Affinity of An(VI) for N4-Tetradentate Donor Ligands: Complexation of the Actinyl(VI) Ions with N4-Tetradentate Ligands
In this report the affinity of four N 4 -tetradentate ligands that incorporate the 2-methylpyridyl functionality with hexavalent actinides has been investigated in methanol solution. The ligands studied include N,N′-bis(2-methylpyridyl)diaminoethane (BPMDAE), N,N′-bis(2-methylpyridyl)-1,3-diaminopro...
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| Veröffentlicht in: | Journal of solution chemistry 2012-05, Vol.41 (4), p.616-629 |
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| creator | Ogden, Mark D. Sinkov, Serguei I. Lumetta, Gregg J. Nash, Kenneth L. |
| description | In this report the affinity of four N
4
-tetradentate ligands that incorporate the 2-methylpyridyl functionality with hexavalent actinides
has been investigated in methanol solution. The ligands studied include N,N′-bis(2-methylpyridyl)diaminoethane (BPMDAE), N,N′-bis(2-methylpyridyl)-1,3-diaminopropane (BPMDAP), N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP), and trans-N,N-bis(2-pyridylmethyl)-1,2-diaminocyclohexane (BPMDAC). Conditional stability constants describing the strength of the interaction were determined by UV–visible spectrophotometry. The log
10
K
101
values for both U(VI) and Pu(VI) are comparable and show the same trend of stability with ligand structure. Dinuclear complexes are also indicated as being important. The log
10
K
201
values for Pu(VI) complexation with the N
4
-ligands are identical for the four ligands (within experimental error), indicating that the structure of the ligand backbone has little effect on the stability of the (PuO
2
)
2
L
2+
complex. The exception to this trend is the behavior of N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP) with Pu(VI). This ligand displays a tendency to reduce Pu(VI) within the experimental time frame of 45 minutes. BPMPIP is the only ligand tested that contains tertiary amines in the ligand backbone. The decomposition of BPMPIP by Pu(VI) suggests a susceptibility of tertiary amines to oxidative degradation. |
| doi_str_mv | 10.1007/s10953-012-9827-2 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_osti_</sourceid><recordid>TN_cdi_osti_scitechconnect_1043109</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>1671327474</sourcerecordid><originalsourceid>FETCH-LOGICAL-c2232-af01e7dad4eb238ad641e141aa74b95f272cf0ef56b8f65dcaf64d6aae2d5ca43</originalsourceid><addsrcrecordid>eNp9kUGPEyEUx4nRxLr6AbxNTEzWAwoMDDPemuquTRq9rF7JK_PYsplCBZq1317qNF5MPJHH-_1_h_cn5DVn7zlj-kPmbFAtZVzQoReaiidkwZUWtB-EfkoWrK7poHvxnLzI-YHVuR_kgjwunfPBl1MTXbMM1z_W7xoXU_NV0jssCUYMBQo2n2Kovxt_D2HMH5tV3B8m_AXFx3BOlh02S1t8OE1_FOsYcvPoy-4f0UXxkjxzMGV8dXmvyPebz3erL3Tz7Xa9Wm6oFaIVFBzjqEcYJW5F28PYSY5ccgAtt4NyQgvrGDrVbXvXqdGC6-TYAaAYlQXZXpE3szfm4k22vqDd2RgC2mI4k229W4WuZ-iQ4s8j5mL2PlucJggYj9nwTvNWaKnPPj6jNsWcEzpzSH4P6VRl5tyEmZswtQlzbsKImnl70UO2MLkEwfr8NyjU0HdK9ZUTM5frKtxjMg_xmEI9z3_kvwFuGpgG</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>1671327474</pqid></control><display><type>article</type><title>Affinity of An(VI) for N4-Tetradentate Donor Ligands: Complexation of the Actinyl(VI) Ions with N4-Tetradentate Ligands</title><source>SpringerLink Journals - AutoHoldings</source><creator>Ogden, Mark D. ; Sinkov, Serguei I. ; Lumetta, Gregg J. ; Nash, Kenneth L.</creator><creatorcontrib>Ogden, Mark D. ; Sinkov, Serguei I. ; Lumetta, Gregg J. ; Nash, Kenneth L. ; Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><description>In this report the affinity of four N
4
-tetradentate ligands that incorporate the 2-methylpyridyl functionality with hexavalent actinides
has been investigated in methanol solution. The ligands studied include N,N′-bis(2-methylpyridyl)diaminoethane (BPMDAE), N,N′-bis(2-methylpyridyl)-1,3-diaminopropane (BPMDAP), N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP), and trans-N,N-bis(2-pyridylmethyl)-1,2-diaminocyclohexane (BPMDAC). Conditional stability constants describing the strength of the interaction were determined by UV–visible spectrophotometry. The log
10
K
101
values for both U(VI) and Pu(VI) are comparable and show the same trend of stability with ligand structure. Dinuclear complexes are also indicated as being important. The log
10
K
201
values for Pu(VI) complexation with the N
4
-ligands are identical for the four ligands (within experimental error), indicating that the structure of the ligand backbone has little effect on the stability of the (PuO
2
)
2
L
2+
complex. The exception to this trend is the behavior of N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP) with Pu(VI). This ligand displays a tendency to reduce Pu(VI) within the experimental time frame of 45 minutes. BPMPIP is the only ligand tested that contains tertiary amines in the ligand backbone. The decomposition of BPMPIP by Pu(VI) suggests a susceptibility of tertiary amines to oxidative degradation.</description><identifier>ISSN: 0095-9782</identifier><identifier>EISSN: 1572-8927</identifier><identifier>DOI: 10.1007/s10953-012-9827-2</identifier><identifier>CODEN: JSLCAG</identifier><language>eng</language><publisher>Boston: Springer US</publisher><subject>ACTINIDES ; AFFINITY ; AMINES ; Backbone ; Chemistry ; Chemistry and Materials Science ; Complexation ; Condensed Matter Physics ; Exact sciences and technology ; General and physical chemistry ; Geochemistry ; Industrial Chemistry/Chemical Engineering ; Inorganic Chemistry ; Ligands ; METHANOL ; Methyl alcohol ; Nitrogen donor ligands ; Non-aqueous media ; Oceanography ; Physical Chemistry ; PIPERAZINES ; Plutonium ; RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY ; Solutions ; SPECTROPHOTOMETRY ; STABILITY ; Trends ; Uranium</subject><ispartof>Journal of solution chemistry, 2012-05, Vol.41 (4), p.616-629</ispartof><rights>Springer Science+Business Media, LLC 2012</rights><rights>2015 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c2232-af01e7dad4eb238ad641e141aa74b95f272cf0ef56b8f65dcaf64d6aae2d5ca43</citedby><cites>FETCH-LOGICAL-c2232-af01e7dad4eb238ad641e141aa74b95f272cf0ef56b8f65dcaf64d6aae2d5ca43</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/s10953-012-9827-2$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s10953-012-9827-2$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>230,314,780,784,885,27924,27925,41488,42557,51319</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=25986558$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1043109$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Ogden, Mark D.</creatorcontrib><creatorcontrib>Sinkov, Serguei I.</creatorcontrib><creatorcontrib>Lumetta, Gregg J.</creatorcontrib><creatorcontrib>Nash, Kenneth L.</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><title>Affinity of An(VI) for N4-Tetradentate Donor Ligands: Complexation of the Actinyl(VI) Ions with N4-Tetradentate Ligands</title><title>Journal of solution chemistry</title><addtitle>J Solution Chem</addtitle><description>In this report the affinity of four N
4
-tetradentate ligands that incorporate the 2-methylpyridyl functionality with hexavalent actinides
has been investigated in methanol solution. The ligands studied include N,N′-bis(2-methylpyridyl)diaminoethane (BPMDAE), N,N′-bis(2-methylpyridyl)-1,3-diaminopropane (BPMDAP), N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP), and trans-N,N-bis(2-pyridylmethyl)-1,2-diaminocyclohexane (BPMDAC). Conditional stability constants describing the strength of the interaction were determined by UV–visible spectrophotometry. The log
10
K
101
values for both U(VI) and Pu(VI) are comparable and show the same trend of stability with ligand structure. Dinuclear complexes are also indicated as being important. The log
10
K
201
values for Pu(VI) complexation with the N
4
-ligands are identical for the four ligands (within experimental error), indicating that the structure of the ligand backbone has little effect on the stability of the (PuO
2
)
2
L
2+
complex. The exception to this trend is the behavior of N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP) with Pu(VI). This ligand displays a tendency to reduce Pu(VI) within the experimental time frame of 45 minutes. BPMPIP is the only ligand tested that contains tertiary amines in the ligand backbone. The decomposition of BPMPIP by Pu(VI) suggests a susceptibility of tertiary amines to oxidative degradation.</description><subject>ACTINIDES</subject><subject>AFFINITY</subject><subject>AMINES</subject><subject>Backbone</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Complexation</subject><subject>Condensed Matter Physics</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Geochemistry</subject><subject>Industrial Chemistry/Chemical Engineering</subject><subject>Inorganic Chemistry</subject><subject>Ligands</subject><subject>METHANOL</subject><subject>Methyl alcohol</subject><subject>Nitrogen donor ligands</subject><subject>Non-aqueous media</subject><subject>Oceanography</subject><subject>Physical Chemistry</subject><subject>PIPERAZINES</subject><subject>Plutonium</subject><subject>RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY</subject><subject>Solutions</subject><subject>SPECTROPHOTOMETRY</subject><subject>STABILITY</subject><subject>Trends</subject><subject>Uranium</subject><issn>0095-9782</issn><issn>1572-8927</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2012</creationdate><recordtype>article</recordtype><recordid>eNp9kUGPEyEUx4nRxLr6AbxNTEzWAwoMDDPemuquTRq9rF7JK_PYsplCBZq1317qNF5MPJHH-_1_h_cn5DVn7zlj-kPmbFAtZVzQoReaiidkwZUWtB-EfkoWrK7poHvxnLzI-YHVuR_kgjwunfPBl1MTXbMM1z_W7xoXU_NV0jssCUYMBQo2n2Kovxt_D2HMH5tV3B8m_AXFx3BOlh02S1t8OE1_FOsYcvPoy-4f0UXxkjxzMGV8dXmvyPebz3erL3Tz7Xa9Wm6oFaIVFBzjqEcYJW5F28PYSY5ccgAtt4NyQgvrGDrVbXvXqdGC6-TYAaAYlQXZXpE3szfm4k22vqDd2RgC2mI4k229W4WuZ-iQ4s8j5mL2PlucJggYj9nwTvNWaKnPPj6jNsWcEzpzSH4P6VRl5tyEmZswtQlzbsKImnl70UO2MLkEwfr8NyjU0HdK9ZUTM5frKtxjMg_xmEI9z3_kvwFuGpgG</recordid><startdate>20120501</startdate><enddate>20120501</enddate><creator>Ogden, Mark D.</creator><creator>Sinkov, Serguei I.</creator><creator>Lumetta, Gregg J.</creator><creator>Nash, Kenneth L.</creator><general>Springer US</general><general>Springer</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7U5</scope><scope>8FD</scope><scope>L7M</scope><scope>OTOTI</scope></search><sort><creationdate>20120501</creationdate><title>Affinity of An(VI) for N4-Tetradentate Donor Ligands: Complexation of the Actinyl(VI) Ions with N4-Tetradentate Ligands</title><author>Ogden, Mark D. ; Sinkov, Serguei I. ; Lumetta, Gregg J. ; Nash, Kenneth L.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c2232-af01e7dad4eb238ad641e141aa74b95f272cf0ef56b8f65dcaf64d6aae2d5ca43</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2012</creationdate><topic>ACTINIDES</topic><topic>AFFINITY</topic><topic>AMINES</topic><topic>Backbone</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Complexation</topic><topic>Condensed Matter Physics</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>Geochemistry</topic><topic>Industrial Chemistry/Chemical Engineering</topic><topic>Inorganic Chemistry</topic><topic>Ligands</topic><topic>METHANOL</topic><topic>Methyl alcohol</topic><topic>Nitrogen donor ligands</topic><topic>Non-aqueous media</topic><topic>Oceanography</topic><topic>Physical Chemistry</topic><topic>PIPERAZINES</topic><topic>Plutonium</topic><topic>RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY</topic><topic>Solutions</topic><topic>SPECTROPHOTOMETRY</topic><topic>STABILITY</topic><topic>Trends</topic><topic>Uranium</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ogden, Mark D.</creatorcontrib><creatorcontrib>Sinkov, Serguei I.</creatorcontrib><creatorcontrib>Lumetta, Gregg J.</creatorcontrib><creatorcontrib>Nash, Kenneth L.</creatorcontrib><creatorcontrib>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Technology Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>OSTI.GOV</collection><jtitle>Journal of solution chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ogden, Mark D.</au><au>Sinkov, Serguei I.</au><au>Lumetta, Gregg J.</au><au>Nash, Kenneth L.</au><aucorp>Pacific Northwest National Lab. (PNNL), Richland, WA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Affinity of An(VI) for N4-Tetradentate Donor Ligands: Complexation of the Actinyl(VI) Ions with N4-Tetradentate Ligands</atitle><jtitle>Journal of solution chemistry</jtitle><stitle>J Solution Chem</stitle><date>2012-05-01</date><risdate>2012</risdate><volume>41</volume><issue>4</issue><spage>616</spage><epage>629</epage><pages>616-629</pages><issn>0095-9782</issn><eissn>1572-8927</eissn><coden>JSLCAG</coden><abstract>In this report the affinity of four N
4
-tetradentate ligands that incorporate the 2-methylpyridyl functionality with hexavalent actinides
has been investigated in methanol solution. The ligands studied include N,N′-bis(2-methylpyridyl)diaminoethane (BPMDAE), N,N′-bis(2-methylpyridyl)-1,3-diaminopropane (BPMDAP), N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP), and trans-N,N-bis(2-pyridylmethyl)-1,2-diaminocyclohexane (BPMDAC). Conditional stability constants describing the strength of the interaction were determined by UV–visible spectrophotometry. The log
10
K
101
values for both U(VI) and Pu(VI) are comparable and show the same trend of stability with ligand structure. Dinuclear complexes are also indicated as being important. The log
10
K
201
values for Pu(VI) complexation with the N
4
-ligands are identical for the four ligands (within experimental error), indicating that the structure of the ligand backbone has little effect on the stability of the (PuO
2
)
2
L
2+
complex. The exception to this trend is the behavior of N,N′-bis(2-pyridylmethyl)piperazine (BPMPIP) with Pu(VI). This ligand displays a tendency to reduce Pu(VI) within the experimental time frame of 45 minutes. BPMPIP is the only ligand tested that contains tertiary amines in the ligand backbone. The decomposition of BPMPIP by Pu(VI) suggests a susceptibility of tertiary amines to oxidative degradation.</abstract><cop>Boston</cop><pub>Springer US</pub><doi>10.1007/s10953-012-9827-2</doi><tpages>14</tpages></addata></record> |
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| ispartof | Journal of solution chemistry, 2012-05, Vol.41 (4), p.616-629 |
| issn | 0095-9782 1572-8927 |
| language | eng |
| recordid | cdi_osti_scitechconnect_1043109 |
| source | SpringerLink Journals - AutoHoldings |
| subjects | ACTINIDES AFFINITY AMINES Backbone Chemistry Chemistry and Materials Science Complexation Condensed Matter Physics Exact sciences and technology General and physical chemistry Geochemistry Industrial Chemistry/Chemical Engineering Inorganic Chemistry Ligands METHANOL Methyl alcohol Nitrogen donor ligands Non-aqueous media Oceanography Physical Chemistry PIPERAZINES Plutonium RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY Solutions SPECTROPHOTOMETRY STABILITY Trends Uranium |
| title | Affinity of An(VI) for N4-Tetradentate Donor Ligands: Complexation of the Actinyl(VI) Ions with N4-Tetradentate Ligands |
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