PittsburghV1, Main, Exploration, bibRecord, 000008

Linking Solution Structures and Energetics: Thorium Nitrate Complexes

Identifieur interne : 000008 ( Main/Exploration ); précédent : 000007; suivant : 000009

Linking Solution Structures and Energetics: Thorium Nitrate Complexes

Auteurs : Suntharalingam Skanthakumar [États-Unis] ; Geng Bang Jin [États-Unis] ; Jian Lin [États-Unis] ; Valérie Vallet [France] ; Lynne Soderholm [États-Unis]

Source :

Journal of Physical Chemistry B [ 1520-6106 ] ; 2017-08-17.

RBID : Hal:hal-01591662

Abstract

Seeking predictive insights into how metal-ion speciation impacts solution chemistry as well as the composition and structure of solid-precipitates, thorium correlations, with both solvent and other solute ions, were quantitatively probed in a series of acidic, nitrate/perchlorate solutions held at constant ionic strength. Difference pair-distribution functions (dPDF), obtained from high-energy X-ray scattering (HEXS) data, provide unprecedented structural information on the number of Th ligating ions in solution and how they change with increasing nitrate concentration. A fit of the end member solution, Th (4 m perchloric acid and no nitrate), reveals a homoleptic Th aqua ion with 10 waters in its first coordination shell. Analyses of the acidic solutions containing nitrate reveal exclusively bidentate NO₃^- complexation with Th, consistent with published solid-state M^IV nitrate structures, where M^IV = Ce, Th, U, Np, Pu. Metrical fits of Th coordination as a function of nitrate concentration are used to calculate Th–NO₃ stability constants, information important to a molecular-scale description of reaction energetics. The coordination environments of Th in solution were compared with single-crystal structures obtained from their precipitates, Th(NO₃)₄(H₂O)₄ and Th(NO₃)₄(H₂O)₃·(H₂O)₂. Relative stabilities of the solid-state compounds, assessed based on the results of molecular quantum chemical calculations, reveal the importance of including an accurate description of complexed waters when predicting relative energetics of dissolved ions in aqueous solution.

Url:

https://hal.archives-ouvertes.fr/hal-01591662

DOI: 10.1021/acs.jpcb.7b06567

Affiliations:

France, États-Unis

Links toward previous steps (curation, corpus...)

to stream Hal, to step Corpus: 000363
to stream Hal, to step Curation: 000363
to stream Hal, to step Checkpoint: 000008
to stream Main, to step Merge: 000008
to stream Main, to step Curation: 000008

Le document en format XML

<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en">Linking Solution Structures and Energetics: Thorium Nitrate Complexes</title>
<author><name sortKey="Skanthakumar, Suntharalingam" sort="Skanthakumar, Suntharalingam" uniqKey="Skanthakumar S" first="Suntharalingam" last="Skanthakumar">Suntharalingam Skanthakumar</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-406836" status="INCOMING">          <orgName>Chemical Sciences and Engineering Division</orgName>
          <desc>            <address>              <addrLine>Argonne, Illinois 60439</addrLine>
              <country key="US"></country>
            </address>
          </desc>
          <listRelation>            <relation active="#struct-49346" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-49346" type="direct"><org type="institution" xml:id="struct-49346" status="VALID">          <orgName>Argonne National Laboratory [Lemont]</orgName>
          <orgName type="acronym">ANL</orgName>
          <desc>            <address>              <addrLine>9700 S Cass Ave B109, Lemont, IL, 60439</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.anl.gov</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Jin, Geng Bang" sort="Jin, Geng Bang" uniqKey="Jin G" first="Geng Bang" last="Jin">Geng Bang Jin</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-406836" status="INCOMING">          <orgName>Chemical Sciences and Engineering Division</orgName>
          <desc>            <address>              <addrLine>Argonne, Illinois 60439</addrLine>
              <country key="US"></country>
            </address>
          </desc>
          <listRelation>            <relation active="#struct-49346" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-49346" type="direct"><org type="institution" xml:id="struct-49346" status="VALID">          <orgName>Argonne National Laboratory [Lemont]</orgName>
          <orgName type="acronym">ANL</orgName>
          <desc>            <address>              <addrLine>9700 S Cass Ave B109, Lemont, IL, 60439</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.anl.gov</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Lin, Jian" sort="Lin, Jian" uniqKey="Lin J" first="Jian" last="Lin">Jian Lin</name>
<affiliation wicri:level="1"><hal:affiliation type="institution" xml:id="struct-67135" status="VALID">          <orgName>Carnegie Mellon University [Pittsburgh]</orgName>
          <orgName type="acronym">CMU</orgName>
          <desc>            <address>              <addrLine>5000 Forbes Ave,  Pittsburgh, PA 15213</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.cmu.edu/</ref>
          </desc>
        </hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Vallet, Valerie" sort="Vallet, Valerie" uniqKey="Vallet V" first="Valérie" last="Vallet">Valérie Vallet</name>
<affiliation wicri:level="1"><hal:affiliation type="researchteam" xml:id="struct-404926" status="VALID">          <orgName>Physico-Chimie Moléculaire Théorique</orgName>
          <orgName type="acronym">PCMT</orgName>
          <desc>            <address>              <country key="FR"></country>
            </address>
            <ref type="url">http://www.phlam.univ-lille1.fr/spip.php?article120</ref>
          </desc>
          <listRelation>            <relation active="#struct-43887" type="direct"></relation>
            <relation active="#struct-92973" type="indirect"></relation>
            <relation name="UMR8523" active="#struct-441569" type="indirect"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-43887" type="direct"><org type="laboratory" xml:id="struct-43887" status="VALID">          <idno type="RNSR">199812851G</idno>
          <idno type="ISNI">0000 0004 0368 4014</idno>
          <idno type="IdRef">161618847</idno>
          <orgName>Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523</orgName>
          <orgName type="acronym">PhLAM</orgName>
          <desc>            <address>              <addrLine>Bât. P5 − USTLF−59655 Villeneuve d’Ascq cedex </addrLine>
              <country key="FR"></country>
            </address>
            <ref type="url">http://www.phlam.univ-lille1.fr/</ref>
          </desc>
          <listRelation>            <relation active="#struct-92973" type="direct"></relation>
            <relation name="UMR8523" active="#struct-441569" type="direct"></relation>
          </listRelation>
        </org>
</tutelle>
<tutelle active="#struct-92973" type="indirect"><org type="institution" xml:id="struct-92973" status="VALID">          <idno type="IdRef">026404184</idno>
          <orgName>Université de Lille, Sciences et Technologies</orgName>
          <desc>            <address>              <addrLine>Cité Scientifique - 59655 Villeneuve d'Ascq Cedex</addrLine>
              <country key="FR"></country>
            </address>
            <ref type="url">http://www.univ-lille1.fr/</ref>
          </desc>
        </org>
</tutelle>
<tutelle name="UMR8523" active="#struct-441569" type="indirect"><org type="institution" xml:id="struct-441569" status="VALID">          <idno type="IdRef">02636817X</idno>
          <idno type="ISNI">0000000122597504</idno>
          <orgName>Centre National de la Recherche Scientifique</orgName>
          <orgName type="acronym">CNRS</orgName>
          <date type="start">1939-10-19</date>
          <desc>            <address>              <country key="FR"></country>
            </address>
            <ref type="url">http://www.cnrs.fr/</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>France</country>
</affiliation>
</author>
<author><name sortKey="Soderholm, Lynne" sort="Soderholm, Lynne" uniqKey="Soderholm L" first="Lynne" last="Soderholm">Lynne Soderholm</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-406836" status="INCOMING">          <orgName>Chemical Sciences and Engineering Division</orgName>
          <desc>            <address>              <addrLine>Argonne, Illinois 60439</addrLine>
              <country key="US"></country>
            </address>
          </desc>
          <listRelation>            <relation active="#struct-49346" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-49346" type="direct"><org type="institution" xml:id="struct-49346" status="VALID">          <orgName>Argonne National Laboratory [Lemont]</orgName>
          <orgName type="acronym">ANL</orgName>
          <desc>            <address>              <addrLine>9700 S Cass Ave B109, Lemont, IL, 60439</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.anl.gov</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
</titleStmt>
<publicationStmt><idno type="wicri:source">HAL</idno>
<idno type="RBID">Hal:hal-01591662</idno>
<idno type="halId">hal-01591662</idno>
<idno type="halUri">https://hal.archives-ouvertes.fr/hal-01591662</idno>
<idno type="url">https://hal.archives-ouvertes.fr/hal-01591662</idno>
<idno type="doi">10.1021/acs.jpcb.7b06567</idno>
<date when="2017-08-17">2017-08-17</date>
<idno type="wicri:Area/Hal/Corpus">000363</idno>
<idno type="wicri:Area/Hal/Curation">000363</idno>
<idno type="wicri:Area/Hal/Checkpoint">000008</idno>
<idno type="wicri:explorRef" wicri:stream="Hal" wicri:step="Checkpoint">000008</idno>
<idno type="wicri:doubleKey">1520-6106:2017:Skanthakumar S:linking:solution:structures</idno>
<idno type="wicri:Area/Main/Merge">000008</idno>
<idno type="wicri:Area/Main/Curation">000008</idno>
<idno type="wicri:Area/Main/Exploration">000008</idno>
</publicationStmt>
<sourceDesc><biblStruct><analytic><title xml:lang="en">Linking Solution Structures and Energetics: Thorium Nitrate Complexes</title>
<author><name sortKey="Skanthakumar, Suntharalingam" sort="Skanthakumar, Suntharalingam" uniqKey="Skanthakumar S" first="Suntharalingam" last="Skanthakumar">Suntharalingam Skanthakumar</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-406836" status="INCOMING">          <orgName>Chemical Sciences and Engineering Division</orgName>
          <desc>            <address>              <addrLine>Argonne, Illinois 60439</addrLine>
              <country key="US"></country>
            </address>
          </desc>
          <listRelation>            <relation active="#struct-49346" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-49346" type="direct"><org type="institution" xml:id="struct-49346" status="VALID">          <orgName>Argonne National Laboratory [Lemont]</orgName>
          <orgName type="acronym">ANL</orgName>
          <desc>            <address>              <addrLine>9700 S Cass Ave B109, Lemont, IL, 60439</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.anl.gov</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Jin, Geng Bang" sort="Jin, Geng Bang" uniqKey="Jin G" first="Geng Bang" last="Jin">Geng Bang Jin</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-406836" status="INCOMING">          <orgName>Chemical Sciences and Engineering Division</orgName>
          <desc>            <address>              <addrLine>Argonne, Illinois 60439</addrLine>
              <country key="US"></country>
            </address>
          </desc>
          <listRelation>            <relation active="#struct-49346" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-49346" type="direct"><org type="institution" xml:id="struct-49346" status="VALID">          <orgName>Argonne National Laboratory [Lemont]</orgName>
          <orgName type="acronym">ANL</orgName>
          <desc>            <address>              <addrLine>9700 S Cass Ave B109, Lemont, IL, 60439</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.anl.gov</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Lin, Jian" sort="Lin, Jian" uniqKey="Lin J" first="Jian" last="Lin">Jian Lin</name>
<affiliation wicri:level="1"><hal:affiliation type="institution" xml:id="struct-67135" status="VALID">          <orgName>Carnegie Mellon University [Pittsburgh]</orgName>
          <orgName type="acronym">CMU</orgName>
          <desc>            <address>              <addrLine>5000 Forbes Ave,  Pittsburgh, PA 15213</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.cmu.edu/</ref>
          </desc>
        </hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
<author><name sortKey="Vallet, Valerie" sort="Vallet, Valerie" uniqKey="Vallet V" first="Valérie" last="Vallet">Valérie Vallet</name>
<affiliation wicri:level="1"><hal:affiliation type="researchteam" xml:id="struct-404926" status="VALID">          <orgName>Physico-Chimie Moléculaire Théorique</orgName>
          <orgName type="acronym">PCMT</orgName>
          <desc>            <address>              <country key="FR"></country>
            </address>
            <ref type="url">http://www.phlam.univ-lille1.fr/spip.php?article120</ref>
          </desc>
          <listRelation>            <relation active="#struct-43887" type="direct"></relation>
            <relation active="#struct-92973" type="indirect"></relation>
            <relation name="UMR8523" active="#struct-441569" type="indirect"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-43887" type="direct"><org type="laboratory" xml:id="struct-43887" status="VALID">          <idno type="RNSR">199812851G</idno>
          <idno type="ISNI">0000 0004 0368 4014</idno>
          <idno type="IdRef">161618847</idno>
          <orgName>Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523</orgName>
          <orgName type="acronym">PhLAM</orgName>
          <desc>            <address>              <addrLine>Bât. P5 − USTLF−59655 Villeneuve d’Ascq cedex </addrLine>
              <country key="FR"></country>
            </address>
            <ref type="url">http://www.phlam.univ-lille1.fr/</ref>
          </desc>
          <listRelation>            <relation active="#struct-92973" type="direct"></relation>
            <relation name="UMR8523" active="#struct-441569" type="direct"></relation>
          </listRelation>
        </org>
</tutelle>
<tutelle active="#struct-92973" type="indirect"><org type="institution" xml:id="struct-92973" status="VALID">          <idno type="IdRef">026404184</idno>
          <orgName>Université de Lille, Sciences et Technologies</orgName>
          <desc>            <address>              <addrLine>Cité Scientifique - 59655 Villeneuve d'Ascq Cedex</addrLine>
              <country key="FR"></country>
            </address>
            <ref type="url">http://www.univ-lille1.fr/</ref>
          </desc>
        </org>
</tutelle>
<tutelle name="UMR8523" active="#struct-441569" type="indirect"><org type="institution" xml:id="struct-441569" status="VALID">          <idno type="IdRef">02636817X</idno>
          <idno type="ISNI">0000000122597504</idno>
          <orgName>Centre National de la Recherche Scientifique</orgName>
          <orgName type="acronym">CNRS</orgName>
          <date type="start">1939-10-19</date>
          <desc>            <address>              <country key="FR"></country>
            </address>
            <ref type="url">http://www.cnrs.fr/</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>France</country>
</affiliation>
</author>
<author><name sortKey="Soderholm, Lynne" sort="Soderholm, Lynne" uniqKey="Soderholm L" first="Lynne" last="Soderholm">Lynne Soderholm</name>
<affiliation wicri:level="1"><hal:affiliation type="department" xml:id="struct-406836" status="INCOMING">          <orgName>Chemical Sciences and Engineering Division</orgName>
          <desc>            <address>              <addrLine>Argonne, Illinois 60439</addrLine>
              <country key="US"></country>
            </address>
          </desc>
          <listRelation>            <relation active="#struct-49346" type="direct"></relation>
          </listRelation>
        <tutelles><tutelle active="#struct-49346" type="direct"><org type="institution" xml:id="struct-49346" status="VALID">          <orgName>Argonne National Laboratory [Lemont]</orgName>
          <orgName type="acronym">ANL</orgName>
          <desc>            <address>              <addrLine>9700 S Cass Ave B109, Lemont, IL, 60439</addrLine>
              <country key="US"></country>
            </address>
            <ref type="url">http://www.anl.gov</ref>
          </desc>
        </org>
</tutelle>
</tutelles>
</hal:affiliation>
<country>États-Unis</country>
</affiliation>
</author>
</analytic>
<idno type="DOI">10.1021/acs.jpcb.7b06567</idno>
<series><title level="j">Journal of Physical Chemistry B</title>
<idno type="ISSN">1520-6106</idno>
<imprint><date type="datePub">2017-08-17</date>
</imprint>
</series>
</biblStruct>
</sourceDesc>
</fileDesc>
<profileDesc><textClass></textClass>
</profileDesc>
</teiHeader>
<front><div type="abstract" xml:lang="en">Seeking predictive insights into how metal-ion speciation impacts solution chemistry as well as the composition and structure of solid-precipitates, thorium correlations, with both solvent and other solute ions, were quantitatively probed in a series of acidic, nitrate/perchlorate solutions held at constant ionic strength. Difference pair-distribution functions (dPDF), obtained from high-energy X-ray scattering (HEXS) data, provide unprecedented structural information on the number of Th ligating ions in solution and how they change with increasing nitrate concentration. A fit of the end member solution, Th (4 m perchloric acid and no nitrate), reveals a homoleptic Th aqua ion with 10 waters in its first coordination shell. Analyses of the acidic solutions containing nitrate reveal exclusively bidentate NO₃^- complexation with Th, consistent with published solid-state M^IV nitrate structures, where M^IV = Ce, Th, U, Np, Pu. Metrical fits of Th coordination as a function of nitrate concentration are used to calculate Th–NO₃ stability constants, information important to a molecular-scale description of reaction energetics. The coordination environments of Th in solution were compared with single-crystal structures obtained from their precipitates, Th(NO₃)₄(H₂O)₄ and Th(NO₃)₄(H₂O)₃·(H₂O)₂. Relative stabilities of the solid-state compounds, assessed based on the results of molecular quantum chemical calculations, reveal the importance of including an accurate description of complexed waters when predicting relative energetics of dissolved ions in aqueous solution.</div>
</front>
</TEI>
<affiliations><list><country><li>France</li>
<li>États-Unis</li>
</country>
</list>
<tree><country name="États-Unis"><noRegion><name sortKey="Skanthakumar, Suntharalingam" sort="Skanthakumar, Suntharalingam" uniqKey="Skanthakumar S" first="Suntharalingam" last="Skanthakumar">Suntharalingam Skanthakumar</name>
</noRegion>
<name sortKey="Jin, Geng Bang" sort="Jin, Geng Bang" uniqKey="Jin G" first="Geng Bang" last="Jin">Geng Bang Jin</name>
<name sortKey="Lin, Jian" sort="Lin, Jian" uniqKey="Lin J" first="Jian" last="Lin">Jian Lin</name>
<name sortKey="Soderholm, Lynne" sort="Soderholm, Lynne" uniqKey="Soderholm L" first="Lynne" last="Soderholm">Lynne Soderholm</name>
</country>
<country name="France"><noRegion><name sortKey="Vallet, Valerie" sort="Vallet, Valerie" uniqKey="Vallet V" first="Valérie" last="Vallet">Valérie Vallet</name>
</noRegion>
</country>
</tree>
</affiliations>
</record>

Pour manipuler ce document sous Unix (Dilib)

EXPLOR_STEP=$WICRI_ROOT/Wicri/Amérique/explor/PittsburghV1/Data/Main/Exploration

HfdSelect -h $EXPLOR_STEP/biblio.hfd -nk 000008 | SxmlIndent | more

HfdSelect -h $EXPLOR_AREA/Data/Main/Exploration/biblio.hfd -nk 000008 | SxmlIndent | more

Pour mettre un lien sur cette page dans le réseau Wicri

{{Explor lien
   |wiki=    Wicri/Amérique
   |area=    PittsburghV1
   |flux=    Main
   |étape=   Exploration
   |type=    RBID
   |clé=     Hal:hal-01591662
   |texte=   Linking Solution Structures and Energetics: Thorium Nitrate Complexes
}}

This area was generated with Dilib version V0.6.38.
Data generation: Fri Jun 18 17:37:45 2021. Site generation: Fri Jun 18 18:15:47 2021

	Serveur d'exploration sur Pittsburgh
	Attention, ce site est en cours de développement ! Attention, site généré par des moyens informatiques à partir de corpus bruts. Les informations ne sont donc pas validées.

Serveur d'exploration sur Pittsburgh

Linking Solution Structures and Energetics: Thorium Nitrate Complexes

Linking Solution Structures and Energetics: Thorium Nitrate Complexes

Source :

Abstract

Links toward previous steps (curation, corpus...)

Le document en format XML

Pour manipuler ce document sous Unix (Dilib)

Pour mettre un lien sur cette page dans le réseau Wicri