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dc.contributor.author
Feng, Min
dc.contributor.author
Petek, Hrvoje
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Shi, Yongliang
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Sun, Hao
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Zhao, Jin
dc.contributor.author
Calaza, Florencia Carolina
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dc.contributor.author
Sterrer, Martin
dc.contributor.author
Freund, Hans
dc.date.available
2016-12-20T19:29:22Z
dc.date.issued
2015-11
dc.identifier.citation
Feng, Min; Petek, Hrvoje; Shi, Yongliang; Sun, Hao; Zhao, Jin; et al.; Cooperative Chemisorption-Induced Physisorption of CO2 Molecules by Metal-Organic Chains; American Chemical Society; Acs Nano; 9; 11-2015; 12124-12136
dc.identifier.issn
1936-0851
dc.identifier.uri
http://hdl.handle.net/11336/9841
dc.description.abstract
Effective CO2 capture and reduction can be achieved through a molecularscale understanding of interaction of CO2 molecules with chemically active sites and thecooperative effects they induce in functional materials. Self-assembled arrays of parallelchains composed of Au adatoms connected by 1,4-phenylene diisocyanide (PDI) linkersdecorating Au surfaces exhibit self-catalyzed CO2 capture leading to large scale surfacerestructuring at 77 K (ACS Nano 2014, 8, 86448652). We explore the cooperativeinteractions among CO2 molecules, Au-PDI chains and Au substrates that are responsiblefor the self-catalyzed capture by low temperature scanning tunneling microscopy (LTSTM),X-ray photoelectron spectroscopy (XPS), infrared reflection absorption spectroscopy(IRAS), temperature-programmed desorption (TPD), and dispersion corrected densityfunctional theory (DFT). Decorating Au surfaces with Au-PDI chains gives the interfacialmetalorganic polymer characteristics of both a homogeneous and heterogeneouscatalyst. Au-PDI chains activate the normally inert Au surfaces by promoting CO2 chemisorption at the Au adatom sites even at <20 K. The CO2 δ- speciescoordinating Au adatoms in-turn seed physisorption of CO2 molecules in highly ordered two-dimensional (2D) clusters, which grow with increasing dose to a fullmonolayer and, surprisingly, can be imaged withmolecular resolution on Au crystal terraces. The dispersion interactions with the substrate force the monolayerto assume a rhombic structure similar to a high-pressure CO2 crystalline solid rather than the cubic dry ice phase. The Au surface supported Au-PDI chains providea platform for investigating the physical and chemical interactions involved in CO2 capture and reduction.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
American Chemical Society
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dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
Co2 . Co2 Δ- . Co2 Reduction . Co2 Cluster
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Chemisorption Induced Physisorption
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Metalorganic Chains
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1,4-Phenylene Diisocyanide
dc.subject.classification
Física Atómica, Molecular y Química
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dc.subject.classification
Ciencias Físicas
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dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
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dc.title
Cooperative Chemisorption-Induced Physisorption of CO2 Molecules by Metal-Organic Chains
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2016-12-16T14:28:25Z
dc.journal.volume
9
dc.journal.pagination
12124-12136
dc.journal.pais
Estados Unidos
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dc.journal.ciudad
Washington
dc.description.fil
Fil: Feng, Min. Chinese Academy Of Sciences; República de China. University Of Pittsburgh; Estados Unidos
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Fil: Petek, Hrvoje. University of Pittsburgh; Estados Unidos
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Fil: Shi, Yongliang. University of Science and Technology of China; China
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Fil: Sun, Hao. University of Science and Technology of China; China
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Fil: Zhao, Jin. University of Science and Technology of China; China
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Fil: Calaza, Florencia Carolina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química (i); Argentina
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Fil: Sterrer, Martin. Fritz-Haber-Institute der Max-Plank-Gesellschaft; Alemania
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Fil: Freund, Hans. University Of Graz; Austria
dc.journal.title
Acs Nano
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dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/acsnano.5b05222
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1021/acsnano.5b05222
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