TY - JOUR
T1 - Evaluation of Pt alloys as electrocatalysts for oxalic acid oxidation
T2 - A combined experimental and computational study
AU - Perry, Albert
AU - Babanova, Sofia
AU - Matanovic, Ivana
AU - Neumman, Anica
AU - Serov, Alexey
AU - Artyushkova, Kateryna
AU - Atanassov, Plamen
N1 - Publisher Copyright:
© The Author(s) 2016. Published by ECS. All rights reserved.
PY - 2016
Y1 - 2016
N2 - In this study we combined experimental approaches and density functional theory to evaluate novel platinum-based materials as electrocatalysts for oxalic acid oxidation. Several Pt alloys, PtSn (1:1), PtSn (19:1), PtRu (1:4), PtRuSn (5:4:1), and PtRhSn (3:1:4), were synthetized using sacrificial support method and tested for oxidation of oxalic acid at pH 4. It was shown that PtSn (1:1) and PtRu (1:4) have higher mass activity relative to Pt. These two materials along with Pt and one of the least active alloys, PtSn (19:1), were further analyzed for the oxidation of oxalic acid at different pHs. The results show that all samples tested followed an identical trend of decreased onset potential with increased pH and increased catalytic activity with decreased pH. Density functional theory was further utilized to gain a fundamental knowledge about the mechanism of oxalic acid oxidation on Pt, PtSn (1:1), and PtRu (1:4). The results of the calculations along with the experimentally observed dependence of generated currents on the oxalic acid concentration indicate that the mechanism of oxalic acid oxidation on Pt proceeds without the participation of surface oxidizing species, while on Pt alloys it involves their participation.
AB - In this study we combined experimental approaches and density functional theory to evaluate novel platinum-based materials as electrocatalysts for oxalic acid oxidation. Several Pt alloys, PtSn (1:1), PtSn (19:1), PtRu (1:4), PtRuSn (5:4:1), and PtRhSn (3:1:4), were synthetized using sacrificial support method and tested for oxidation of oxalic acid at pH 4. It was shown that PtSn (1:1) and PtRu (1:4) have higher mass activity relative to Pt. These two materials along with Pt and one of the least active alloys, PtSn (19:1), were further analyzed for the oxidation of oxalic acid at different pHs. The results show that all samples tested followed an identical trend of decreased onset potential with increased pH and increased catalytic activity with decreased pH. Density functional theory was further utilized to gain a fundamental knowledge about the mechanism of oxalic acid oxidation on Pt, PtSn (1:1), and PtRu (1:4). The results of the calculations along with the experimentally observed dependence of generated currents on the oxalic acid concentration indicate that the mechanism of oxalic acid oxidation on Pt proceeds without the participation of surface oxidizing species, while on Pt alloys it involves their participation.
UR - http://www.scopus.com/inward/record.url?scp=84982731577&partnerID=8YFLogxK
U2 - 10.1149/2.0861609jes
DO - 10.1149/2.0861609jes
M3 - Article
AN - SCOPUS:84982731577
SN - 0013-4651
VL - 163
SP - H787-H795
JO - Journal of the Electrochemical Society
JF - Journal of the Electrochemical Society
IS - 9
ER -