Please use this identifier to cite or link to this item: http://hdl.handle.net/2445/177679
Title: A Semiempirical Method to Detect and Correct DFT-Based Gas-Phase Errors and Its Application in Electrocatalysis
Author: Granda Marulanda, Laura P.
Rendón Calle, Alejandra
Builes, Santiago
Illas i Riera, Francesc
Koper, Marc T. M.
Calle Vallejo, Federico
Keywords: Electrocatàlisi
Enginyeria de gas
Electrocatalysis
Gas engineering
Issue Date: 26-May-2020
Publisher: American Chemical Society
Abstract: Computational 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.
Note: Reproducció del document publicat a: https://doi.org/10.1021/acscatal.0c01075
It is part of: ACS Catalysis, 2020, vol. 10, num. 12, p. 6900-6907
URI: http://hdl.handle.net/2445/177679
Related resource: https://doi.org/10.1021/acscatal.0c01075
ISSN: 2155-5435
Appears in Collections:Articles publicats en revistes (Institut de Química Teòrica i Computacional (IQTCUB))
Articles publicats en revistes (Ciència dels Materials i Química Física)

Files in This Item:
File Description SizeFormat 
704746.pdf1.51 MBAdobe PDFView/Open


This item is licensed under a Creative Commons License Creative Commons