Evaluation of Pt Alloys as Electrocatalysts for Oxalic Acid Oxidation: A Combined Experimental and Computational Study
- Univ. of New Mexico, Albuquerque, NM (United States). Center for Micro-Engineered Materials (CMEM), Dept. of Chemical and Biological Engineering
- Univ. of New Mexico, Albuquerque, NM (United States). Center for Micro-Engineered Materials (CMEM), Dept. of Chemical and Biological Engineering; Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division
- Oregon State Univ., Corvallis, OR (United States). School of Chemical, Biological and Environmental Engineering
Here 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). In conclusion, 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.
- Research Organization:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Organization:
- Department of Defence (DOD); USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- AC52-06NA25396; W911NF-14-1-0263; AC02- 05CH11231
- OSTI ID:
- 1338746
- Report Number(s):
- LA-UR-16-20329
- Journal Information:
- Journal of the Electrochemical Society, Vol. 163, Issue 9; ISSN 0013-4651
- Publisher:
- The Electrochemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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