27 Al Pulsed Field Gradient, Diffusion-NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions
Pulsed field gradient nuclear magnetic resonance (PFG-NMR) measurements were successfully applied to the Al ( I = 5/2) nucleus in concentrated electrolytes to investigate the diffusion of aluminate ions [Al(OH) ] in simulant high-level nuclear waste (3 M NaOH) between 25 and 85 °C. The temperature-d...
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| Veröffentlicht in: | The journal of physical chemistry. B 2018-12, Vol.122 (48), p.10907-10912 |
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| creator | Graham, Trent R Han, Kee Sung Dembowski, Mateusz Krzysko, Anthony J Zhang, Xin Hu, Jianzhi Clark, Sue B Clark, Aurora E Schenter, Gregory K Pearce, Carolyn I Rosso, Kevin M |
| description | Pulsed field gradient nuclear magnetic resonance (PFG-NMR) measurements were successfully applied to the
Al ( I = 5/2) nucleus in concentrated electrolytes to investigate the diffusion of aluminate ions [Al(OH)
] in simulant high-level nuclear waste (3 M NaOH) between 25 and 85 °C. The temperature-dependent diffusion coefficients obtained from
H,
Na, and
Al PFG-NMR were well fit by a Vogel-Fulcher-Tammann model and a power law equation. Comparison of
Al diffusion coefficients of 0.1 M Al(OH)
in ∼3 M MOH (where M = Na
, K
, (CH
)
N
) at room temperature varied in agreement with the expected changes in solution viscosity via Stokes-Einstein relationship, confirming that the dominant Al species at these conditions are Al(OH)
monomers. This
Al PFG-NMR study extends an established methodology to a previously unexplored nucleus enabling this experimental technique to be leverage for exploring ion transport, speciation, and solution structure in concentrated electrolytes. |
| doi_str_mv | 10.1021/acs.jpcb.8b10145 |
| format | Article |
| fullrecord | <record><control><sourceid>pubmed_osti_</sourceid><recordid>TN_cdi_osti_scitechconnect_1596368</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>30354130</sourcerecordid><originalsourceid>FETCH-LOGICAL-c1380-68d4ee026f7548739b517b99d17375ead78f509de9d901586db26af14998b9883</originalsourceid><addsrcrecordid>eNo9kM9PwyAUx4nRuDm9ezLEs51QSgvHZXNzydTF6bmh_FBmR5vSmuzg_y7NpgfCC7zPe_l-ALjGaIxRjO-F9ONtLYsxKzDCCT0BQ0xjFIWTnR7rFKN0AC683yIU05il52BAEKEJJmgIfuIMTkq47kqvFZxbXSq4aISy2rV3cGaN6bytXPT89Ao3tZZtU3lZ1XtYGbipym_Rhl842zuxs9JD4RRchoe1sI11H9C6MP1LlNbpUHQ760Sre7DrOX8JzowIm6-O9wi8zx_epo_R6mWxnE5WkcSEhQhMJVqjODUZTVhGeEFxVnCucEYyqoXKmKGIK80VR5iyVBVxKgxOOGcFZ4yMwO1hbuVbm3tpWy0_ZeVcCJRjylOS9k3o0CRDRt9ok9eN3Ylmn2OU97rzoDvvdedH3QG5OSB1V-y0-gf-_JJfK5N8Sg</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype></control><display><type>article</type><title>27 Al Pulsed Field Gradient, Diffusion-NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions</title><source>ACS Publications</source><creator>Graham, Trent R ; Han, Kee Sung ; Dembowski, Mateusz ; Krzysko, Anthony J ; Zhang, Xin ; Hu, Jianzhi ; Clark, Sue B ; Clark, Aurora E ; Schenter, Gregory K ; Pearce, Carolyn I ; Rosso, Kevin M</creator><creatorcontrib>Graham, Trent R ; Han, Kee Sung ; Dembowski, Mateusz ; Krzysko, Anthony J ; Zhang, Xin ; Hu, Jianzhi ; Clark, Sue B ; Clark, Aurora E ; Schenter, Gregory K ; Pearce, Carolyn I ; Rosso, Kevin M ; Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL) ; Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM)</creatorcontrib><description>Pulsed field gradient nuclear magnetic resonance (PFG-NMR) measurements were successfully applied to the
Al ( I = 5/2) nucleus in concentrated electrolytes to investigate the diffusion of aluminate ions [Al(OH)
] in simulant high-level nuclear waste (3 M NaOH) between 25 and 85 °C. The temperature-dependent diffusion coefficients obtained from
H,
Na, and
Al PFG-NMR were well fit by a Vogel-Fulcher-Tammann model and a power law equation. Comparison of
Al diffusion coefficients of 0.1 M Al(OH)
in ∼3 M MOH (where M = Na
, K
, (CH
)
N
) at room temperature varied in agreement with the expected changes in solution viscosity via Stokes-Einstein relationship, confirming that the dominant Al species at these conditions are Al(OH)
monomers. This
Al PFG-NMR study extends an established methodology to a previously unexplored nucleus enabling this experimental technique to be leverage for exploring ion transport, speciation, and solution structure in concentrated electrolytes.</description><identifier>ISSN: 1520-6106</identifier><identifier>EISSN: 1520-5207</identifier><identifier>DOI: 10.1021/acs.jpcb.8b10145</identifier><identifier>PMID: 30354130</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>Diffusion ; Electrolytes ; Ions ; Mixtures ; Transport properties</subject><ispartof>The journal of physical chemistry. B, 2018-12, Vol.122 (48), p.10907-10912</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c1380-68d4ee026f7548739b517b99d17375ead78f509de9d901586db26af14998b9883</citedby><cites>FETCH-LOGICAL-c1380-68d4ee026f7548739b517b99d17375ead78f509de9d901586db26af14998b9883</cites><orcidid>0000-0001-9381-721X ; 0000-0002-3535-1818 ; 0000-0001-8879-747X ; 0000-0002-8474-7720 ; 0000-0001-8907-8004 ; 0000-0002-6665-8417 ; 0000-0003-2000-858X ; 0000-0002-2438-9730 ; 0000-0003-3098-1615 ; 000000032000858X ; 0000000284747720 ; 0000000235351818 ; 0000000189078004 ; 0000000224389730 ; 000000018879747X ; 0000000266658417 ; 000000019381721X ; 0000000330981615</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,776,780,881,2751,27903,27904</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/30354130$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/1596368$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Graham, Trent R</creatorcontrib><creatorcontrib>Han, Kee Sung</creatorcontrib><creatorcontrib>Dembowski, Mateusz</creatorcontrib><creatorcontrib>Krzysko, Anthony J</creatorcontrib><creatorcontrib>Zhang, Xin</creatorcontrib><creatorcontrib>Hu, Jianzhi</creatorcontrib><creatorcontrib>Clark, Sue B</creatorcontrib><creatorcontrib>Clark, Aurora E</creatorcontrib><creatorcontrib>Schenter, Gregory K</creatorcontrib><creatorcontrib>Pearce, Carolyn I</creatorcontrib><creatorcontrib>Rosso, Kevin M</creatorcontrib><creatorcontrib>Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM)</creatorcontrib><title>27 Al Pulsed Field Gradient, Diffusion-NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions</title><title>The journal of physical chemistry. B</title><addtitle>J Phys Chem B</addtitle><description>Pulsed field gradient nuclear magnetic resonance (PFG-NMR) measurements were successfully applied to the
Al ( I = 5/2) nucleus in concentrated electrolytes to investigate the diffusion of aluminate ions [Al(OH)
] in simulant high-level nuclear waste (3 M NaOH) between 25 and 85 °C. The temperature-dependent diffusion coefficients obtained from
H,
Na, and
Al PFG-NMR were well fit by a Vogel-Fulcher-Tammann model and a power law equation. Comparison of
Al diffusion coefficients of 0.1 M Al(OH)
in ∼3 M MOH (where M = Na
, K
, (CH
)
N
) at room temperature varied in agreement with the expected changes in solution viscosity via Stokes-Einstein relationship, confirming that the dominant Al species at these conditions are Al(OH)
monomers. This
Al PFG-NMR study extends an established methodology to a previously unexplored nucleus enabling this experimental technique to be leverage for exploring ion transport, speciation, and solution structure in concentrated electrolytes.</description><subject>Diffusion</subject><subject>Electrolytes</subject><subject>Ions</subject><subject>Mixtures</subject><subject>Transport properties</subject><issn>1520-6106</issn><issn>1520-5207</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNo9kM9PwyAUx4nRuDm9ezLEs51QSgvHZXNzydTF6bmh_FBmR5vSmuzg_y7NpgfCC7zPe_l-ALjGaIxRjO-F9ONtLYsxKzDCCT0BQ0xjFIWTnR7rFKN0AC683yIU05il52BAEKEJJmgIfuIMTkq47kqvFZxbXSq4aISy2rV3cGaN6bytXPT89Ao3tZZtU3lZ1XtYGbipym_Rhl842zuxs9JD4RRchoe1sI11H9C6MP1LlNbpUHQ760Sre7DrOX8JzowIm6-O9wi8zx_epo_R6mWxnE5WkcSEhQhMJVqjODUZTVhGeEFxVnCucEYyqoXKmKGIK80VR5iyVBVxKgxOOGcFZ4yMwO1hbuVbm3tpWy0_ZeVcCJRjylOS9k3o0CRDRt9ok9eN3Ylmn2OU97rzoDvvdedH3QG5OSB1V-y0-gf-_JJfK5N8Sg</recordid><startdate>20181206</startdate><enddate>20181206</enddate><creator>Graham, Trent R</creator><creator>Han, Kee Sung</creator><creator>Dembowski, Mateusz</creator><creator>Krzysko, Anthony J</creator><creator>Zhang, Xin</creator><creator>Hu, Jianzhi</creator><creator>Clark, Sue B</creator><creator>Clark, Aurora E</creator><creator>Schenter, Gregory K</creator><creator>Pearce, Carolyn I</creator><creator>Rosso, Kevin M</creator><general>American Chemical Society</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-9381-721X</orcidid><orcidid>https://orcid.org/0000-0002-3535-1818</orcidid><orcidid>https://orcid.org/0000-0001-8879-747X</orcidid><orcidid>https://orcid.org/0000-0002-8474-7720</orcidid><orcidid>https://orcid.org/0000-0001-8907-8004</orcidid><orcidid>https://orcid.org/0000-0002-6665-8417</orcidid><orcidid>https://orcid.org/0000-0003-2000-858X</orcidid><orcidid>https://orcid.org/0000-0002-2438-9730</orcidid><orcidid>https://orcid.org/0000-0003-3098-1615</orcidid><orcidid>https://orcid.org/000000032000858X</orcidid><orcidid>https://orcid.org/0000000284747720</orcidid><orcidid>https://orcid.org/0000000235351818</orcidid><orcidid>https://orcid.org/0000000189078004</orcidid><orcidid>https://orcid.org/0000000224389730</orcidid><orcidid>https://orcid.org/000000018879747X</orcidid><orcidid>https://orcid.org/0000000266658417</orcidid><orcidid>https://orcid.org/000000019381721X</orcidid><orcidid>https://orcid.org/0000000330981615</orcidid></search><sort><creationdate>20181206</creationdate><title>27 Al Pulsed Field Gradient, Diffusion-NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions</title><author>Graham, Trent R ; Han, Kee Sung ; Dembowski, Mateusz ; Krzysko, Anthony J ; Zhang, Xin ; Hu, Jianzhi ; Clark, Sue B ; Clark, Aurora E ; Schenter, Gregory K ; Pearce, Carolyn I ; Rosso, Kevin M</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c1380-68d4ee026f7548739b517b99d17375ead78f509de9d901586db26af14998b9883</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Diffusion</topic><topic>Electrolytes</topic><topic>Ions</topic><topic>Mixtures</topic><topic>Transport properties</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Graham, Trent R</creatorcontrib><creatorcontrib>Han, Kee Sung</creatorcontrib><creatorcontrib>Dembowski, Mateusz</creatorcontrib><creatorcontrib>Krzysko, Anthony J</creatorcontrib><creatorcontrib>Zhang, Xin</creatorcontrib><creatorcontrib>Hu, Jianzhi</creatorcontrib><creatorcontrib>Clark, Sue B</creatorcontrib><creatorcontrib>Clark, Aurora E</creatorcontrib><creatorcontrib>Schenter, Gregory K</creatorcontrib><creatorcontrib>Pearce, Carolyn I</creatorcontrib><creatorcontrib>Rosso, Kevin M</creatorcontrib><creatorcontrib>Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM)</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>The journal of physical chemistry. B</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Graham, Trent R</au><au>Han, Kee Sung</au><au>Dembowski, Mateusz</au><au>Krzysko, Anthony J</au><au>Zhang, Xin</au><au>Hu, Jianzhi</au><au>Clark, Sue B</au><au>Clark, Aurora E</au><au>Schenter, Gregory K</au><au>Pearce, Carolyn I</au><au>Rosso, Kevin M</au><aucorp>Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)</aucorp><aucorp>Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>27 Al Pulsed Field Gradient, Diffusion-NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions</atitle><jtitle>The journal of physical chemistry. B</jtitle><addtitle>J Phys Chem B</addtitle><date>2018-12-06</date><risdate>2018</risdate><volume>122</volume><issue>48</issue><spage>10907</spage><epage>10912</epage><pages>10907-10912</pages><issn>1520-6106</issn><eissn>1520-5207</eissn><abstract>Pulsed field gradient nuclear magnetic resonance (PFG-NMR) measurements were successfully applied to the
Al ( I = 5/2) nucleus in concentrated electrolytes to investigate the diffusion of aluminate ions [Al(OH)
] in simulant high-level nuclear waste (3 M NaOH) between 25 and 85 °C. The temperature-dependent diffusion coefficients obtained from
H,
Na, and
Al PFG-NMR were well fit by a Vogel-Fulcher-Tammann model and a power law equation. Comparison of
Al diffusion coefficients of 0.1 M Al(OH)
in ∼3 M MOH (where M = Na
, K
, (CH
)
N
) at room temperature varied in agreement with the expected changes in solution viscosity via Stokes-Einstein relationship, confirming that the dominant Al species at these conditions are Al(OH)
monomers. This
Al PFG-NMR study extends an established methodology to a previously unexplored nucleus enabling this experimental technique to be leverage for exploring ion transport, speciation, and solution structure in concentrated electrolytes.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>30354130</pmid><doi>10.1021/acs.jpcb.8b10145</doi><tpages>6</tpages><orcidid>https://orcid.org/0000-0001-9381-721X</orcidid><orcidid>https://orcid.org/0000-0002-3535-1818</orcidid><orcidid>https://orcid.org/0000-0001-8879-747X</orcidid><orcidid>https://orcid.org/0000-0002-8474-7720</orcidid><orcidid>https://orcid.org/0000-0001-8907-8004</orcidid><orcidid>https://orcid.org/0000-0002-6665-8417</orcidid><orcidid>https://orcid.org/0000-0003-2000-858X</orcidid><orcidid>https://orcid.org/0000-0002-2438-9730</orcidid><orcidid>https://orcid.org/0000-0003-3098-1615</orcidid><orcidid>https://orcid.org/000000032000858X</orcidid><orcidid>https://orcid.org/0000000284747720</orcidid><orcidid>https://orcid.org/0000000235351818</orcidid><orcidid>https://orcid.org/0000000189078004</orcidid><orcidid>https://orcid.org/0000000224389730</orcidid><orcidid>https://orcid.org/000000018879747X</orcidid><orcidid>https://orcid.org/0000000266658417</orcidid><orcidid>https://orcid.org/000000019381721X</orcidid><orcidid>https://orcid.org/0000000330981615</orcidid></addata></record> |
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| language | eng |
| recordid | cdi_osti_scitechconnect_1596368 |
| source | ACS Publications |
| subjects | Diffusion Electrolytes Ions Mixtures Transport properties |
| title | 27 Al Pulsed Field Gradient, Diffusion-NMR Spectroscopy of Solvation Dynamics and Ion Pairing in Alkaline Aluminate Solutions |
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