Formation and Characterisation of the Silver Hydride Nanocluster Cation [Ag3H2((Ph2P)2CH2)]+ and Its Release of Hydrogen
Identifieur interne : 003E06 ( Main/Exploration ); précédent : 003E05; suivant : 003E07Formation and Characterisation of the Silver Hydride Nanocluster Cation [Ag3H2((Ph2P)2CH2)]+ and Its Release of Hydrogen
Auteurs : Marion Girod [France] ; Marjan Krsti [Croatie] ; Rodolphe Antoine [France] ; Luke Macaleese [France] ; Jérome Lemoine [France] ; Athanasios Zavras [Australie] ; George N. Khairallah [Australie] ; Vlasta Bona I Outeck [Croatie, Allemagne, Australie] ; Philippe Dugourd [France, Australie] ; Richard A. J. O'Hair [Australie]Source :
- Chemistry – A European Journal [ 0947-6539 ] ; 2014-12-08.
Abstract
Multistage mass spectrometry and density functional theory (DFT) were used to characterise the small silver hydride nanocluster, [Ag3H2L]+ (where L=(Ph2P)2CH2) and its gas‐phase unimolecular chemistry. Collision‐induced dissociation (CID) yields [Ag2HL]+ as the major product while laser‐induced dissociation (LID) proceeds via H2 formation and subsequent release from [Ag3H2L]+, giving rise to [Ag3L]+ as the major product. Deuterium labelling studies on [Ag3D2L]+ prove that the source of H2 is from the hydrides and not from the ligand. Comparison of TD‐DFT absorption patterns obtained for the optimised structures with action spectroscopy results, allows assignment of the measured features to structures of precursors and products. Molecular dynamics “on the fly” reveal that AgH loss is favoured in the ground state, but H2 formation and loss is preferred in the first excited state S1, in agreement with CID and LID experimental findings. This indicates favourable photo‐induced formation of H2 and subsequent release from [Ag3H2L]+, an important finding in context of metal hydrides as a hydrogen storage medium, which can subsequently be released by heating or irradiation with light.
Url:
DOI: 10.1002/chem.201404110
Affiliations:
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Khairallah</name><affiliation wicri:level="4"><country xml:lang="fr">Australie</country><wicri:regionArea>School of Chemistry, University of Melbourne</wicri:regionArea><placeName><settlement type="city">Melbourne</settlement><region type="état">Victoria (État)</region></placeName><orgName type="university">Université de Melbourne</orgName></affiliation></author><author><name sortKey="Bona I Outeck, Vlasta" sort="Bona I Outeck, Vlasta" uniqKey="Bona I Outeck V" first="Vlasta" last="Bona I Outeck">Vlasta Bona I Outeck</name><affiliation wicri:level="1"><country xml:lang="fr">Croatie</country><wicri:regionArea>Interdisciplinary Center for Advanced Science and Technology (ICAST), University of Split</wicri:regionArea><wicri:noRegion>University of Split</wicri:noRegion></affiliation><affiliation wicri:level="1"><country xml:lang="fr">Allemagne</country><wicri:regionArea>Humboldt‐Universität Berlin, Institut für Chemie</wicri:regionArea><wicri:noRegion>Institut für Chemie</wicri:noRegion><wicri:noRegion>Institut für Chemie</wicri:noRegion></affiliation><affiliation wicri:level="1"><country wicri:rule="url">Allemagne</country></affiliation><affiliation wicri:level="4"><country xml:lang="fr">Australie</country><wicri:regionArea>Vlasta Bonačić‐Koutecký, Interdisciplinary Center for Advanced Science and Technology (ICAST), University of Split, Split (Croatia)Philippe Dugourd, Université of Lyon, 69622 (France)Richard A. J. O'Hair, School of Chemistry, University of Melbourne</wicri:regionArea><placeName><settlement type="city">Melbourne</settlement><region type="état">Victoria (État)</region></placeName><orgName type="university">Université de Melbourne</orgName></affiliation></author><author><name sortKey="Dugourd, Philippe" sort="Dugourd, Philippe" uniqKey="Dugourd P" first="Philippe" last="Dugourd">Philippe Dugourd</name><affiliation wicri:level="1"><country xml:lang="fr">France</country><wicri:regionArea>Université of Lyon</wicri:regionArea></affiliation><affiliation wicri:level="1"><country xml:lang="fr">France</country><wicri:regionArea>Institut Lumière Matière, Université Lyon 1, CNRS UMR 5306</wicri:regionArea><wicri:noRegion>CNRS UMR 5306</wicri:noRegion><wicri:noRegion>CNRS UMR 5306</wicri:noRegion></affiliation><affiliation wicri:level="1"><country wicri:rule="url">France</country></affiliation><affiliation wicri:level="4"><country xml:lang="fr">Australie</country><wicri:regionArea>Vlasta Bonačić‐Koutecký, Interdisciplinary Center for Advanced Science and Technology (ICAST), University of Split, Split (Croatia)Philippe Dugourd, Université of Lyon, 69622 (France)Richard A. J. O'Hair, School of Chemistry, University of Melbourne</wicri:regionArea><placeName><settlement type="city">Melbourne</settlement><region type="état">Victoria (État)</region></placeName><orgName type="university">Université de Melbourne</orgName></affiliation></author><author><name sortKey="O Hair, Richard A J" sort="O Hair, Richard A J" uniqKey="O Hair R" first="Richard A. J." last="O'Hair">Richard A. J. O'Hair</name><affiliation wicri:level="4"><country xml:lang="fr">Australie</country><wicri:regionArea>School of Chemistry, University of Melbourne</wicri:regionArea><placeName><settlement type="city">Melbourne</settlement><region type="état">Victoria (État)</region></placeName><orgName type="university">Université de Melbourne</orgName></affiliation><affiliation wicri:level="1"><country wicri:rule="url">Australie</country></affiliation><affiliation wicri:level="4"><country xml:lang="fr">Australie</country><wicri:regionArea>Vlasta Bonačić‐Koutecký, Interdisciplinary Center for Advanced Science and Technology (ICAST), University of Split, Split (Croatia)Philippe Dugourd, Université of Lyon, 69622 (France)Richard A. J. O'Hair, School of Chemistry, University of Melbourne</wicri:regionArea><placeName><settlement type="city">Melbourne</settlement><region type="état">Victoria (État)</region></placeName><orgName type="university">Université de Melbourne</orgName></affiliation></author></analytic><monogr></monogr><series><title level="j" type="main">Chemistry – A European Journal</title><title level="j" type="alt">CHEMISTRY - A EUROPEAN JOURNAL</title><idno type="ISSN">0947-6539</idno><idno type="eISSN">1521-3765</idno><imprint><biblScope unit="vol">20</biblScope><biblScope unit="issue">50</biblScope><biblScope unit="page" from="16626">16626</biblScope><biblScope unit="page" to="16633">16633</biblScope><biblScope unit="page-count">8</biblScope><publisher>WILEY‐VCH Verlag</publisher><pubPlace>Weinheim</pubPlace><date type="published" when="2014-12-08">2014-12-08</date></imprint><idno type="ISSN">0947-6539</idno></series></biblStruct></sourceDesc><seriesStmt><idno type="ISSN">0947-6539</idno></seriesStmt></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Multistage mass spectrometry and density functional theory (DFT) were used to characterise the small silver hydride nanocluster, [Ag3H2L]+ (where L=(Ph2P)2CH2) and its gas‐phase unimolecular chemistry. Collision‐induced dissociation (CID) yields [Ag2HL]+ as the major product while laser‐induced dissociation (LID) proceeds via H2 formation and subsequent release from [Ag3H2L]+, giving rise to [Ag3L]+ as the major product. Deuterium labelling studies on [Ag3D2L]+ prove that the source of H2 is from the hydrides and not from the ligand. Comparison of TD‐DFT absorption patterns obtained for the optimised structures with action spectroscopy results, allows assignment of the measured features to structures of precursors and products. Molecular dynamics “on the fly” reveal that AgH loss is favoured in the ground state, but H2 formation and loss is preferred in the first excited state S1, in agreement with CID and LID experimental findings. This indicates favourable photo‐induced formation of H2 and subsequent release from [Ag3H2L]+, an important finding in context of metal hydrides as a hydrogen storage medium, which can subsequently be released by heating or irradiation with light.</div></front></TEI><affiliations><list><country><li>Allemagne</li><li>Australie</li><li>Croatie</li><li>France</li></country><region><li>Victoria (État)</li></region><settlement><li>Melbourne</li></settlement><orgName><li>Université de Melbourne</li></orgName></list><tree><country name="France"><noRegion><name sortKey="Girod, Marion" sort="Girod, Marion" uniqKey="Girod M" first="Marion" last="Girod">Marion Girod</name></noRegion><name sortKey="Antoine, Rodolphe" sort="Antoine, Rodolphe" uniqKey="Antoine R" first="Rodolphe" last="Antoine">Rodolphe Antoine</name><name sortKey="Antoine, Rodolphe" sort="Antoine, Rodolphe" uniqKey="Antoine R" first="Rodolphe" last="Antoine">Rodolphe Antoine</name><name sortKey="Dugourd, Philippe" sort="Dugourd, Philippe" uniqKey="Dugourd P" first="Philippe" last="Dugourd">Philippe Dugourd</name><name sortKey="Dugourd, Philippe" sort="Dugourd, Philippe" uniqKey="Dugourd P" first="Philippe" last="Dugourd">Philippe Dugourd</name><name sortKey="Dugourd, Philippe" sort="Dugourd, Philippe" uniqKey="Dugourd P" first="Philippe" last="Dugourd">Philippe Dugourd</name><name sortKey="Girod, Marion" sort="Girod, Marion" uniqKey="Girod M" first="Marion" last="Girod">Marion Girod</name><name sortKey="Lemoine, Jerome" sort="Lemoine, Jerome" uniqKey="Lemoine J" first="Jérome" last="Lemoine">Jérome Lemoine</name><name sortKey="Lemoine, Jerome" sort="Lemoine, Jerome" uniqKey="Lemoine J" first="Jérome" last="Lemoine">Jérome Lemoine</name><name sortKey="Macaleese, Luke" sort="Macaleese, Luke" uniqKey="Macaleese L" first="Luke" last="Macaleese">Luke Macaleese</name><name sortKey="Macaleese, Luke" sort="Macaleese, Luke" uniqKey="Macaleese L" first="Luke" last="Macaleese">Luke Macaleese</name></country><country name="Croatie"><noRegion><name sortKey="Krsti, Marjan" sort="Krsti, Marjan" uniqKey="Krsti M" first="Marjan" last="Krsti">Marjan Krsti</name></noRegion><name sortKey="Bona I Outeck, Vlasta" sort="Bona I Outeck, Vlasta" uniqKey="Bona I Outeck V" first="Vlasta" last="Bona I Outeck">Vlasta Bona I Outeck</name></country><country name="Australie"><region name="Victoria (État)"><name sortKey="Zavras, Athanasios" sort="Zavras, Athanasios" uniqKey="Zavras A" first="Athanasios" last="Zavras">Athanasios Zavras</name></region><name sortKey="Bona I Outeck, Vlasta" sort="Bona I Outeck, Vlasta" uniqKey="Bona I Outeck V" first="Vlasta" last="Bona I Outeck">Vlasta Bona I Outeck</name><name sortKey="Dugourd, Philippe" sort="Dugourd, Philippe" uniqKey="Dugourd P" first="Philippe" last="Dugourd">Philippe Dugourd</name><name sortKey="Khairallah, George N" sort="Khairallah, George N" uniqKey="Khairallah G" first="George N." last="Khairallah">George N. Khairallah</name><name sortKey="O Hair, Richard A J" sort="O Hair, Richard A J" uniqKey="O Hair R" first="Richard A. J." last="O'Hair">Richard A. J. O'Hair</name><name sortKey="O Hair, Richard A J" sort="O Hair, Richard A J" uniqKey="O Hair R" first="Richard A. J." last="O'Hair">Richard A. J. O'Hair</name><name sortKey="O Hair, Richard A J" sort="O Hair, Richard A J" uniqKey="O Hair R" first="Richard A. J." last="O'Hair">Richard A. J. O'Hair</name></country><country name="Allemagne"><noRegion><name sortKey="Bona I Outeck, Vlasta" sort="Bona I Outeck, Vlasta" uniqKey="Bona I Outeck V" first="Vlasta" last="Bona I Outeck">Vlasta Bona I Outeck</name></noRegion><name sortKey="Bona I Outeck, Vlasta" sort="Bona I Outeck, Vlasta" uniqKey="Bona I Outeck V" first="Vlasta" last="Bona I Outeck">Vlasta Bona I Outeck</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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