TY - JOUR
T1 - Toward understanding CO oxidation on high-entropy alloy electrocatalysts
AU - Salinas-Quezada, María Paula
AU - Pedersen, Jack K.
AU - Sebastián-Pascual, Paula
AU - Chorkendorff, Ib
AU - Biswas, Krishanu
AU - Rossmeisl, Jan
AU - Escudero-Escribano, María
N1 - Publisher Copyright:
© 2024 RSC.
PY - 2024
Y1 - 2024
N2 - Understanding the catalytic activity of high-entropy alloys (HEAs) toward the conversion of small molecules such as carbon monoxide (CO) can provide insight into their structure-property relations. The identification of specific descriptors that govern the CO oxidation on HEAs is crucial to design new materials with customized compositions and structures. Herein, we have rationally assessed the CO oxidation mechanism on an extended AgAuCuPdPt HEA electrocatalyst under an acidic electrolyte. We compare the HEA performance with respect to platinum (Pt), palladium (Pd), and gold (Au) monometallic surfaces for CO oxidation. We also evaluated the same reaction on a binary AuPd alloy and a quaternary AuCuPdPt polycrystalline alloy with the aim of understanding the surface composition effects of the HEA. To provide insights into the descriptors controlling the CO oxidation mechanism and overpotential of the different alloy chemistry, we have combined cyclic voltammetry, surface-sensitive characterisation techniques and density functional theory (DFT) simulations. We show that silver (Ag) can improve the catalytic oxidation of CO by perturbing the *OH adsorption energy of Pd, leading to a lower onset potential. Additionally, we observed that Au segregates on the surface and that Cu is not stable at high applied potentials after CO oxidation. We highlight that HEA electrocatalysts are a valuable platform for designing more active and selective electrocatalyst surfaces.
AB - Understanding the catalytic activity of high-entropy alloys (HEAs) toward the conversion of small molecules such as carbon monoxide (CO) can provide insight into their structure-property relations. The identification of specific descriptors that govern the CO oxidation on HEAs is crucial to design new materials with customized compositions and structures. Herein, we have rationally assessed the CO oxidation mechanism on an extended AgAuCuPdPt HEA electrocatalyst under an acidic electrolyte. We compare the HEA performance with respect to platinum (Pt), palladium (Pd), and gold (Au) monometallic surfaces for CO oxidation. We also evaluated the same reaction on a binary AuPd alloy and a quaternary AuCuPdPt polycrystalline alloy with the aim of understanding the surface composition effects of the HEA. To provide insights into the descriptors controlling the CO oxidation mechanism and overpotential of the different alloy chemistry, we have combined cyclic voltammetry, surface-sensitive characterisation techniques and density functional theory (DFT) simulations. We show that silver (Ag) can improve the catalytic oxidation of CO by perturbing the *OH adsorption energy of Pd, leading to a lower onset potential. Additionally, we observed that Au segregates on the surface and that Cu is not stable at high applied potentials after CO oxidation. We highlight that HEA electrocatalysts are a valuable platform for designing more active and selective electrocatalyst surfaces.
U2 - 10.1039/d4ey00023d
DO - 10.1039/d4ey00023d
M3 - Journal article
AN - SCOPUS:85192987386
SN - 2753-801x
VL - 2
SP - 941
EP - 952
JO - Ees Catalysis
JF - Ees Catalysis
ER -