Mechanistic Picture and Kinetic Analysis of Surface-Confined Ullmann Polymerization.
Identifieur interne : 001487 ( PubMed/Corpus ); précédent : 001486; suivant : 001488Mechanistic Picture and Kinetic Analysis of Surface-Confined Ullmann Polymerization.
Auteurs : Marco Di Giovannantonio ; Massimo Tomellini ; Josh Lipton-Duffin ; Gianluca Galeotti ; Maryam Ebrahimi ; Albano Cossaro ; Alberto Verdini ; Neerav Kharche ; Vincent Meunier ; Guillaume Vasseur ; Yannick Fagot-Revurat ; Dmitrii F. Perepichka ; Federico Rosei ; Giorgio ContiniSource :
- 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
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Perepichka</name><affiliation><nlm:affiliation>Department of Chemistry, McGill University , 801 Sherbrooke Street, West Montreal, Quebec H3A 0B8, Canada.</nlm:affiliation></affiliation></author><author><name sortKey="Rosei, Federico" sort="Rosei, Federico" uniqKey="Rosei F" first="Federico" last="Rosei">Federico Rosei</name><affiliation><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation></affiliation></author><author><name sortKey="Contini, Giorgio" sort="Contini, Giorgio" uniqKey="Contini G" first="Giorgio" last="Contini">Giorgio Contini</name><affiliation><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation></affiliation></author></titleStmt><publicationStmt><idno type="wicri:source">PubMed</idno><date when="2016">2016</date><idno type="RBID">pubmed:27958750</idno><idno type="pmid">27958750</idno><idno type="doi">10.1021/jacs.6b09728</idno><idno type="wicri:Area/PubMed/Corpus">001487</idno><idno type="wicri:explorRef" wicri:stream="PubMed" wicri:step="Corpus" wicri:corpus="PubMed">001487</idno></publicationStmt><sourceDesc><biblStruct><analytic><title xml:lang="en">Mechanistic Picture and Kinetic Analysis of Surface-Confined Ullmann Polymerization.</title><author><name sortKey="Di Giovannantonio, Marco" sort="Di Giovannantonio, Marco" uniqKey="Di Giovannantonio M" first="Marco" last="Di Giovannantonio">Marco Di Giovannantonio</name><affiliation><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation></affiliation></author><author><name sortKey="Tomellini, Massimo" sort="Tomellini, Massimo" uniqKey="Tomellini M" first="Massimo" last="Tomellini">Massimo Tomellini</name><affiliation><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation></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><nlm:affiliation>Institute for Future Environments, Queensland University of Technology (QUT) , 2 George Street, Brisbane, Queensland 4001, Australia.</nlm:affiliation></affiliation></author><author><name sortKey="Galeotti, Gianluca" sort="Galeotti, Gianluca" uniqKey="Galeotti G" first="Gianluca" last="Galeotti">Gianluca Galeotti</name><affiliation><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation></affiliation></author><author><name sortKey="Ebrahimi, Maryam" sort="Ebrahimi, Maryam" uniqKey="Ebrahimi M" first="Maryam" last="Ebrahimi">Maryam Ebrahimi</name><affiliation><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation></affiliation></author><author><name sortKey="Cossaro, Albano" sort="Cossaro, Albano" uniqKey="Cossaro A" first="Albano" last="Cossaro">Albano Cossaro</name><affiliation><nlm:affiliation>CNR-IOM , Laboratorio TASC, 34149 Trieste, Italy.</nlm:affiliation></affiliation></author><author><name sortKey="Verdini, Alberto" sort="Verdini, Alberto" uniqKey="Verdini A" first="Alberto" last="Verdini">Alberto Verdini</name><affiliation><nlm:affiliation>CNR-IOM , Laboratorio TASC, 34149 Trieste, Italy.</nlm:affiliation></affiliation></author><author><name sortKey="Kharche, Neerav" sort="Kharche, Neerav" uniqKey="Kharche N" first="Neerav" last="Kharche">Neerav Kharche</name><affiliation><nlm:affiliation>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180, United States.</nlm:affiliation></affiliation></author><author><name sortKey="Meunier, Vincent" sort="Meunier, Vincent" uniqKey="Meunier V" first="Vincent" last="Meunier">Vincent Meunier</name><affiliation><nlm:affiliation>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180, United States.</nlm:affiliation></affiliation></author><author><name sortKey="Vasseur, Guillaume" sort="Vasseur, Guillaume" uniqKey="Vasseur G" first="Guillaume" last="Vasseur">Guillaume Vasseur</name><affiliation><nlm:affiliation>Donostia International Physics Center (DIPC) , Paseo Manuel Lardizabal 4, 20018 San Sebastián, Spain.</nlm:affiliation></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><nlm:affiliation>Institut Jean Lamour, UMR 7198, Université de Lorraine/CNRS , B.P. 70239, Vandoeuvre-Les-Nancy F-54506, France.</nlm:affiliation></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><nlm:affiliation>Department of Chemistry, McGill University , 801 Sherbrooke Street, West Montreal, Quebec H3A 0B8, Canada.</nlm:affiliation></affiliation></author><author><name sortKey="Rosei, Federico" sort="Rosei, Federico" uniqKey="Rosei F" first="Federico" last="Rosei">Federico Rosei</name><affiliation><nlm:affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</nlm:affiliation></affiliation></author><author><name sortKey="Contini, Giorgio" sort="Contini, Giorgio" uniqKey="Contini G" first="Giorgio" last="Contini">Giorgio Contini</name><affiliation><nlm:affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</nlm:affiliation></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><pubmed><MedlineCitation Status="In-Data-Review" Owner="NLM"><PMID Version="1">27958750</PMID><DateCreated><Year>2016</Year><Month>12</Month><Day>13</Day></DateCreated><DateRevised><Year>2016</Year><Month>12</Month><Day>28</Day></DateRevised><Article PubModel="Print-Electronic"><Journal><ISSN IssnType="Electronic">1520-5126</ISSN><JournalIssue CitedMedium="Internet"><Volume>138</Volume><Issue>51</Issue><PubDate><Year>2016</Year><Month>Dec</Month><Day>28</Day></PubDate></JournalIssue><Title>Journal of the American Chemical Society</Title><ISOAbbreviation>J. Am. Chem. Soc.</ISOAbbreviation></Journal><ArticleTitle>Mechanistic Picture and Kinetic Analysis of Surface-Confined Ullmann Polymerization.</ArticleTitle><Pagination><MedlinePgn>16696-16702</MedlinePgn></Pagination><ELocationID EIdType="doi" ValidYN="Y">10.1021/jacs.6b09728</ELocationID><Abstract><AbstractText>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.</AbstractText></Abstract><AuthorList CompleteYN="Y"><Author ValidYN="Y"><LastName>Di Giovannantonio</LastName><ForeName>Marco</ForeName><Initials>M</Initials><AffiliationInfo><Affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Tomellini</LastName><ForeName>Massimo</ForeName><Initials>M</Initials><AffiliationInfo><Affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Lipton-Duffin</LastName><ForeName>Josh</ForeName><Initials>J</Initials><AffiliationInfo><Affiliation>Institute for Future Environments, Queensland University of Technology (QUT) , 2 George Street, Brisbane, Queensland 4001, Australia.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Galeotti</LastName><ForeName>Gianluca</ForeName><Initials>G</Initials><AffiliationInfo><Affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Ebrahimi</LastName><ForeName>Maryam</ForeName><Initials>M</Initials><AffiliationInfo><Affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Cossaro</LastName><ForeName>Albano</ForeName><Initials>A</Initials><AffiliationInfo><Affiliation>CNR-IOM , Laboratorio TASC, 34149 Trieste, Italy.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Verdini</LastName><ForeName>Alberto</ForeName><Initials>A</Initials><Identifier Source="ORCID">http://orcid.org/0000-0001-8880-2080</Identifier><AffiliationInfo><Affiliation>CNR-IOM , Laboratorio TASC, 34149 Trieste, Italy.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Kharche</LastName><ForeName>Neerav</ForeName><Initials>N</Initials><AffiliationInfo><Affiliation>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180, United States.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Meunier</LastName><ForeName>Vincent</ForeName><Initials>V</Initials><AffiliationInfo><Affiliation>Department of Physics, Applied Physics, and Astronomy, Rensselaer Polytechnic Institute , 110 Eighth Street, Troy, New York 12180, United States.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Vasseur</LastName><ForeName>Guillaume</ForeName><Initials>G</Initials><AffiliationInfo><Affiliation>Donostia International Physics Center (DIPC) , Paseo Manuel Lardizabal 4, 20018 San Sebastián, Spain.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Fagot-Revurat</LastName><ForeName>Yannick</ForeName><Initials>Y</Initials><AffiliationInfo><Affiliation>Institut Jean Lamour, UMR 7198, Université de Lorraine/CNRS , B.P. 70239, Vandoeuvre-Les-Nancy F-54506, France.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Perepichka</LastName><ForeName>Dmitrii F</ForeName><Initials>DF</Initials><AffiliationInfo><Affiliation>Department of Chemistry, McGill University , 801 Sherbrooke Street, West Montreal, Quebec H3A 0B8, Canada.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Rosei</LastName><ForeName>Federico</ForeName><Initials>F</Initials><AffiliationInfo><Affiliation>Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique , 1650 Boulevard Lionel-Boulet, Varennes, Quebec J3X 1S2, Canada.</Affiliation></AffiliationInfo><AffiliationInfo><Affiliation>Institute for Fundamental and Frontier Science, University of Electronic Science and Technology of China , Chengdu 610054, PR China.</Affiliation></AffiliationInfo></Author><Author ValidYN="Y"><LastName>Contini</LastName><ForeName>Giorgio</ForeName><Initials>G</Initials><Identifier Source="ORCID">http://orcid.org/0000-0002-6248-9716</Identifier><AffiliationInfo><Affiliation>Istituto di Struttura della Materia, CNR , Via Fosso del Cavaliere 100, 00133 Roma, Italy.</Affiliation></AffiliationInfo></Author></AuthorList><Language>eng</Language><PublicationTypeList><PublicationType UI="D016428">Journal Article</PublicationType></PublicationTypeList><ArticleDate DateType="Electronic"><Year>2016</Year><Month>12</Month><Day>13</Day></ArticleDate></Article><MedlineJournalInfo><Country>United States</Country><MedlineTA>J Am Chem Soc</MedlineTA><NlmUniqueID>7503056</NlmUniqueID><ISSNLinking>0002-7863</ISSNLinking></MedlineJournalInfo></MedlineCitation><PubmedData><History><PubMedPubDate PubStatus="pubmed"><Year>2016</Year><Month>12</Month><Day>14</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="medline"><Year>2016</Year><Month>12</Month><Day>14</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate><PubMedPubDate PubStatus="entrez"><Year>2016</Year><Month>12</Month><Day>14</Day><Hour>6</Hour><Minute>0</Minute></PubMedPubDate></History><PublicationStatus>ppublish</PublicationStatus><ArticleIdList><ArticleId IdType="pubmed">27958750</ArticleId><ArticleId IdType="doi">10.1021/jacs.6b09728</ArticleId></ArticleIdList></PubmedData></pubmed></record>Pour manipuler ce 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