Scoping evaluation of trace isotopic ratios within the noble metal-phase as indicators of reactor class
ORIGEN-ARP is used to simulate nine fuel types (six reactor classes) in a scoping study investigating potential isotopic indicators contained within the noble metal phase formed in used nuclear fuel. A concurrent effort compares predictions of these noble metal phase isotopic inventories to measured...
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Veröffentlicht in: | Progress in nuclear energy (New series) 2019-11, Vol.117 (C), p.103059, Article 103059 |
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description | ORIGEN-ARP is used to simulate nine fuel types (six reactor classes) in a scoping study investigating potential isotopic indicators contained within the noble metal phase formed in used nuclear fuel. A concurrent effort compares predictions of these noble metal phase isotopic inventories to measured values in three approved testing materials (ATMs) of various burnups ranging from 28 to 70 MWd/kgM. The noble metal phase elements (Mo-Tc-Ru-Rh-Pd-Te) are chemically unreactive and remain undissolved following dissolution as a fine black residue. This characteristic is appealing for nuclear forensics or nuclear archeology, in which information is often sought regarding fuel burnup and reactor class in order to verify past operating declarations. Intra-element isotope ratio predictions that compare favorably to the chemical measurements of the three ATMs are plotted as a function of burnup to determine the feasibility to distinguish reactor class or burnup. This evaluation of intra-elemental isotope ratios specific to the noble metal phase provides a prospect to determine reactor class from remaining, undissolved solids following reprocessing. This would be particularly valuable in assessing the source of used nuclear fuel at an undeclared reprocessing facility. Results of predicted isotope ratios are reported that show promise as indicators at low burnups ( |
doi_str_mv | 10.1016/j.pnucene.2019.103059 |
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•Six of 18 intra-element noble metal phase isotope ratios predicted by ORIGEN-ARP compare within 10% of measured values.•Ru 100/104 isotopic ratio serves a burnup indicator for unknown reactor type.•Reactors fueled with natural U distinguishable at low burnup (<5 MWd/kgM).•Pd 105/110 vs Ru 100/104 is proposed for further consideration as a low burnup indicator of reactor class.</description><identifier>ISSN: 0149-1970</identifier><identifier>EISSN: 1878-4224</identifier><identifier>DOI: 10.1016/j.pnucene.2019.103059</identifier><language>eng</language><publisher>Oxford: Elsevier Ltd</publisher><subject>Archaeology ; Dissolution ; Epsilon phase ; Evaluation ; Indicators ; Irradiated fuel ; Isotope ratios ; Isotopes ; Noble metals ; Nuclear archeology ; Nuclear forensics ; Nuclear fuel reprocessing ; Nuclear reactors ; Organic chemistry ; Palladium ; Phase transitions ; Predictions ; Spent nuclear fuels</subject><ispartof>Progress in nuclear energy (New series), 2019-11, Vol.117 (C), p.103059, Article 103059</ispartof><rights>2019 Elsevier Ltd</rights><rights>Copyright Elsevier BV Nov 2019</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c411t-5b2a867aab9059e3a973993dcd40e435545c3d01426a940e40794be0048e52a73</citedby><cites>FETCH-LOGICAL-c411t-5b2a867aab9059e3a973993dcd40e435545c3d01426a940e40794be0048e52a73</cites><orcidid>0000-0002-7573-4215 ; 0000-0003-4463-3929 ; 0000000275734215 ; 0000000344633929</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0149197019301544$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>230,314,776,780,881,3537,27901,27902,65534</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1776399$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Palmer, Camille J.</creatorcontrib><creatorcontrib>Gerez, Kyzer R.</creatorcontrib><creatorcontrib>Schwantes, Jon M.</creatorcontrib><creatorcontrib>Clark, Richard A.</creatorcontrib><title>Scoping evaluation of trace isotopic ratios within the noble metal-phase as indicators of reactor class</title><title>Progress in nuclear energy (New series)</title><description>ORIGEN-ARP is used to simulate nine fuel types (six reactor classes) in a scoping study investigating potential isotopic indicators contained within the noble metal phase formed in used nuclear fuel. A concurrent effort compares predictions of these noble metal phase isotopic inventories to measured values in three approved testing materials (ATMs) of various burnups ranging from 28 to 70 MWd/kgM. The noble metal phase elements (Mo-Tc-Ru-Rh-Pd-Te) are chemically unreactive and remain undissolved following dissolution as a fine black residue. This characteristic is appealing for nuclear forensics or nuclear archeology, in which information is often sought regarding fuel burnup and reactor class in order to verify past operating declarations. Intra-element isotope ratio predictions that compare favorably to the chemical measurements of the three ATMs are plotted as a function of burnup to determine the feasibility to distinguish reactor class or burnup. This evaluation of intra-elemental isotope ratios specific to the noble metal phase provides a prospect to determine reactor class from remaining, undissolved solids following reprocessing. This would be particularly valuable in assessing the source of used nuclear fuel at an undeclared reprocessing facility. Results of predicted isotope ratios are reported that show promise as indicators at low burnups (<5 MWd/kgM) and are compared to the measurements at higher burnups for the three ATMs.
•Six of 18 intra-element noble metal phase isotope ratios predicted by ORIGEN-ARP compare within 10% of measured values.•Ru 100/104 isotopic ratio serves a burnup indicator for unknown reactor type.•Reactors fueled with natural U distinguishable at low burnup (<5 MWd/kgM).•Pd 105/110 vs Ru 100/104 is proposed for further consideration as a low burnup indicator of reactor class.</description><subject>Archaeology</subject><subject>Dissolution</subject><subject>Epsilon phase</subject><subject>Evaluation</subject><subject>Indicators</subject><subject>Irradiated fuel</subject><subject>Isotope ratios</subject><subject>Isotopes</subject><subject>Noble metals</subject><subject>Nuclear archeology</subject><subject>Nuclear forensics</subject><subject>Nuclear fuel reprocessing</subject><subject>Nuclear reactors</subject><subject>Organic chemistry</subject><subject>Palladium</subject><subject>Phase transitions</subject><subject>Predictions</subject><subject>Spent nuclear fuels</subject><issn>0149-1970</issn><issn>1878-4224</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2019</creationdate><recordtype>article</recordtype><recordid>eNqFUE1LAzEUDKJgrf4EIeh5a7KbNM1JRPyCggf1HF6zr23KNlmTVPHfu2G9e3qPN_OGmSHkkrMZZ3x-s5v1_mDR46xmXA-3hkl9RCZ8oRaVqGtxTCaMC11xrdgpOUtpxxhXXMoJ2bzZ0Du_ofgF3QGyC56GNc0RLFKXQh5QS2MBEv12ees8zVukPqw6pHvM0FX9FhJSSNT51lnIIaaiERHssFPbQUrn5GQNXcKLvzklH48P7_fP1fL16eX-bllZwXmu5KqGxVwBrPSQARvQqtG6aW0rGIpGSiFt0w5h6jnocmJKixUyJhYoa1DNlFyNuiFlZ5J1Ge3WBu_RZsOVmhe5KbkeSX0MnwdM2ezCIfrBl6kbzmUtBSssObJsDClFXJs-uj3EH8OZKcWbnfkr3pTizVj88Hc7_uGQ88thLDbQW2xdLC7a4P5R-AV8l45O</recordid><startdate>201911</startdate><enddate>201911</enddate><creator>Palmer, Camille J.</creator><creator>Gerez, Kyzer R.</creator><creator>Schwantes, Jon M.</creator><creator>Clark, Richard A.</creator><general>Elsevier Ltd</general><general>Elsevier BV</general><general>Elsevier</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7TB</scope><scope>8FD</scope><scope>FR3</scope><scope>KR7</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0002-7573-4215</orcidid><orcidid>https://orcid.org/0000-0003-4463-3929</orcidid><orcidid>https://orcid.org/0000000275734215</orcidid><orcidid>https://orcid.org/0000000344633929</orcidid></search><sort><creationdate>201911</creationdate><title>Scoping evaluation of trace isotopic ratios within the noble metal-phase as indicators of reactor class</title><author>Palmer, Camille J. ; Gerez, Kyzer R. ; Schwantes, Jon M. ; Clark, Richard A.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c411t-5b2a867aab9059e3a973993dcd40e435545c3d01426a940e40794be0048e52a73</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2019</creationdate><topic>Archaeology</topic><topic>Dissolution</topic><topic>Epsilon phase</topic><topic>Evaluation</topic><topic>Indicators</topic><topic>Irradiated fuel</topic><topic>Isotope ratios</topic><topic>Isotopes</topic><topic>Noble metals</topic><topic>Nuclear archeology</topic><topic>Nuclear forensics</topic><topic>Nuclear fuel reprocessing</topic><topic>Nuclear reactors</topic><topic>Organic chemistry</topic><topic>Palladium</topic><topic>Phase transitions</topic><topic>Predictions</topic><topic>Spent nuclear fuels</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Palmer, Camille J.</creatorcontrib><creatorcontrib>Gerez, Kyzer R.</creatorcontrib><creatorcontrib>Schwantes, Jon M.</creatorcontrib><creatorcontrib>Clark, Richard A.</creatorcontrib><collection>CrossRef</collection><collection>Mechanical & Transportation Engineering Abstracts</collection><collection>Technology Research Database</collection><collection>Engineering Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>OSTI.GOV</collection><jtitle>Progress in nuclear energy (New series)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Palmer, Camille J.</au><au>Gerez, Kyzer R.</au><au>Schwantes, Jon M.</au><au>Clark, Richard A.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Scoping evaluation of trace isotopic ratios within the noble metal-phase as indicators of reactor class</atitle><jtitle>Progress in nuclear energy (New series)</jtitle><date>2019-11</date><risdate>2019</risdate><volume>117</volume><issue>C</issue><spage>103059</spage><pages>103059-</pages><artnum>103059</artnum><issn>0149-1970</issn><eissn>1878-4224</eissn><abstract>ORIGEN-ARP is used to simulate nine fuel types (six reactor classes) in a scoping study investigating potential isotopic indicators contained within the noble metal phase formed in used nuclear fuel. A concurrent effort compares predictions of these noble metal phase isotopic inventories to measured values in three approved testing materials (ATMs) of various burnups ranging from 28 to 70 MWd/kgM. The noble metal phase elements (Mo-Tc-Ru-Rh-Pd-Te) are chemically unreactive and remain undissolved following dissolution as a fine black residue. This characteristic is appealing for nuclear forensics or nuclear archeology, in which information is often sought regarding fuel burnup and reactor class in order to verify past operating declarations. Intra-element isotope ratio predictions that compare favorably to the chemical measurements of the three ATMs are plotted as a function of burnup to determine the feasibility to distinguish reactor class or burnup. This evaluation of intra-elemental isotope ratios specific to the noble metal phase provides a prospect to determine reactor class from remaining, undissolved solids following reprocessing. This would be particularly valuable in assessing the source of used nuclear fuel at an undeclared reprocessing facility. Results of predicted isotope ratios are reported that show promise as indicators at low burnups (<5 MWd/kgM) and are compared to the measurements at higher burnups for the three ATMs.
•Six of 18 intra-element noble metal phase isotope ratios predicted by ORIGEN-ARP compare within 10% of measured values.•Ru 100/104 isotopic ratio serves a burnup indicator for unknown reactor type.•Reactors fueled with natural U distinguishable at low burnup (<5 MWd/kgM).•Pd 105/110 vs Ru 100/104 is proposed for further consideration as a low burnup indicator of reactor class.</abstract><cop>Oxford</cop><pub>Elsevier Ltd</pub><doi>10.1016/j.pnucene.2019.103059</doi><orcidid>https://orcid.org/0000-0002-7573-4215</orcidid><orcidid>https://orcid.org/0000-0003-4463-3929</orcidid><orcidid>https://orcid.org/0000000275734215</orcidid><orcidid>https://orcid.org/0000000344633929</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Archaeology Dissolution Epsilon phase Evaluation Indicators Irradiated fuel Isotope ratios Isotopes Noble metals Nuclear archeology Nuclear forensics Nuclear fuel reprocessing Nuclear reactors Organic chemistry Palladium Phase transitions Predictions Spent nuclear fuels |
title | Scoping evaluation of trace isotopic ratios within the noble metal-phase as indicators of reactor class |
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