduced just prior to application) behaved essentially similarly to the freshly synthesized (and reduced) sorbents in the sorption tests. This suggests that zerovalent silver experiences some oxidation resulting in deactivation of some sites.</description><identifier>ISSN: 0929-5607</identifier><identifier>EISSN: 1572-8757</identifier><identifier>DOI: 10.1007/s10450-024-00473-8</identifier><language>eng</language><publisher>New York: Springer US</publisher><subject>Adsorption ; Chemistry ; Chemistry and Materials Science ; Decomposition reactions ; Engineering Thermodynamics ; Heat and Mass Transfer ; Industrial Chemistry/Chemical Engineering ; Moisture effects ; Nuclear capture ; Nuclear fuel reprocessing ; Oxidation ; Rate constants ; Reaction kinetics ; Silver ; Sorbents ; Sorption ; Spent nuclear fuels ; Surfaces and Interfaces ; Thin Films</subject><ispartof>Adsorption : journal of the International Adsorption Society, 2024, Vol.30 (6), p.915-924</ispartof><rights>The Author(s) 2024</rights><rights>The Author(s) 2024. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c341t-e7fcbcba3ced78c177da6659393c46825395d1655762e756969b86a3220c41593</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s10450-024-00473-8$$EPDF$$P50$$Gspringer$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s10450-024-00473-8$$EHTML$$P50$$Gspringer$$Hfree_for_read</linktohtml><link.rule.ids>230,314,776,780,881,27901,27902,41464,42533,51294</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/2339653$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Goettsche, Heinrik</creatorcontrib><creatorcontrib>Raja, Krishnan</creatorcontrib><creatorcontrib>Sabbarwall, Piyush</creatorcontrib><creatorcontrib>Utgikar, Vivek</creatorcontrib><title>Effects of moisture and aging upon decomposition of methyl iodide by reduced silver mordenite</title><title>Adsorption : journal of the International Adsorption Society</title><addtitle>Adsorption</addtitle><description>Reduced silver mordenite has been considered as a sorbent for the capture of organic iodides, especially methyl iodide, from off-gases produced by aqueous used nuclear fuel reprocessing operations. The adsorption capacity of this material has been unpredictable especially when NO
x
and water are present. Previous work has found that a catalytic decomposition reaction is occurring on the surface but few determinations have been made of the kinetics of this reaction. The work presented tested the adsorption behavior and apparent catalytic reaction rate in humid conditions and compared those to dry conditions testing. Both experiments observed a first order reaction with rate constants of 0.0847 L/g sorbent/s and 0.1202 L/g sorbent/s respectively. Such a reduction in apparent rate constant is possibly due to either water obstructing methyl iodide adsorption or product desorption limitation. Changes in the adsorption profile were also apparent between these two, with the humid conditions experiment reaching saturation sooner than the dry conditions experiment. Additionally, an experiment into the effects of sorbent storage in a controlled laboratory environment was performed. The performance of the sorbent materials that were stored with silver in the zerovalent state was slightly inferior to those materials that were stored in ionic form (Ag
+
) and reduced to zerovalent silver immediately prior to subjecting them to sorption test. The materials stored with silver in the ionic form (and reduced just prior to application) behaved essentially similarly to the freshly synthesized (and reduced) sorbents in the sorption tests. This suggests that zerovalent silver experiences some oxidation resulting in deactivation of some sites.</description><subject>Adsorption</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Decomposition reactions</subject><subject>Engineering Thermodynamics</subject><subject>Heat and Mass Transfer</subject><subject>Industrial Chemistry/Chemical Engineering</subject><subject>Moisture effects</subject><subject>Nuclear capture</subject><subject>Nuclear fuel reprocessing</subject><subject>Oxidation</subject><subject>Rate constants</subject><subject>Reaction kinetics</subject><subject>Silver</subject><subject>Sorbents</subject><subject>Sorption</subject><subject>Spent nuclear fuels</subject><subject>Surfaces and Interfaces</subject><subject>Thin Films</subject><issn>0929-5607</issn><issn>1572-8757</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><sourceid>C6C</sourceid><recordid>eNp9kM1KAzEURoMoWKsv4CroevQmmSSTpZT6AwU3upQwk2TalHYyJjNC397UEdy5ChfOd27uh9A1gTsCIO8TgZJDAbQsAErJiuoEzQiXtKgkl6doBoqqgguQ5-gipS0AKCHZDH0s29aZIeHQ4n3waRijw3Vncb323RqPfeiwdSbs-5D84PN0BN2wOeywD9Zbh5sDjs6Oxlmc_O7LxSyK1nV-cJforK13yV39vnP0_rh8WzwXq9enl8XDqjCsJEPhZGsa09QsO2RliJS2FoIrppgpRUU5U9wSwbkU1EkulFBNJWpGKZiSZG6ObiZvSIPXyeTVZmNC1-XTNGVMCc4ydDtBfQyfo0uD3oYxdvlfmoEihAGnR4pOlIkhpeha3Ue_r-NBE9DHrvXUtc5d65-udZVDbAqlDHdrF__U_6S-ASrjgNw</recordid><startdate>2024</startdate><enddate>2024</enddate><creator>Goettsche, Heinrik</creator><creator>Raja, Krishnan</creator><creator>Sabbarwall, Piyush</creator><creator>Utgikar, Vivek</creator><general>Springer US</general><general>Springer Nature B.V</general><general>Springer Science + Business Media</general><scope>C6C</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope></search><sort><creationdate>2024</creationdate><title>Effects of moisture and aging upon decomposition of methyl iodide by reduced silver mordenite</title><author>Goettsche, Heinrik ; Raja, Krishnan ; Sabbarwall, Piyush ; Utgikar, Vivek</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c341t-e7fcbcba3ced78c177da6659393c46825395d1655762e756969b86a3220c41593</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Adsorption</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Decomposition reactions</topic><topic>Engineering Thermodynamics</topic><topic>Heat and Mass Transfer</topic><topic>Industrial Chemistry/Chemical Engineering</topic><topic>Moisture effects</topic><topic>Nuclear capture</topic><topic>Nuclear fuel reprocessing</topic><topic>Oxidation</topic><topic>Rate constants</topic><topic>Reaction kinetics</topic><topic>Silver</topic><topic>Sorbents</topic><topic>Sorption</topic><topic>Spent nuclear fuels</topic><topic>Surfaces and Interfaces</topic><topic>Thin Films</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Goettsche, Heinrik</creatorcontrib><creatorcontrib>Raja, Krishnan</creatorcontrib><creatorcontrib>Sabbarwall, Piyush</creatorcontrib><creatorcontrib>Utgikar, Vivek</creatorcontrib><collection>Springer Nature OA Free Journals</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>Adsorption : journal of the International Adsorption Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Goettsche, Heinrik</au><au>Raja, Krishnan</au><au>Sabbarwall, Piyush</au><au>Utgikar, Vivek</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Effects of moisture and aging upon decomposition of methyl iodide by reduced silver mordenite</atitle><jtitle>Adsorption : journal of the International Adsorption Society</jtitle><stitle>Adsorption</stitle><date>2024</date><risdate>2024</risdate><volume>30</volume><issue>6</issue><spage>915</spage><epage>924</epage><pages>915-924</pages><issn>0929-5607</issn><eissn>1572-8757</eissn><abstract>Reduced silver mordenite has been considered as a sorbent for the capture of organic iodides, especially methyl iodide, from off-gases produced by aqueous used nuclear fuel reprocessing operations. The adsorption capacity of this material has been unpredictable especially when NO
x
and water are present. Previous work has found that a catalytic decomposition reaction is occurring on the surface but few determinations have been made of the kinetics of this reaction. The work presented tested the adsorption behavior and apparent catalytic reaction rate in humid conditions and compared those to dry conditions testing. Both experiments observed a first order reaction with rate constants of 0.0847 L/g sorbent/s and 0.1202 L/g sorbent/s respectively. Such a reduction in apparent rate constant is possibly due to either water obstructing methyl iodide adsorption or product desorption limitation. Changes in the adsorption profile were also apparent between these two, with the humid conditions experiment reaching saturation sooner than the dry conditions experiment. Additionally, an experiment into the effects of sorbent storage in a controlled laboratory environment was performed. The performance of the sorbent materials that were stored with silver in the zerovalent state was slightly inferior to those materials that were stored in ionic form (Ag
+
) and reduced to zerovalent silver immediately prior to subjecting them to sorption test. The materials stored with silver in the ionic form (and reduced just prior to application) behaved essentially similarly to the freshly synthesized (and reduced) sorbents in the sorption tests. This suggests that zerovalent silver experiences some oxidation resulting in deactivation of some sites.</abstract><cop>New York</cop><pub>Springer US</pub><doi>10.1007/s10450-024-00473-8</doi><tpages>10</tpages><oa>free_for_read</oa></addata></record> |
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subjects | Adsorption Chemistry Chemistry and Materials Science Decomposition reactions Engineering Thermodynamics Heat and Mass Transfer Industrial Chemistry/Chemical Engineering Moisture effects Nuclear capture Nuclear fuel reprocessing Oxidation Rate constants Reaction kinetics Silver Sorbents Sorption Spent nuclear fuels Surfaces and Interfaces Thin Films |
title | Effects of moisture and aging upon decomposition of methyl iodide by reduced silver mordenite |
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