Formic acid oxidation on Pt-Au nanoparticles: Relation between the catalyst activity and the poisoning rate
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2012
Authors
Obradović, MajaRogan, Jelena
Babić, Biljana M.
Tripković, Amalija
Gautam, A. R. S.
Radmilović, Velimir R.
Gojković, Snežana Lj.
Article (Published version)
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Pt-Au nanoparticles supported on high area carbon were prepared by simultaneous reduction of Au and Pt precursors and by reduction of Pt precursor on already prepared Au nanoparticles. The first method produced a solid solution of Pt in Au containing similar to 5% Pt with the remaining Pt on the nanoparticles' surface. For the Pt:Au precursor ratio of 1:4 and 1:9, the surface ratio was found to be 0.70:0.30 and 0.55:0.45, respectively. By the second method with the Pt:Au precursors ratio of 1:12, the surface ratio was 0.30:0.70. The voltammetric peaks of Pt-oxide reduction and CO(ads) oxidation demonstrated electronic modification of Pt by Au in all catalysts. With decreasing Pt:Au surface ratio the activity for HCOOH oxidation increases and surface coverage by CO(ads) decreases. The highest activity under potentiodynamic and quasi steady-state conditions without poisoning by CO(ads) was observed for the catalyst with the lowest Pt:Au surface ratio. Chronoamperometic test showed that i...ts high catalytic activity is associated with a high deactivation rate. It was postulated that too strong adsorption of a reactive or non-reactive intermediate caused by electron modification of Pt by underlying Au, is responsible for the deactivation. This result stresses that high Pt dispersion, necessary for promotion of the dehydrogenation path in HCOOH oxidation, can produce too strong adsorption of intermediates causing deactivation of the catalyst.
Keywords:
Formic acid electrooxidation / Platinum / Gold / Nanoparticles / Fuel cellSource:
Journal of Power Sources, 2012, 197, 72-79Publisher:
- Elsevier Science Bv, Amsterdam
Funding / projects:
- Development, characterization and application nanostructured and composite electrocatalysts and interactive supports for fuel cells and water electrolysis (RS-172054)
- Reinforcing of Nanotechnology and Functional Materials Centre (EU-245916)
- Reinforcing of Nanotechnology and Functional Materials Centre (EU-245916)
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of EnergyUnited States Department of Energy (DOE) [DE-AC02-05CH11231]
DOI: 10.1016/j.jpowsour.2011.09.043
ISSN: 0378-7753
WoS: 000297394700010
Scopus: 2-s2.0-80054825661
Institution/Community
Tehnološko-metalurški fakultetTY - JOUR AU - Obradović, Maja AU - Rogan, Jelena AU - Babić, Biljana M. AU - Tripković, Amalija AU - Gautam, A. R. S. AU - Radmilović, Velimir R. AU - Gojković, Snežana Lj. PY - 2012 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/2242 AB - Pt-Au nanoparticles supported on high area carbon were prepared by simultaneous reduction of Au and Pt precursors and by reduction of Pt precursor on already prepared Au nanoparticles. The first method produced a solid solution of Pt in Au containing similar to 5% Pt with the remaining Pt on the nanoparticles' surface. For the Pt:Au precursor ratio of 1:4 and 1:9, the surface ratio was found to be 0.70:0.30 and 0.55:0.45, respectively. By the second method with the Pt:Au precursors ratio of 1:12, the surface ratio was 0.30:0.70. The voltammetric peaks of Pt-oxide reduction and CO(ads) oxidation demonstrated electronic modification of Pt by Au in all catalysts. With decreasing Pt:Au surface ratio the activity for HCOOH oxidation increases and surface coverage by CO(ads) decreases. The highest activity under potentiodynamic and quasi steady-state conditions without poisoning by CO(ads) was observed for the catalyst with the lowest Pt:Au surface ratio. Chronoamperometic test showed that its high catalytic activity is associated with a high deactivation rate. It was postulated that too strong adsorption of a reactive or non-reactive intermediate caused by electron modification of Pt by underlying Au, is responsible for the deactivation. This result stresses that high Pt dispersion, necessary for promotion of the dehydrogenation path in HCOOH oxidation, can produce too strong adsorption of intermediates causing deactivation of the catalyst. PB - Elsevier Science Bv, Amsterdam T2 - Journal of Power Sources T1 - Formic acid oxidation on Pt-Au nanoparticles: Relation between the catalyst activity and the poisoning rate EP - 79 SP - 72 VL - 197 DO - 10.1016/j.jpowsour.2011.09.043 ER -
@article{ author = "Obradović, Maja and Rogan, Jelena and Babić, Biljana M. and Tripković, Amalija and Gautam, A. R. S. and Radmilović, Velimir R. and Gojković, Snežana Lj.", year = "2012", abstract = "Pt-Au nanoparticles supported on high area carbon were prepared by simultaneous reduction of Au and Pt precursors and by reduction of Pt precursor on already prepared Au nanoparticles. The first method produced a solid solution of Pt in Au containing similar to 5% Pt with the remaining Pt on the nanoparticles' surface. For the Pt:Au precursor ratio of 1:4 and 1:9, the surface ratio was found to be 0.70:0.30 and 0.55:0.45, respectively. By the second method with the Pt:Au precursors ratio of 1:12, the surface ratio was 0.30:0.70. The voltammetric peaks of Pt-oxide reduction and CO(ads) oxidation demonstrated electronic modification of Pt by Au in all catalysts. With decreasing Pt:Au surface ratio the activity for HCOOH oxidation increases and surface coverage by CO(ads) decreases. The highest activity under potentiodynamic and quasi steady-state conditions without poisoning by CO(ads) was observed for the catalyst with the lowest Pt:Au surface ratio. Chronoamperometic test showed that its high catalytic activity is associated with a high deactivation rate. It was postulated that too strong adsorption of a reactive or non-reactive intermediate caused by electron modification of Pt by underlying Au, is responsible for the deactivation. This result stresses that high Pt dispersion, necessary for promotion of the dehydrogenation path in HCOOH oxidation, can produce too strong adsorption of intermediates causing deactivation of the catalyst.", publisher = "Elsevier Science Bv, Amsterdam", journal = "Journal of Power Sources", title = "Formic acid oxidation on Pt-Au nanoparticles: Relation between the catalyst activity and the poisoning rate", pages = "79-72", volume = "197", doi = "10.1016/j.jpowsour.2011.09.043" }
Obradović, M., Rogan, J., Babić, B. M., Tripković, A., Gautam, A. R. S., Radmilović, V. R.,& Gojković, S. Lj.. (2012). Formic acid oxidation on Pt-Au nanoparticles: Relation between the catalyst activity and the poisoning rate. in Journal of Power Sources Elsevier Science Bv, Amsterdam., 197, 72-79. https://doi.org/10.1016/j.jpowsour.2011.09.043
Obradović M, Rogan J, Babić BM, Tripković A, Gautam ARS, Radmilović VR, Gojković SL. Formic acid oxidation on Pt-Au nanoparticles: Relation between the catalyst activity and the poisoning rate. in Journal of Power Sources. 2012;197:72-79. doi:10.1016/j.jpowsour.2011.09.043 .
Obradović, Maja, Rogan, Jelena, Babić, Biljana M., Tripković, Amalija, Gautam, A. R. S., Radmilović, Velimir R., Gojković, Snežana Lj., "Formic acid oxidation on Pt-Au nanoparticles: Relation between the catalyst activity and the poisoning rate" in Journal of Power Sources, 197 (2012):72-79, https://doi.org/10.1016/j.jpowsour.2011.09.043 . .