Mechanistic Picture and Kinetic Analysis of Surface-Confined Ullmann Polymerization.
Identifieur interne : 001B34 ( Main/Exploration ); précédent : 001B33; suivant : 001B35Mechanistic Picture and Kinetic Analysis of Surface-Confined Ullmann Polymerization.
Auteurs : Marco Di Giovannantonio [Italie] ; Massimo Tomellini [Italie] ; Josh Lipton-Duffin [Australie] ; Gianluca Galeotti [Canada] ; Maryam Ebrahimi [Canada] ; Albano Cossaro [Italie] ; Alberto Verdini [Italie] ; Neerav Kharche [États-Unis] ; Vincent Meunier [États-Unis] ; Guillaume Vasseur [Espagne] ; Yannick Fagot-Revurat [France] ; Dmitrii F. Perepichka [Canada] ; Federico Rosei [Canada] ; Giorgio Contini [Italie]Source :
- Journal of the American Chemical Society [ 1520-5126 ] ; 2016.
Abstract
Surface-confined polymerization via Ullmann coupling is a promising route to create one- and two-dimensional covalent π-conjugated structures, including the bottom-up growth of graphene nanoribbons. Understanding the mechanism of the Ullmann reaction is necessary to provide a platform for rationally controlling the formation of these materials. We use fast X-ray photoelectron spectroscopy (XPS) in kinetic measurements of epitaxial surface polymerization of 1,4-dibromobenzene on Cu(110) and devise a kinetic model based on mean field rate equations, involving a transient state. This state is observed in the energy landscapes calculated by nudged elastic band (NEB) within density functional theory (DFT), which assumes as initial and final geometries of the organometallic and polymeric structures those observed by scanning tunneling microscopy (STM). The kinetic model accounts for all the salient features observed in the experimental curves extracted from the fast-XPS measurements and enables an enhanced understanding of the polymerization process, which is found to follow a nucleation-and-growth behavior preceded by the formation of a transient state.
DOI: 10.1021/jacs.6b09728
PubMed: 27958750
Affiliations:
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wicri:level="1"><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation><country xml:lang="fr">Italie</country><wicri:regionArea>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma</wicri:regionArea><placeName><settlement type="city">Rome</settlement><region nuts="2">Latium</region></placeName></affiliation></author><author><name sortKey="Tomellini, Massimo" sort="Tomellini, Massimo" uniqKey="Tomellini M" first="Massimo" last="Tomellini">Massimo Tomellini</name><affiliation wicri:level="1"><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation><country xml:lang="fr">Italie</country><wicri:regionArea>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma</wicri:regionArea><placeName><settlement type="city">Rome</settlement><region nuts="2">Latium</region></placeName></affiliation></author><author><name sortKey="Lipton Duffin, Josh" sort="Lipton Duffin, Josh" uniqKey="Lipton Duffin J" first="Josh" last="Lipton-Duffin">Josh Lipton-Duffin</name><affiliation wicri:level="1"><nlm:affiliation>Institute for Future Environments, Queensland University of Technology (QUT) , 2 George Street, Brisbane, Queensland 4001, Australia.</nlm:affiliation><country xml:lang="fr">Australie</country><wicri:regionArea>Institute for Future Environments, Queensland University of Technology (QUT) , 2 George Street, Brisbane, Queensland 4001</wicri:regionArea><wicri:noRegion>Queensland 4001</wicri:noRegion></affiliation></author><author><name sortKey="Galeotti, Gianluca" sort="Galeotti, Gianluca" uniqKey="Galeotti G" first="Gianluca" last="Galeotti">Gianluca Galeotti</name><affiliation wicri:level="1"><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation><country xml:lang="fr">Canada</country><wicri:regionArea>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2</wicri:regionArea><wicri:noRegion>Quebec J3X 1S2</wicri:noRegion></affiliation></author><author><name sortKey="Ebrahimi, Maryam" sort="Ebrahimi, Maryam" uniqKey="Ebrahimi M" first="Maryam" last="Ebrahimi">Maryam Ebrahimi</name><affiliation wicri:level="1"><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation><country xml:lang="fr">Canada</country><wicri:regionArea>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2</wicri:regionArea><wicri:noRegion>Quebec J3X 1S2</wicri:noRegion></affiliation></author><author><name sortKey="Cossaro, Albano" sort="Cossaro, Albano" uniqKey="Cossaro A" first="Albano" last="Cossaro">Albano Cossaro</name><affiliation wicri:level="1"><nlm:affiliation>CNR-IOM , Laboratorio TASC, 34149 Trieste, Italy.</nlm:affiliation><country xml:lang="fr">Italie</country><wicri:regionArea>CNR-IOM , Laboratorio TASC, 34149 Trieste</wicri:regionArea><wicri:noRegion>34149 Trieste</wicri:noRegion></affiliation></author><author><name sortKey="Verdini, Alberto" sort="Verdini, Alberto" uniqKey="Verdini A" first="Alberto" last="Verdini">Alberto Verdini</name><affiliation wicri:level="1"><nlm:affiliation>CNR-IOM , Laboratorio TASC, 34149 Trieste, Italy.</nlm:affiliation><country xml:lang="fr">Italie</country><wicri:regionArea>CNR-IOM , Laboratorio TASC, 34149 Trieste</wicri:regionArea><wicri:noRegion>34149 Trieste</wicri:noRegion></affiliation></author><author><name sortKey="Kharche, Neerav" sort="Kharche, Neerav" uniqKey="Kharche N" first="Neerav" last="Kharche">Neerav Kharche</name><affiliation wicri:level="1"><nlm:affiliation>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180, United States.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180</wicri:regionArea><wicri:noRegion>New York 12180</wicri:noRegion></affiliation></author><author><name sortKey="Meunier, Vincent" sort="Meunier, Vincent" uniqKey="Meunier V" first="Vincent" last="Meunier">Vincent Meunier</name><affiliation wicri:level="1"><nlm:affiliation>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180, United States.</nlm:affiliation><country xml:lang="fr">États-Unis</country><wicri:regionArea>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180</wicri:regionArea><wicri:noRegion>New York 12180</wicri:noRegion></affiliation></author><author><name sortKey="Vasseur, Guillaume" sort="Vasseur, Guillaume" uniqKey="Vasseur G" first="Guillaume" last="Vasseur">Guillaume Vasseur</name><affiliation wicri:level="1"><nlm:affiliation>Donostia International Physics Center (DIPC) , Paseo Manuel Lardizabal 4, 20018 San Sebastián, Spain.</nlm:affiliation><country xml:lang="fr">Espagne</country><wicri:regionArea>Donostia International Physics Center (DIPC) , Paseo Manuel Lardizabal 4, 20018 San Sebastián</wicri:regionArea><wicri:noRegion>20018 San Sebastián</wicri:noRegion></affiliation></author><author><name sortKey="Fagot Revurat, Yannick" sort="Fagot Revurat, Yannick" uniqKey="Fagot Revurat Y" first="Yannick" last="Fagot-Revurat">Yannick Fagot-Revurat</name><affiliation wicri:level="1"><nlm:affiliation>Institut Jean Lamour, UMR 7198, Université de Lorraine/CNRS , B.P. 70239, Vandoeuvre-Les-Nancy F-54506, France.</nlm:affiliation><country xml:lang="fr">France</country><wicri:regionArea>Institut Jean Lamour, UMR 7198, Université de Lorraine/CNRS , B.P. 70239, Vandoeuvre-Les-Nancy F-54506</wicri:regionArea><wicri:noRegion>54506</wicri:noRegion><wicri:noRegion>54506</wicri:noRegion></affiliation></author><author><name sortKey="Perepichka, Dmitrii F" sort="Perepichka, Dmitrii F" uniqKey="Perepichka D" first="Dmitrii F" last="Perepichka">Dmitrii F. Perepichka</name><affiliation wicri:level="1"><nlm:affiliation>Department of Chemistry, McGill University , 801 Sherbrooke Street, West Montreal, Quebec H3A 0B8, Canada.</nlm:affiliation><country xml:lang="fr">Canada</country><wicri:regionArea>Department of Chemistry, McGill University , 801 Sherbrooke Street, West Montreal, Quebec H3A 0B8</wicri:regionArea><wicri:noRegion>Quebec H3A 0B8</wicri:noRegion></affiliation></author><author><name sortKey="Rosei, Federico" sort="Rosei, Federico" uniqKey="Rosei F" first="Federico" last="Rosei">Federico Rosei</name><affiliation wicri:level="1"><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation><country xml:lang="fr">Canada</country><wicri:regionArea>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2</wicri:regionArea><wicri:noRegion>Quebec J3X 1S2</wicri:noRegion></affiliation></author><author><name sortKey="Contini, Giorgio" sort="Contini, Giorgio" uniqKey="Contini G" first="Giorgio" last="Contini">Giorgio Contini</name><affiliation wicri:level="1"><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation><country xml:lang="fr">Italie</country><wicri:regionArea>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma</wicri:regionArea><placeName><settlement type="city">Rome</settlement><region nuts="2">Latium</region></placeName></affiliation></author></analytic><series><title level="j">Journal of the American Chemical Society</title><idno type="eISSN">1520-5126</idno><imprint><date when="2016" type="published">2016</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Surface-confined polymerization via Ullmann coupling is a promising route to create one- and two-dimensional covalent π-conjugated structures, including the bottom-up growth of graphene nanoribbons. Understanding the mechanism of the Ullmann reaction is necessary to provide a platform for rationally controlling the formation of these materials. We use fast X-ray photoelectron spectroscopy (XPS) in kinetic measurements of epitaxial surface polymerization of 1,4-dibromobenzene on Cu(110) and devise a kinetic model based on mean field rate equations, involving a transient state. This state is observed in the energy landscapes calculated by nudged elastic band (NEB) within density functional theory (DFT), which assumes as initial and final geometries of the organometallic and polymeric structures those observed by scanning tunneling microscopy (STM). The kinetic model accounts for all the salient features observed in the experimental curves extracted from the fast-XPS measurements and enables an enhanced understanding of the polymerization process, which is found to follow a nucleation-and-growth behavior preceded by the formation of a transient state.</div></front></TEI><affiliations><list><country><li>Australie</li><li>Canada</li><li>Espagne</li><li>France</li><li>Italie</li><li>États-Unis</li></country><region><li>Latium</li></region><settlement><li>Rome</li></settlement></list><tree><country name="Italie"><region name="Latium"><name sortKey="Di Giovannantonio, Marco" sort="Di Giovannantonio, Marco" uniqKey="Di Giovannantonio M" first="Marco" last="Di Giovannantonio">Marco Di Giovannantonio</name></region><name sortKey="Contini, Giorgio" sort="Contini, Giorgio" uniqKey="Contini G" first="Giorgio" last="Contini">Giorgio Contini</name><name sortKey="Cossaro, Albano" sort="Cossaro, Albano" uniqKey="Cossaro A" first="Albano" last="Cossaro">Albano Cossaro</name><name sortKey="Tomellini, Massimo" sort="Tomellini, Massimo" uniqKey="Tomellini M" first="Massimo" last="Tomellini">Massimo Tomellini</name><name sortKey="Verdini, Alberto" sort="Verdini, Alberto" uniqKey="Verdini A" first="Alberto" last="Verdini">Alberto Verdini</name></country><country name="Australie"><noRegion><name sortKey="Lipton Duffin, Josh" sort="Lipton Duffin, Josh" uniqKey="Lipton Duffin J" first="Josh" last="Lipton-Duffin">Josh Lipton-Duffin</name></noRegion></country><country name="Canada"><noRegion><name sortKey="Galeotti, Gianluca" sort="Galeotti, Gianluca" uniqKey="Galeotti G" first="Gianluca" last="Galeotti">Gianluca Galeotti</name></noRegion><name sortKey="Ebrahimi, Maryam" sort="Ebrahimi, Maryam" uniqKey="Ebrahimi M" first="Maryam" last="Ebrahimi">Maryam Ebrahimi</name><name sortKey="Perepichka, Dmitrii F" sort="Perepichka, Dmitrii F" uniqKey="Perepichka D" first="Dmitrii F" last="Perepichka">Dmitrii F. Perepichka</name><name sortKey="Rosei, Federico" sort="Rosei, Federico" uniqKey="Rosei F" first="Federico" last="Rosei">Federico Rosei</name></country><country name="États-Unis"><noRegion><name sortKey="Kharche, Neerav" sort="Kharche, Neerav" uniqKey="Kharche N" first="Neerav" last="Kharche">Neerav Kharche</name></noRegion><name sortKey="Meunier, Vincent" sort="Meunier, Vincent" uniqKey="Meunier V" first="Vincent" last="Meunier">Vincent Meunier</name></country><country name="Espagne"><noRegion><name sortKey="Vasseur, Guillaume" sort="Vasseur, Guillaume" uniqKey="Vasseur G" first="Guillaume" last="Vasseur">Guillaume Vasseur</name></noRegion></country><country name="France"><noRegion><name sortKey="Fagot Revurat, Yannick" sort="Fagot Revurat, Yannick" uniqKey="Fagot Revurat Y" first="Yannick" last="Fagot-Revurat">Yannick Fagot-Revurat</name></noRegion></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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HfdIndexSelect -h $EXPLOR_AREA/Data/Main/Exploration/RBID.i -Sk "pubmed:27958750" \
| HfdSelect -Kh $EXPLOR_AREA/Data/Main/Exploration/biblio.hfd \
| NlmPubMed2Wicri -a AustralieFrV1
| This area was generated with Dilib version V0.6.33. |  |