Computational study of electrochemical CO2 reduction at transition metal electrodes

dc.contributorAalto-yliopistofi
dc.contributorAalto Universityen
dc.contributor.authorHussain, Javed
dc.contributor.authorSkúlason, Egill
dc.contributor.authorJónsson, Hannes
dc.contributor.departmentUniversity of Iceland
dc.contributor.departmentDepartment of Applied Physics
dc.date.accessioned2017-04-28T09:52:34Z
dc.date.available2017-04-28T09:52:34Z
dc.date.issued2015
dc.description.abstractA detailed understanding of the mechanism of electrochemical reduction of CO2 to form hydrocarbons can help design improved catalysts for this important reaction. Density functional theory calculations were used here to model the various elementary steps in this reaction on transition metal surfaces, in particular Cu(111) and Pt(111). The minimum energy paths for sequential protonation by either Tafel or Heyrovsky mechanism were calculated using the nudged elastic band method for applied potentials comparable to those used in experimental studies, ranging from -0.7 V to -1.7 V. A detailed mechanism for CO2 reduction on Cu(111) has been identified where the highest activation energy is 0.5 eV at -1.3 V vs. RHE. On Pt(111), a different mechanism is found to be optimal but it involves a higher barrier, 0.7 eV at -1.0 V vs. RHE. Hydrogen production is then a faster reaction with activation energy of only 0.3 eV on Pt(111) at the same potential, while on Cu(111) hydrogen production has an activation energy of 0.9 eV at -1.3 V. These results are consistent with experimental findings where copper electrodes are found to lead to relatively high yield of CH4 while H2 forms almost exclusively at platinum electrodes.en
dc.description.versionPeer revieweden
dc.format.extent7
dc.format.extent1865-1871
dc.format.mimetypeapplication/pdf
dc.identifier.citationHussain , J , Skúlason , E & Jónsson , H 2015 , ' Computational study of electrochemical CO 2 reduction at transition metal electrodes ' , PROCEDIA COMPUTER SCIENCE , vol. 51 , pp. 1865-1871 . https://doi.org/10.1016/j.procs.2015.05.419en
dc.identifier.doi10.1016/j.procs.2015.05.419
dc.identifier.issn1877-0509
dc.identifier.otherPURE UUID: 0853b11a-4530-48ba-b152-efcc2b785f8a
dc.identifier.otherPURE ITEMURL: https://research.aalto.fi/en/publications/0853b11a-4530-48ba-b152-efcc2b785f8a
dc.identifier.otherPURE LINK: http://www.scopus.com/inward/record.url?scp=84939208809&partnerID=8YFLogxK
dc.identifier.otherPURE FILEURL: https://research.aalto.fi/files/11745512/1_s2.0_S1877050915012272_main.pdf
dc.identifier.urihttps://aaltodoc.aalto.fi/handle/123456789/25295
dc.identifier.urnURN:NBN:fi:aalto-201704283698
dc.language.isoenen
dc.relation.ispartofseriesPROCEDIA COMPUTER SCIENCEen
dc.relation.ispartofseriesVolume 51en
dc.rightsopenAccessen
dc.subject.keywordDensity functional theory
dc.subject.keywordElectrocatalysis
dc.subject.keywordElectrochemical reduction of carbon dioxide
dc.subject.keywordNudged elastic band
dc.titleComputational study of electrochemical CO2 reduction at transition metal electrodesen
dc.typeA1 Alkuperäisartikkeli tieteellisessä aikakauslehdessäfi
dc.type.versionpublishedVersion
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