Ageing of EUROBITUM bituminised radioactive waste: An ATR-FTIR spectroscopy study
The extent of the physico-chemical processes of concern in the study of the acceptability of Eurobitum bituminised radioactive waste for underground disposal (water uptake by hygroscopic NaNO 3 – swelling – pressure build-up – NaNO 3 leaching) will depend on the degree of ageing of the bituminous ma...
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| Veröffentlicht in: | Journal of nuclear materials 2009-08, Vol.393 (1), p.175-185 |
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| creator | Valcke, E. Rorif, F. Smets, S. |
| description | The extent of the physico-chemical processes of concern in the study of the acceptability of Eurobitum bituminised radioactive waste for underground disposal (water uptake by hygroscopic NaNO
3 – swelling – pressure build-up – NaNO
3 leaching) will depend on the degree of ageing of the bituminous matrix. In the work reported here, the ageing behaviour was studied by comparing the characteristics of 25
years old radioactive Eurobitum with those of 25
years old non-radioactive Eurobitum samples that were heated or gamma-irradiated in the presence or absence of oxygen. Chemical changes in the bitumen structure were followed in the mid-infrared region with Attenuated Total Reflectance Fourier Transform InfraRed Spectroscopy (ATR-FTIR) by measuring the evolution of the band heights at 1700
cm
−1 (C
O functional groups) and 1600
cm
−1 (C
C double bonds). Needle penetration depths and ring and ball softening points were determined for some samples. Oxidation of bitumen in the presence of oxygen results in a distinct increase of both the number of C
O and C
C functionalities, with a positive linear relationship existing between the two groups. The production of C
O functional groups seems to promote the generation of C
C double bonds. Heating at 130
°C is much more efficient than gamma irradiation at low to moderate dose rates (20–140
Gy/h) to oxidise the bitumen. As the oxygen concentration decreases, for instance by diffusion limitation deeper inside the bitumen, the number of C
O and C
C functionalities formed per unit of time decreases. A similar behaviour was observed for 25
years old radioactive Eurobitum. In absence of oxygen, gamma irradiation still results in a small increase of the number of C
O functional groups, probably by oxygen still adsorbed on the bitumen, and in a relatively higher amount of C
C double bonds. The surface layer ( |
| doi_str_mv | 10.1016/j.jnucmat.2009.06.001 |
| format | Article |
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3 – swelling – pressure build-up – NaNO
3 leaching) will depend on the degree of ageing of the bituminous matrix. In the work reported here, the ageing behaviour was studied by comparing the characteristics of 25
years old radioactive Eurobitum with those of 25
years old non-radioactive Eurobitum samples that were heated or gamma-irradiated in the presence or absence of oxygen. Chemical changes in the bitumen structure were followed in the mid-infrared region with Attenuated Total Reflectance Fourier Transform InfraRed Spectroscopy (ATR-FTIR) by measuring the evolution of the band heights at 1700
cm
−1 (C
O functional groups) and 1600
cm
−1 (C
C double bonds). Needle penetration depths and ring and ball softening points were determined for some samples. Oxidation of bitumen in the presence of oxygen results in a distinct increase of both the number of C
O and C
C functionalities, with a positive linear relationship existing between the two groups. The production of C
O functional groups seems to promote the generation of C
C double bonds. Heating at 130
°C is much more efficient than gamma irradiation at low to moderate dose rates (20–140
Gy/h) to oxidise the bitumen. As the oxygen concentration decreases, for instance by diffusion limitation deeper inside the bitumen, the number of C
O and C
C functionalities formed per unit of time decreases. A similar behaviour was observed for 25
years old radioactive Eurobitum. In absence of oxygen, gamma irradiation still results in a small increase of the number of C
O functional groups, probably by oxygen still adsorbed on the bitumen, and in a relatively higher amount of C
C double bonds. The surface layer (<5
cm) of 25
years old radioactive Eurobitum was heavily oxidised. The material had become very hard and brittle, and was full of small fissures. Due to these fissures, radio-oxidation processes took also place deeper inside the waste. The consequences of these observations for the long-term behaviour of Eurobitum in underground disposal conditions are discussed.</description><identifier>ISSN: 0022-3115</identifier><identifier>EISSN: 1873-4820</identifier><identifier>DOI: 10.1016/j.jnucmat.2009.06.001</identifier><identifier>CODEN: JNUMAM</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Applied sciences ; Controled nuclear fusion plants ; Energy ; Energy. Thermal use of fuels ; Exact sciences and technology ; Fission nuclear power plants ; Fuels ; Installations for energy generation and conversion: thermal and electrical energy ; Nuclear fuels</subject><ispartof>Journal of nuclear materials, 2009-08, Vol.393 (1), p.175-185</ispartof><rights>2009 Elsevier B.V.</rights><rights>2009 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c371t-5ffbf975d636ddd83fdb036e4985a2de3d18c6e6545a24947b506ffddeb14d1f3</citedby><cites>FETCH-LOGICAL-c371t-5ffbf975d636ddd83fdb036e4985a2de3d18c6e6545a24947b506ffddeb14d1f3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.jnucmat.2009.06.001$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=21896131$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Valcke, E.</creatorcontrib><creatorcontrib>Rorif, F.</creatorcontrib><creatorcontrib>Smets, S.</creatorcontrib><title>Ageing of EUROBITUM bituminised radioactive waste: An ATR-FTIR spectroscopy study</title><title>Journal of nuclear materials</title><description>The extent of the physico-chemical processes of concern in the study of the acceptability of Eurobitum bituminised radioactive waste for underground disposal (water uptake by hygroscopic NaNO
3 – swelling – pressure build-up – NaNO
3 leaching) will depend on the degree of ageing of the bituminous matrix. In the work reported here, the ageing behaviour was studied by comparing the characteristics of 25
years old radioactive Eurobitum with those of 25
years old non-radioactive Eurobitum samples that were heated or gamma-irradiated in the presence or absence of oxygen. Chemical changes in the bitumen structure were followed in the mid-infrared region with Attenuated Total Reflectance Fourier Transform InfraRed Spectroscopy (ATR-FTIR) by measuring the evolution of the band heights at 1700
cm
−1 (C
O functional groups) and 1600
cm
−1 (C
C double bonds). Needle penetration depths and ring and ball softening points were determined for some samples. Oxidation of bitumen in the presence of oxygen results in a distinct increase of both the number of C
O and C
C functionalities, with a positive linear relationship existing between the two groups. The production of C
O functional groups seems to promote the generation of C
C double bonds. Heating at 130
°C is much more efficient than gamma irradiation at low to moderate dose rates (20–140
Gy/h) to oxidise the bitumen. As the oxygen concentration decreases, for instance by diffusion limitation deeper inside the bitumen, the number of C
O and C
C functionalities formed per unit of time decreases. A similar behaviour was observed for 25
years old radioactive Eurobitum. In absence of oxygen, gamma irradiation still results in a small increase of the number of C
O functional groups, probably by oxygen still adsorbed on the bitumen, and in a relatively higher amount of C
C double bonds. The surface layer (<5
cm) of 25
years old radioactive Eurobitum was heavily oxidised. The material had become very hard and brittle, and was full of small fissures. Due to these fissures, radio-oxidation processes took also place deeper inside the waste. The consequences of these observations for the long-term behaviour of Eurobitum in underground disposal conditions are discussed.</description><subject>Applied sciences</subject><subject>Controled nuclear fusion plants</subject><subject>Energy</subject><subject>Energy. Thermal use of fuels</subject><subject>Exact sciences and technology</subject><subject>Fission nuclear power plants</subject><subject>Fuels</subject><subject>Installations for energy generation and conversion: thermal and electrical energy</subject><subject>Nuclear fuels</subject><issn>0022-3115</issn><issn>1873-4820</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2009</creationdate><recordtype>article</recordtype><recordid>eNqFkF1LwzAUhoMoOD9-gpAb8ar1pGnS1huZw4-BIo7tOqTJiWRs7UxaZf_ejg1vvToceN7z8RByxSBlwOTtMl02vVnrLs0AqhRkCsCOyIiVBU_yMoNjMgLIsoQzJk7JWYxLABAViBH5GH-ibz5p6-jjYvb-MJ0v3mjtu37tGx_R0qCtb7Xp_DfSHx07vKPjho7ns-RpPp3RuEHThTaadrOlsevt9oKcOL2KeHmo52Tx9DifvCSv78_Tyfg1MbxgXSKcq11VCCu5tNaW3NkauMS8KoXOLHLLSiNRinxo8yovagHSOWuxZrlljp-Tm_3cTWi_eoydWvtocLXSDbZ9VMWQlAWvsoEUe9IMh8aATm2CX-uwVQzUzqBaqoNBtTOoQKrB4JC7PmzQ0eiVC7oxPv6FM1ZWkvEdd7_ncHj322NQ0XhsDFofBjvKtv6fTb-xOok-</recordid><startdate>20090815</startdate><enddate>20090815</enddate><creator>Valcke, E.</creator><creator>Rorif, F.</creator><creator>Smets, S.</creator><general>Elsevier B.V</general><general>Elsevier</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7ST</scope><scope>7TV</scope><scope>C1K</scope><scope>SOI</scope></search><sort><creationdate>20090815</creationdate><title>Ageing of EUROBITUM bituminised radioactive waste: An ATR-FTIR spectroscopy study</title><author>Valcke, E. ; Rorif, F. ; Smets, S.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c371t-5ffbf975d636ddd83fdb036e4985a2de3d18c6e6545a24947b506ffddeb14d1f3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2009</creationdate><topic>Applied sciences</topic><topic>Controled nuclear fusion plants</topic><topic>Energy</topic><topic>Energy. Thermal use of fuels</topic><topic>Exact sciences and technology</topic><topic>Fission nuclear power plants</topic><topic>Fuels</topic><topic>Installations for energy generation and conversion: thermal and electrical energy</topic><topic>Nuclear fuels</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Valcke, E.</creatorcontrib><creatorcontrib>Rorif, F.</creatorcontrib><creatorcontrib>Smets, S.</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><collection>Environment Abstracts</collection><collection>Pollution Abstracts</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Environment Abstracts</collection><jtitle>Journal of nuclear materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Valcke, E.</au><au>Rorif, F.</au><au>Smets, S.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Ageing of EUROBITUM bituminised radioactive waste: An ATR-FTIR spectroscopy study</atitle><jtitle>Journal of nuclear materials</jtitle><date>2009-08-15</date><risdate>2009</risdate><volume>393</volume><issue>1</issue><spage>175</spage><epage>185</epage><pages>175-185</pages><issn>0022-3115</issn><eissn>1873-4820</eissn><coden>JNUMAM</coden><abstract>The extent of the physico-chemical processes of concern in the study of the acceptability of Eurobitum bituminised radioactive waste for underground disposal (water uptake by hygroscopic NaNO
3 – swelling – pressure build-up – NaNO
3 leaching) will depend on the degree of ageing of the bituminous matrix. In the work reported here, the ageing behaviour was studied by comparing the characteristics of 25
years old radioactive Eurobitum with those of 25
years old non-radioactive Eurobitum samples that were heated or gamma-irradiated in the presence or absence of oxygen. Chemical changes in the bitumen structure were followed in the mid-infrared region with Attenuated Total Reflectance Fourier Transform InfraRed Spectroscopy (ATR-FTIR) by measuring the evolution of the band heights at 1700
cm
−1 (C
O functional groups) and 1600
cm
−1 (C
C double bonds). Needle penetration depths and ring and ball softening points were determined for some samples. Oxidation of bitumen in the presence of oxygen results in a distinct increase of both the number of C
O and C
C functionalities, with a positive linear relationship existing between the two groups. The production of C
O functional groups seems to promote the generation of C
C double bonds. Heating at 130
°C is much more efficient than gamma irradiation at low to moderate dose rates (20–140
Gy/h) to oxidise the bitumen. As the oxygen concentration decreases, for instance by diffusion limitation deeper inside the bitumen, the number of C
O and C
C functionalities formed per unit of time decreases. A similar behaviour was observed for 25
years old radioactive Eurobitum. In absence of oxygen, gamma irradiation still results in a small increase of the number of C
O functional groups, probably by oxygen still adsorbed on the bitumen, and in a relatively higher amount of C
C double bonds. The surface layer (<5
cm) of 25
years old radioactive Eurobitum was heavily oxidised. The material had become very hard and brittle, and was full of small fissures. Due to these fissures, radio-oxidation processes took also place deeper inside the waste. The consequences of these observations for the long-term behaviour of Eurobitum in underground disposal conditions are discussed.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.jnucmat.2009.06.001</doi><tpages>11</tpages></addata></record> |
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| subjects | Applied sciences Controled nuclear fusion plants Energy Energy. Thermal use of fuels Exact sciences and technology Fission nuclear power plants Fuels Installations for energy generation and conversion: thermal and electrical energy Nuclear fuels |
| title | Ageing of EUROBITUM bituminised radioactive waste: An ATR-FTIR spectroscopy study |
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