| dc.contributor.author | Abarca, Gabriel [Univ Mayor, Fac Ciencias, Ctr Nanotecnol Aplicada] | es_CL |
| dc.contributor.author | Pizarro, Ana | es_CL |
| dc.contributor.author | Gutíérrez-Cerón, Cristián | es_CL |
| dc.contributor.author | Cortés-Arriagada, Diego | es_CL |
| dc.contributor.author | Bernardi, Fabiano | es_CL |
| dc.contributor.author | Berrios, Cristhian | es_CL |
| dc.contributor.author | Silva, Juan F. | es_CL |
| dc.contributor.author | Rezende, Marcos C. | es_CL |
| dc.contributor.author | Zagal, José H. | es_CL |
| dc.contributor.author | Onate, Rubén | es_CL |
| dc.contributor.author | Ponce, Ingrid | es_CL |
| dc.date.accessioned | 2020-04-08T14:11:55Z | |
| dc.date.accessioned | 2020-04-13T18:12:35Z | |
| dc.date.available | 2020-04-08T14:11:55Z | |
| dc.date.available | 2020-04-13T18:12:35Z | |
| dc.date.issued | 2018 | es_CL |
| dc.identifier.citation | Pizarro, A., Abarca, G., Gutiérrez-Cerón, C., Cortés-Arriagada, D., Bernardi, F., Berrios, C., ... & Ponce, I. (2018). Building pyridinium molecular wires as axial ligands for tuning the electrocatalytic activity of iron phthalocyanines for the oxygen reduction reaction. ACS Catalysis, 8(9), 8406-8419. | es_CL |
| dc.identifier.issn | 2155-5435 | es_CL |
| dc.identifier.uri | https://doi.org/10.1021/acscatal.8b01479 | es_CL |
| dc.identifier.uri | http://repositorio.umayor.cl/xmlui/handle/sibum/6108 | |
| dc.description.abstract | We have been able to"tune"the electrocatalytic activity of iron phthalocyanine (FePc) and iron hexadodeca-chlorophthalocyanine (16(Cl)FePc) for the oxygen reduction reaction (ORR) by manipulating the"pull effect"of pyridinium molecules axially bounded to the phthalocyanine complexes (FePcs). These axial ligands play both the role of molecular anchors and also of molecular wires. The axial ligands also affect the reactivity of the Fe metal center in the phthalocyanine. The"pull effect"originates from the positive charge located on the pyridinium core. We have explored the influence of the core positions (Up or Down), in two structural pyridiniums isomers on the activity of FePc and 16(Cl)FePc for the ORR. Of all self-assembled catalysts tested, the highest catalytic activity was exhibited by the Au(111)/Up/FePc system. XPS measurements and DFT calculations showed that it is possible to tailor the FePc-N(pyridiniums) Fe-O-2 binding energies, by changing the core positions and affecting the"pull effect"of pyridiniums. This affects directly the catalytic activity of FePcs. The plot of activity as (log I)(E) versus the calculated Fe-O-2 binding energies gives an activity volcano correlation, indicating that an optimum binding energy of O-2 with the Fe center provides the highest activity. | es_CL |
| dc.description.sponsorship | PAI-CONICYT [79150041]; CONICYTComision Nacional de Investigacion Cientifica y Tecnologica (CONICYT); FondecytComision Nacional de Investigacion Cientifica y Tecnologica (CONICYT)CONICYT FONDECYT [1140192, 1181037, 1171408]; Dicyt-USACH [021842ZM]; Fondecyt IniciacionComision Nacional de Investigacion Cientifica y Tecnologica (CONICYT)CONICYT FONDECYT [11170879]; supercomputing infrastructure of the NLHPC [ECM-02]; Millennium Project [RC120001]; Dicyt-USACH | es_CL |
| dc.description.sponsorship | A.P and I.P thank PAI-CONICYT 79150041 and Fondecyt Regular 1171408. R.O. thanks CONICYT doctoral fellowships, and J.F.S. thanks Fondecyt 1140192. C.G.-C. thanks Dicyt-USACH for a postdoctoral grant 021842ZM. G.A. thanks Fondecyt Iniciacion 11170879. Powered@NLHPC: This research was partially supported by the supercomputing infrastructure of the NLHPC (ECM-02). J.H.Z. thanks the Millennium Project RC120001, Fondecyt 1181037, and Dicyt-USACH for financial support. The authors are thankful to LNLS (Brazil) for the use of beamline (SXS-18986). | es_CL |
| dc.language.iso | en | es_CL |
| dc.publisher | AMER CHEMICAL SOC | es_CL |
| dc.rights | Attribution-NonCommercial-NoDerivs 3.0 Chile | |
| dc.source | ACS Catal., SEP 2018. 8(9): p. 8406-8419 | |
| dc.subject | Chemistry, Physical | es_CL |
| dc.title | Building Pyridinium Molecular Wires as Axial Ligands for Tuning the Electrocatalytic Activity of Iron Phthalocyanines for the Oxygen Reduction Reaction | es_CL |
| dc.type | Artículo | es_CL |
| umayor.facultad | CIENCIAS | es_CL |
| umayor.politicas.sherpa/romeo | RoMEO white journal (El archivo no está formalmente admitido). Disponible en: http://sherpa.ac.uk/romeo/index.php | es_CL |
| umayor.indexado | WOS:000444364800070 | es_CL |
| umayor.indexado | SIN PMID | es_CL |
| dc.identifier.doi | DOI: 10.1021/acscatal.8b01479 | es_CL] |
| umayor.indicadores.wos-(cuartil) | Q1 | es_CL |
| umayor.indicadores.scopus-(scimago-sjr) | SCIMAGO/ INDICE H: 139 H | es_CL |