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dc.contributor.author
Cattaneo, Mauricio  
dc.contributor.author
Guo, Facheng  
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Kelly, H. Ray  
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Videla, Pablo E.  
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Kiefer, Laura  
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Gebre, Sara  
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Ge, Aimin  
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Liu, Qiliang  
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Wu, Shaoxiong  
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Lian, Tianquan  
dc.contributor.author
Batista, Víctor S.  
dc.date.available
2021-07-27T12:18:25Z  
dc.date.issued
2020-02  
dc.identifier.citation
Cattaneo, Mauricio; Guo, Facheng; Kelly, H. Ray; Videla, Pablo E.; Kiefer, Laura; et al.; Robust Binding of Disulfide-Substituted Rhenium Bipyridyl Complexes for CO2 Reduction on Gold Electrodes; Frontiers Media S.A.; Frontiers in Chemistry; 8; 2-2020; 1-10  
dc.identifier.issn
2296-2646  
dc.identifier.uri
http://hdl.handle.net/11336/137014  
dc.description.abstract
Heterogenization of homogenous catalysts on electrode surfaces provides a valuable approach for characterization of catalytic processes in operando conditions using surface selective spectroelectrochemistry methods. Ligand design plays a central role in the attachment mode and the resulting functionality of the heterogenized catalyst as determined by the orientation of the catalyst relative to the surface and the nature of specific interactions that modulate the redox properties under the heterogeneous electrode conditions. Here, we introduce new [Re(L)(CO)3Cl] catalysts for CO2 reduction with sulfur-based anchoring groups on a bipyridyl ligand, where L = 3,3′-disulfide-2,2′-bipyridine (SSbpy) and 3,3′-thio-2,2′-bipyridine (Sbpy). Spectroscopic and electrochemical analysis complemented by computational modeling at the density functional theory level identify the complex [Re(SSbpy)(CO)3Cl] as a multi-electron acceptor that combines the redox properties of both the rhenium tricarbonyl core and the disulfide functional group on the bipyridyl ligand. The first reduction at −0.85 V (vs. SCE) involves a two-electron process that breaks the disulfide bond, activating it for surface attachment. The heterogenized complex exhibits robust anchoring on gold surfaces, as probed by vibrational sum-frequency generation (SFG) spectroscopy. The binding configuration is normal to the surface, exposing the active site to the CO2 substrate in solution. The attachment mode is thus particularly suitable for electrocatalytic CO2 reduction.  
dc.format
application/pdf  
dc.language.iso
eng  
dc.publisher
Frontiers Media S.A.  
dc.rights
info:eu-repo/semantics/openAccess  
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/  
dc.subject
CO2 REDUCTION  
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DISULFIDE  
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MODIFIED GOLD SURFACES  
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RHENIUM COMPLEXES  
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SFG SPECTROSCOPY  
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SPECTROELECTROCHEMISTRY  
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Físico-Química, Ciencia de los Polímeros, Electroquímica  
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Ciencias Químicas  
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CIENCIAS NATURALES Y EXACTAS  
dc.title
Robust Binding of Disulfide-Substituted Rhenium Bipyridyl Complexes for CO2 Reduction on Gold Electrodes  
dc.type
info:eu-repo/semantics/article  
dc.type
info:ar-repo/semantics/artículo  
dc.type
info:eu-repo/semantics/publishedVersion  
dc.date.updated
2021-07-26T15:16:22Z  
dc.journal.volume
8  
dc.journal.pagination
1-10  
dc.journal.pais
Suiza  
dc.journal.ciudad
Viena  
dc.description.fil
Fil: Cattaneo, Mauricio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Química del Noroeste. Universidad Nacional de Tucumán. Facultad de Bioquímica, Química y Farmacia. Instituto de Química del Noroeste; Argentina  
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Fil: Guo, Facheng. University of Yale; Estados Unidos  
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Fil: Kelly, H. Ray. University of Yale; Estados Unidos  
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Fil: Videla, Pablo E.. University of Yale; Estados Unidos  
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Fil: Kiefer, Laura. Emory University; Estados Unidos  
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Fil: Gebre, Sara. Emory University; Estados Unidos  
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Fil: Ge, Aimin. Emory University; Estados Unidos  
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Fil: Liu, Qiliang. Emory University; Estados Unidos  
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Fil: Wu, Shaoxiong. Emory University; Estados Unidos  
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Fil: Lian, Tianquan. Emory University; Estados Unidos  
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Fil: Batista, Víctor S.. University of Yale; Estados Unidos  
dc.journal.title
Frontiers in Chemistry  
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://www.frontiersin.org/article/10.3389/fchem.2020.00086/full  
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.3389/fchem.2020.00086