Interactions of HCl and H2O with the surface of PuO2
In order to explore the potential of heat treatment to decontaminate chloride-contaminated legacy plutonium dioxide (PuO2) powders from the UK stockpile, samples retrieved from storage have been heated in air from 400 to 950 °C. These samples also contain high levels of other adsorbed gases from the...
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| Veröffentlicht in: | Journal of Nuclear Materials 2019-05, Vol.518, p.256-264 |
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| creator | Sutherland-Harper, Sophie Livens, Francis Pearce, Carolyn Hobbs, Jeff Orr, Robin Taylor, Robin Webb, Kevin Kaltsoyannis, Nikolas |
| description | In order to explore the potential of heat treatment to decontaminate chloride-contaminated legacy plutonium dioxide (PuO2) powders from the UK stockpile, samples retrieved from storage have been heated in air from 400 to 950 °C. These samples also contain high levels of other adsorbed gases from the atmosphere, including water. The amounts of chloride remaining on the PuO2 particles after heat treatment (measured by a caustic leaching process) decrease whilst the amounts of volatilised chloride increase with increasing heat treatment temperature. Clear evidence for a non-leachable (strongly bound) chloride species on the PuO2 surface is found from the thermal treatments. The lattice parameter decreases with increasing heat treatment temperature, reflecting annealing of structural defects caused by over 35 years of radiation damage, with no change in the fcc Fm3¯m crystal structure. Heating chloride-contaminated PuO2 powder to ∼230 °C and cooling back to ambient temperature in a sealed vessel reveals the production of H2, He, NO and CO gases. Water adsorption/desorption behaviour with the untreated PuO2 powder is remarkably different than PuO2 which had previously been heat treated at 700 °C. From thermal treatments in open and sealed systems it is concluded that water and chloride co-adsorb and interact on the PuO2 surface and each affects the adsorption/desorption behaviour of the other. These data also support practical considerations for repackaging of chloride-contaminated PuO2 for long term safe and secure storage at Sellafield.
[Display omitted]
•First study of UK chloride-contaminated PuO2 retrieved from storage.•>700 °C needed to volatilise chloride efficiently.•Evidence of leachable and non-leachable species on PuO2 surface.•Unusual water adsorption behaviour on chloride-contaminated PuO2. |
| doi_str_mv | 10.1016/j.jnucmat.2019.02.036 |
| format | Article |
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[Display omitted]
•First study of UK chloride-contaminated PuO2 retrieved from storage.•>700 °C needed to volatilise chloride efficiently.•Evidence of leachable and non-leachable species on PuO2 surface.•Unusual water adsorption behaviour on chloride-contaminated PuO2.</description><identifier>ISSN: 0022-3115</identifier><identifier>EISSN: 1873-4820</identifier><identifier>DOI: 10.1016/j.jnucmat.2019.02.036</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Adsorbed water ; Adsorption ; Ambient temperature ; Caustic leaching ; Chloride ; Chlorides ; Contamination ; Crystal defects ; Crystal structure ; Decontamination ; Defect annealing ; Desorption ; Gases ; Heat treating ; Heat treatment ; Leaching ; Plutonium ; Plutonium dioxide ; Powder ; Radiation ; Radiation damage ; Stockpiling ; Storage ; Structural damage ; Surface chemistry ; Temperature effects ; Thermal treatment ; Water</subject><ispartof>Journal of Nuclear Materials, 2019-05, Vol.518, p.256-264</ispartof><rights>2019 Elsevier B.V.</rights><rights>Copyright Elsevier BV May 2019</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c341t-eda70f5b2a37e1f3b21f20fe5d67fb5343d53ab85673a417ca008c2f15152573</citedby><cites>FETCH-LOGICAL-c341t-eda70f5b2a37e1f3b21f20fe5d67fb5343d53ab85673a417ca008c2f15152573</cites><orcidid>0000-0003-3098-1615 ; 0000-0002-3685-277X ; 0000-0003-0293-5742</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.jnucmat.2019.02.036$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,881,3536,27903,27904,45974</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1530589$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Sutherland-Harper, Sophie</creatorcontrib><creatorcontrib>Livens, Francis</creatorcontrib><creatorcontrib>Pearce, Carolyn</creatorcontrib><creatorcontrib>Hobbs, Jeff</creatorcontrib><creatorcontrib>Orr, Robin</creatorcontrib><creatorcontrib>Taylor, Robin</creatorcontrib><creatorcontrib>Webb, Kevin</creatorcontrib><creatorcontrib>Kaltsoyannis, Nikolas</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><title>Interactions of HCl and H2O with the surface of PuO2</title><title>Journal of Nuclear Materials</title><description>In order to explore the potential of heat treatment to decontaminate chloride-contaminated legacy plutonium dioxide (PuO2) powders from the UK stockpile, samples retrieved from storage have been heated in air from 400 to 950 °C. These samples also contain high levels of other adsorbed gases from the atmosphere, including water. The amounts of chloride remaining on the PuO2 particles after heat treatment (measured by a caustic leaching process) decrease whilst the amounts of volatilised chloride increase with increasing heat treatment temperature. Clear evidence for a non-leachable (strongly bound) chloride species on the PuO2 surface is found from the thermal treatments. The lattice parameter decreases with increasing heat treatment temperature, reflecting annealing of structural defects caused by over 35 years of radiation damage, with no change in the fcc Fm3¯m crystal structure. Heating chloride-contaminated PuO2 powder to ∼230 °C and cooling back to ambient temperature in a sealed vessel reveals the production of H2, He, NO and CO gases. Water adsorption/desorption behaviour with the untreated PuO2 powder is remarkably different than PuO2 which had previously been heat treated at 700 °C. From thermal treatments in open and sealed systems it is concluded that water and chloride co-adsorb and interact on the PuO2 surface and each affects the adsorption/desorption behaviour of the other. These data also support practical considerations for repackaging of chloride-contaminated PuO2 for long term safe and secure storage at Sellafield.
[Display omitted]
•First study of UK chloride-contaminated PuO2 retrieved from storage.•>700 °C needed to volatilise chloride efficiently.•Evidence of leachable and non-leachable species on PuO2 surface.•Unusual water adsorption behaviour on chloride-contaminated PuO2.</description><subject>Adsorbed water</subject><subject>Adsorption</subject><subject>Ambient temperature</subject><subject>Caustic leaching</subject><subject>Chloride</subject><subject>Chlorides</subject><subject>Contamination</subject><subject>Crystal defects</subject><subject>Crystal structure</subject><subject>Decontamination</subject><subject>Defect annealing</subject><subject>Desorption</subject><subject>Gases</subject><subject>Heat treating</subject><subject>Heat treatment</subject><subject>Leaching</subject><subject>Plutonium</subject><subject>Plutonium dioxide</subject><subject>Powder</subject><subject>Radiation</subject><subject>Radiation damage</subject><subject>Stockpiling</subject><subject>Storage</subject><subject>Structural damage</subject><subject>Surface chemistry</subject><subject>Temperature effects</subject><subject>Thermal treatment</subject><subject>Water</subject><issn>0022-3115</issn><issn>1873-4820</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNqFkMFKAzEQhoMoWKuPICx63nWSbDbpSaSoLRTqofeQzSY0S5toklV8e3dp757mMN8__PMhdI-hwoCbp77q_aCPKlcE8KICUgFtLtAMC07LWhC4RDMAQkqKMbtGNyn1AMAWwGaoXvtsotLZBZ-KYIvV8lAo3xUrsi1-XN4XeW-KNESrtJn2H8OW3KIrqw7J3J3nHO3eXnfLVbnZvq-XL5tS0xrn0nSKg2UtUZQbbGlLsCVgDesabltGa9oxqlrBGk5VjblWAEITixlmhHE6Rw-nsyFlJ5N22ei9Dt4bnSVmFJhYjNDjCfqM4WswKcs-DNGPtSQhhAvKBYiRYidKx5BSNFZ-RndU8VdikJNE2cuzRDlJlEDkKHHMPZ9yZnzz25k41TBem87FqUUX3D8X_gD233nz</recordid><startdate>20190501</startdate><enddate>20190501</enddate><creator>Sutherland-Harper, Sophie</creator><creator>Livens, Francis</creator><creator>Pearce, Carolyn</creator><creator>Hobbs, Jeff</creator><creator>Orr, Robin</creator><creator>Taylor, Robin</creator><creator>Webb, Kevin</creator><creator>Kaltsoyannis, Nikolas</creator><general>Elsevier B.V</general><general>Elsevier BV</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7QQ</scope><scope>7SR</scope><scope>7ST</scope><scope>7TB</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>JG9</scope><scope>L7M</scope><scope>SOI</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0003-3098-1615</orcidid><orcidid>https://orcid.org/0000-0002-3685-277X</orcidid><orcidid>https://orcid.org/0000-0003-0293-5742</orcidid></search><sort><creationdate>20190501</creationdate><title>Interactions of HCl and H2O with the surface of PuO2</title><author>Sutherland-Harper, Sophie ; Livens, Francis ; Pearce, Carolyn ; Hobbs, Jeff ; Orr, Robin ; Taylor, Robin ; Webb, Kevin ; Kaltsoyannis, Nikolas</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c341t-eda70f5b2a37e1f3b21f20fe5d67fb5343d53ab85673a417ca008c2f15152573</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Adsorbed water</topic><topic>Adsorption</topic><topic>Ambient temperature</topic><topic>Caustic leaching</topic><topic>Chloride</topic><topic>Chlorides</topic><topic>Contamination</topic><topic>Crystal defects</topic><topic>Crystal structure</topic><topic>Decontamination</topic><topic>Defect annealing</topic><topic>Desorption</topic><topic>Gases</topic><topic>Heat treating</topic><topic>Heat treatment</topic><topic>Leaching</topic><topic>Plutonium</topic><topic>Plutonium dioxide</topic><topic>Powder</topic><topic>Radiation</topic><topic>Radiation damage</topic><topic>Stockpiling</topic><topic>Storage</topic><topic>Structural damage</topic><topic>Surface chemistry</topic><topic>Temperature effects</topic><topic>Thermal treatment</topic><topic>Water</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Sutherland-Harper, Sophie</creatorcontrib><creatorcontrib>Livens, Francis</creatorcontrib><creatorcontrib>Pearce, Carolyn</creatorcontrib><creatorcontrib>Hobbs, Jeff</creatorcontrib><creatorcontrib>Orr, Robin</creatorcontrib><creatorcontrib>Taylor, Robin</creatorcontrib><creatorcontrib>Webb, Kevin</creatorcontrib><creatorcontrib>Kaltsoyannis, Nikolas</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. 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(PNNL), Richland, WA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Interactions of HCl and H2O with the surface of PuO2</atitle><jtitle>Journal of Nuclear Materials</jtitle><date>2019-05-01</date><risdate>2019</risdate><volume>518</volume><spage>256</spage><epage>264</epage><pages>256-264</pages><issn>0022-3115</issn><eissn>1873-4820</eissn><abstract>In order to explore the potential of heat treatment to decontaminate chloride-contaminated legacy plutonium dioxide (PuO2) powders from the UK stockpile, samples retrieved from storage have been heated in air from 400 to 950 °C. These samples also contain high levels of other adsorbed gases from the atmosphere, including water. The amounts of chloride remaining on the PuO2 particles after heat treatment (measured by a caustic leaching process) decrease whilst the amounts of volatilised chloride increase with increasing heat treatment temperature. Clear evidence for a non-leachable (strongly bound) chloride species on the PuO2 surface is found from the thermal treatments. The lattice parameter decreases with increasing heat treatment temperature, reflecting annealing of structural defects caused by over 35 years of radiation damage, with no change in the fcc Fm3¯m crystal structure. Heating chloride-contaminated PuO2 powder to ∼230 °C and cooling back to ambient temperature in a sealed vessel reveals the production of H2, He, NO and CO gases. Water adsorption/desorption behaviour with the untreated PuO2 powder is remarkably different than PuO2 which had previously been heat treated at 700 °C. From thermal treatments in open and sealed systems it is concluded that water and chloride co-adsorb and interact on the PuO2 surface and each affects the adsorption/desorption behaviour of the other. These data also support practical considerations for repackaging of chloride-contaminated PuO2 for long term safe and secure storage at Sellafield.
[Display omitted]
•First study of UK chloride-contaminated PuO2 retrieved from storage.•>700 °C needed to volatilise chloride efficiently.•Evidence of leachable and non-leachable species on PuO2 surface.•Unusual water adsorption behaviour on chloride-contaminated PuO2.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.jnucmat.2019.02.036</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0003-3098-1615</orcidid><orcidid>https://orcid.org/0000-0002-3685-277X</orcidid><orcidid>https://orcid.org/0000-0003-0293-5742</orcidid><oa>free_for_read</oa></addata></record> |
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| ispartof | Journal of Nuclear Materials, 2019-05, Vol.518, p.256-264 |
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| source | Elsevier ScienceDirect Journals Complete |
| subjects | Adsorbed water Adsorption Ambient temperature Caustic leaching Chloride Chlorides Contamination Crystal defects Crystal structure Decontamination Defect annealing Desorption Gases Heat treating Heat treatment Leaching Plutonium Plutonium dioxide Powder Radiation Radiation damage Stockpiling Storage Structural damage Surface chemistry Temperature effects Thermal treatment Water |
| title | Interactions of HCl and H2O with the surface of PuO2 |
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