A Semiempirical Method to Detect and Correct DFT-Based Gas-Phase Errors and Its Application in Electrocatalysis

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dc.citation.journalTitleAcs Catalysiseng
dc.contributor.authorGranda-Marulanda, Laura P.
dc.contributor.authorRendon-Calle, Alejandra
dc.contributor.authorBuiles, Santiago
dc.contributor.authorIllas, Francesc
dc.contributor.authorKoper, Marc T. M.
dc.contributor.authorCalle-Vallejo, Federico
dc.contributor.departmentUniversidad EAFIT. Departamento de Ingeniería de Procesosspa
dc.contributor.researchgroupDesarrollo y Diseño de Procesosspa
dc.date.accessioned2021-04-12T19:06:22Z
dc.date.available2021-04-12T19:06:22Z
dc.date.issued2020-06-19
dc.description.abstractComputational models of adsorption at metal surfaces are often based on DFT and make use of the generalized gradient approximation. This likely implies the presence of sizable errors in the gas-phase energetics. Here, we take a step closer toward chemical accuracy with a semiempirical method to correct the gas-phase energetics of PBE, PW91, RPBE, and BEEF-vdW exchange-correlation functionals. The proposed two-step method is tested on a data set of 27 gas-phase molecules belonging to the carbon cycle: first, the errors are pinpointed based on formation energies, and second, the respective corrections are sequentially applied to ensure the progressive lowering of the data set's mean and maximum errors. We illustrate the benefits of the method in electrocatalysis by a substantial improvement of the calculated equilibrium and onset potentials for CO2 reduction to CO on Au, Ag, and Cu electrodes. This suggests that fast and systematic gas-phase corrections can be devised to augment the predictive power of computational catalysis models.eng
dc.identifierhttps://eafit.fundanetsuite.com/Publicaciones/ProdCientif/PublicacionFrw.aspx?id=11911
dc.identifier.doi10.1021/acscatal.0c01075
dc.identifier.issn21555435
dc.identifier.otherWOS;000543663800033
dc.identifier.otherSCOPUS;2-s2.0-85087830924
dc.identifier.urihttp://hdl.handle.net/10784/28276
dc.language.isoeng
dc.publisherAMER CHEMICAL SOC
dc.relationDOI;10.1021/acscatal.0c01075
dc.relationWOS;000543663800033
dc.relationSCOPUS;2-s2.0-85087830924
dc.relation.urihttps://www.scopus.com/inward/record.uri?eid=2-s2.0-85087830924&doi=10.1021%2facscatal.0c01075&partnerID=40&md5=831870679aff8635a7fcb3f21f83832a
dc.rightsAMER CHEMICAL SOC
dc.sourceAcs Catalysis
dc.subjectgas-phase errorseng
dc.subjectgas-phase correctionseng
dc.subjectcarbon monoxideeng
dc.subjectcarbon dioxideeng
dc.subjectDFTeng
dc.subjectelectrochemical reduction of CO2eng
dc.titleA Semiempirical Method to Detect and Correct DFT-Based Gas-Phase Errors and Its Application in Electrocatalysiseng
dc.typeinfo:eu-repo/semantics/article
dc.typeinfo:eu-repo/semantics/publishedVersion
dc.typeinfo:eu-repo/semantics/articleeng
dc.typearticleeng
dc.typeinfo:eu-repo/semantics/publishedVersioneng
dc.typepublishedVersioneng
dc.type.localArtículospa

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