Publication
Competitive paths for methanol decomposition on ruthenium: a DFT study
| dc.contributor.author | Pessoa, Ana S. Moura | |
| dc.contributor.author | Fajín, Jose L. C. | |
| dc.contributor.author | Pinto, Ana S. S. | |
| dc.contributor.author | Mandado, Marcos | |
| dc.contributor.author | Cordeiro, M. Natália D. S. | |
| dc.date.accessioned | 2016-01-18T14:18:09Z | |
| dc.date.available | 2016-01-18T14:18:09Z | |
| dc.date.issued | 2015 | |
| dc.description.abstract | Methanol decomposition is one of the key reactions in direct methanol fuel cell (DMFC) state-of-the-art technology, research, and development. However, its mechanism still presents many uncertainties, which, if answered, would permit us to refine the manufacture of DMFCs. The mechanism of methanol decomposition on ruthenium surfaces was investigated using density functional theory and a periodic supercell approach. The possible pathways, involving either initial C−H, C−O or O−H scission, were defined from experimental evidence regarding the methanol decomposition on ruthenium and other metallic surfaces. The study yielded the O−H scission pathway as having both the most favorable energetics and kinetics. The computational data, which present a remarkable closeness with the experimental results, also indicate methanol adsorption, the starting point in all possible pathways, to be of weak nature, implying a considerable rate of methanol desorption from the ruthenium, compromising the reaction. | pt_PT |
| dc.description.sponsorship | Thanks are due to Fundação para a Ciência e Tecnologia (FCT), Lisbon, Portugal and to FEDER for financial support to LAQV@ REQUIMTE, project UID/QUI/50006/2013. J.L.C.F. acknowledges FCT for Grant SFRH/BPD/64566/2009 cofinanced by the Programa Operacional Potencial Humano (POPH)/Fundo Social Europeu (FSE) and Quadro de Referência Estratégico Nacional 2009-2013 do Governo da República Portuguesa | |
| dc.identifier.doi | 10.1021/acs.jpcc.5b06671 | pt_PT |
| dc.identifier.issn | 1932-7447 | |
| dc.identifier.uri | http://hdl.handle.net/10400.22/7409 | |
| dc.language.iso | eng | pt_PT |
| dc.peerreviewed | yes | pt_PT |
| dc.publisher | American Chemical Society | pt_PT |
| dc.relation | UID/QUI/50006/2013 | |
| dc.relation | SFRH/BPD/64566/2009 | |
| dc.relation.publisherversion | http://pubs.acs.org/doi/abs/10.1021/acs.jpcc.5b06671 | pt_PT |
| dc.title | Competitive paths for methanol decomposition on ruthenium: a DFT study | pt_PT |
| dc.type | journal article | |
| dspace.entity.type | Publication | |
| oaire.citation.endPage | 27391 | pt_PT |
| oaire.citation.issue | 49 | pt_PT |
| oaire.citation.startPage | 27382 | pt_PT |
| oaire.citation.title | Journal of Physical Chemistry C | pt_PT |
| oaire.citation.volume | 119 | pt_PT |
| rcaap.rights | closedAccess | pt_PT |
| rcaap.type | article | pt_PT |