United States Department of Energy, Office of Science, Office of Basic Energy Sciences, Grant DE-AC02-05CH11231

Link to this page

United States Department of Energy, Office of Science, Office of Basic Energy Sciences, Grant DE-AC02-05CH11231

Authors

Publications

Pt nanoparticles on tin oxide based support as a beneficial catalyst for oxygen reduction in alkaline solutions

Elezović, Nevenka; Radmilović, Velimir R.; Kovač, Janez; Babić, Biljana M.; Gajić Krstajić, Ljiljana; Krstajić, Nedeljko

(Royal Society of Chemistry, 2015)

TY  - JOUR
AU  - Elezović, Nevenka
AU  - Radmilović, Velimir R.
AU  - Kovač, Janez
AU  - Babić, Biljana M.
AU  - Gajić Krstajić, Ljiljana
AU  - Krstajić, Nedeljko
PY  - 2015
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5795
AB  - A platinum nanocatalyst on Sb doped tin oxide support (Sb-SnO2) was synthesized and characterized as a catalyst for oxygen reduction reaction in 0.1 mol dm(-3) NaOH solution at 25 degrees C. Sb (5%) doped tin oxide support was synthesized by a modified hydrazine reduction procedure. The platinum nanocatalyst (20% Pt) on Sb-SnO2 support was synthesized by a borohydride reduction method. The synthesized support and catalyst were characterized by high resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS) and X-ray diffraction technique (XRD). X-ray photoelectron spectroscopy was applied to characterize the chemical status of elements before and after Pt-treatment. XPS spectra of Sn 3d, Pt 4f, Sb 3d and O 1s revealed that the Pt-deposition on Sb-SnO2 support induced the reduction of the Sn(4+) oxidation state to Sn(2+) and Sn(0) states, while Pt remained in the metallic state and Sb was in the (3+) oxidation state. Homogenous Pt nanoparticle distribution over the support, without pronounced particle agglomeration, was confirmed by HRTEM technique. The average Pt particle size was 2.9 nm. The electrochemically active Pt surface area of the catalyst was determined by the integration of the cyclic voltammetry curve in the potential region of underpotential deposition of hydrogen, after double layer charge correction, taking into account the reference value of 210 mu C cm(-2) for full monolayer coverage. This calculation gave the value of 51 m(2) g(-1). The kinetics of the oxygen reduction reaction with Pt/[Sb-SnO2 catalyst was studied by cyclic voltammetry and linear sweep voltammetry using a rotating gold disc electrode. Two different Tafel slopes were observed: one close to 60 mV dec(-1) in the low current density region, and another at similar to 120 mV dec(-1) in the higher current densities region, as was already referred in previous reports for the oxygen reduction reaction with polycrystalline Pt, as well as with different Pt based nanocatalysts. The specific activities for oxygen reduction, expressed in terms of kinetic current densities per electrochemically Pt active surface area, as well as per mass of Pt loaded, at the constant potential of practical interest (0.85 V and 0.90 V vs. RHE), were compared to a carbon supported (Vulcan XC-72) catalyst. The Pt/[Sb-SnO2 catalyst exhibited similar catalytic activity for oxygen reduction reaction like carbon supported one. The advantages of the carbon free support application in terms of the durability and stability of the catalysts were proved by accelerated stability tests.
PB  - Royal Society of Chemistry
T2  - RSC Advances
T1  - Pt nanoparticles on tin oxide based support as a beneficial catalyst for oxygen reduction in alkaline solutions
EP  - 15929
IS  - 21
SP  - 15923
VL  - 5
DO  - 10.1039/c4ra13391a
UR  - https://hdl.handle.net/21.15107/rcub_dais_3354
ER  - 
@article{
author = "Elezović, Nevenka and Radmilović, Velimir R. and Kovač, Janez and Babić, Biljana M. and Gajić Krstajić, Ljiljana and Krstajić, Nedeljko",
year = "2015",
abstract = "A platinum nanocatalyst on Sb doped tin oxide support (Sb-SnO2) was synthesized and characterized as a catalyst for oxygen reduction reaction in 0.1 mol dm(-3) NaOH solution at 25 degrees C. Sb (5%) doped tin oxide support was synthesized by a modified hydrazine reduction procedure. The platinum nanocatalyst (20% Pt) on Sb-SnO2 support was synthesized by a borohydride reduction method. The synthesized support and catalyst were characterized by high resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS) and X-ray diffraction technique (XRD). X-ray photoelectron spectroscopy was applied to characterize the chemical status of elements before and after Pt-treatment. XPS spectra of Sn 3d, Pt 4f, Sb 3d and O 1s revealed that the Pt-deposition on Sb-SnO2 support induced the reduction of the Sn(4+) oxidation state to Sn(2+) and Sn(0) states, while Pt remained in the metallic state and Sb was in the (3+) oxidation state. Homogenous Pt nanoparticle distribution over the support, without pronounced particle agglomeration, was confirmed by HRTEM technique. The average Pt particle size was 2.9 nm. The electrochemically active Pt surface area of the catalyst was determined by the integration of the cyclic voltammetry curve in the potential region of underpotential deposition of hydrogen, after double layer charge correction, taking into account the reference value of 210 mu C cm(-2) for full monolayer coverage. This calculation gave the value of 51 m(2) g(-1). The kinetics of the oxygen reduction reaction with Pt/[Sb-SnO2 catalyst was studied by cyclic voltammetry and linear sweep voltammetry using a rotating gold disc electrode. Two different Tafel slopes were observed: one close to 60 mV dec(-1) in the low current density region, and another at similar to 120 mV dec(-1) in the higher current densities region, as was already referred in previous reports for the oxygen reduction reaction with polycrystalline Pt, as well as with different Pt based nanocatalysts. The specific activities for oxygen reduction, expressed in terms of kinetic current densities per electrochemically Pt active surface area, as well as per mass of Pt loaded, at the constant potential of practical interest (0.85 V and 0.90 V vs. RHE), were compared to a carbon supported (Vulcan XC-72) catalyst. The Pt/[Sb-SnO2 catalyst exhibited similar catalytic activity for oxygen reduction reaction like carbon supported one. The advantages of the carbon free support application in terms of the durability and stability of the catalysts were proved by accelerated stability tests.",
publisher = "Royal Society of Chemistry",
journal = "RSC Advances",
title = "Pt nanoparticles on tin oxide based support as a beneficial catalyst for oxygen reduction in alkaline solutions",
pages = "15929-15923",
number = "21",
volume = "5",
doi = "10.1039/c4ra13391a",
url = "https://hdl.handle.net/21.15107/rcub_dais_3354"
}
Elezović, N., Radmilović, V. R., Kovač, J., Babić, B. M., Gajić Krstajić, L.,& Krstajić, N.. (2015). Pt nanoparticles on tin oxide based support as a beneficial catalyst for oxygen reduction in alkaline solutions. in RSC Advances
Royal Society of Chemistry., 5(21), 15923-15929.
https://doi.org/10.1039/c4ra13391a
https://hdl.handle.net/21.15107/rcub_dais_3354
Elezović N, Radmilović VR, Kovač J, Babić BM, Gajić Krstajić L, Krstajić N. Pt nanoparticles on tin oxide based support as a beneficial catalyst for oxygen reduction in alkaline solutions. in RSC Advances. 2015;5(21):15923-15929.
doi:10.1039/c4ra13391a
https://hdl.handle.net/21.15107/rcub_dais_3354 .
Elezović, Nevenka, Radmilović, Velimir R., Kovač, Janez, Babić, Biljana M., Gajić Krstajić, Ljiljana, Krstajić, Nedeljko, "Pt nanoparticles on tin oxide based support as a beneficial catalyst for oxygen reduction in alkaline solutions" in RSC Advances, 5, no. 21 (2015):15923-15929,
https://doi.org/10.1039/c4ra13391a .,
https://hdl.handle.net/21.15107/rcub_dais_3354 .
1
23
21
23

Synthesis, characterization and electrocatalytical behavior of Nb-TiO2/Pt nanocatalyst for oxygen reduction reaction

Elezović, Nevenka R.; Babić, Biljana M.; Gajić Krstajić, Ljiljana; Radmilović, Velimir R.; Krstajić, Nedeljko; Vračar, Ljiljana

(Elsevier, 2010)

TY  - JOUR
AU  - Elezović, Nevenka R.
AU  - Babić, Biljana M.
AU  - Gajić Krstajić, Ljiljana
AU  - Radmilović, Velimir R.
AU  - Krstajić, Nedeljko
AU  - Vračar, Ljiljana
PY  - 2010
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5617
AB  - In order to point out the effect of the support to the catalyst for oxygen reduction reaction nano-crystalline Nb-doped TiO2 was synthesized through a modified sol-gel route procedure. The specific surface area of the support, SBET, and pore size distribution, were calculated from the adsorption isotherms using the gravimetric McBain method. The support was characterized by X-ray diffraction (XRD) technique. The borohydride reduction method was used to prepare Nb-TiO2 supported Pt (20 wt.%) catalyst. The synthesized catalyst was analyzed by TEM technique. Finally, the catalytic activity of this new catalyst for oxygen reduction reaction was investigated in acid solution, in the absence and the presence of methanol, and its activity was compared towards the results on C/Pt catalysts. Kinetic analysis reveals that the oxygen reduction reaction on Nb-TiO2/Pt catalyst follows four-electron process leading to water, as in the case of C/Pt electrode, but the Tafel plots normalized to the electrochemically active surface area show very remarkable enhancement in activity of Nb-TiO2/Pt expressed through the value of the current density at the constant potential. Moreover, Nb-TiO2/Pt catalyst exhibits higher methanol tolerance during the oxygen reduction reaction than the C/Pt catalyst. The enhancement in the activity of Nb-TiO2/Pt is consequence of both: the interactions of Pt nanoparticles with the support and the energy shift of the surface d-states with respect to the Fermi level what changes the surface reactivity. © 2010 Elsevier B.V.
PB  - Elsevier
T2  - Journal of Power Sources
T1  - Synthesis, characterization and electrocatalytical behavior of Nb-TiO2/Pt nanocatalyst for oxygen reduction reaction
EP  - 3968
IS  - 13
SP  - 3961
VL  - 195
DO  - 10.1016/j.jpowsour.2010.01.035
UR  - https://hdl.handle.net/21.15107/rcub_dais_3418
ER  - 
@article{
author = "Elezović, Nevenka R. and Babić, Biljana M. and Gajić Krstajić, Ljiljana and Radmilović, Velimir R. and Krstajić, Nedeljko and Vračar, Ljiljana",
year = "2010",
abstract = "In order to point out the effect of the support to the catalyst for oxygen reduction reaction nano-crystalline Nb-doped TiO2 was synthesized through a modified sol-gel route procedure. The specific surface area of the support, SBET, and pore size distribution, were calculated from the adsorption isotherms using the gravimetric McBain method. The support was characterized by X-ray diffraction (XRD) technique. The borohydride reduction method was used to prepare Nb-TiO2 supported Pt (20 wt.%) catalyst. The synthesized catalyst was analyzed by TEM technique. Finally, the catalytic activity of this new catalyst for oxygen reduction reaction was investigated in acid solution, in the absence and the presence of methanol, and its activity was compared towards the results on C/Pt catalysts. Kinetic analysis reveals that the oxygen reduction reaction on Nb-TiO2/Pt catalyst follows four-electron process leading to water, as in the case of C/Pt electrode, but the Tafel plots normalized to the electrochemically active surface area show very remarkable enhancement in activity of Nb-TiO2/Pt expressed through the value of the current density at the constant potential. Moreover, Nb-TiO2/Pt catalyst exhibits higher methanol tolerance during the oxygen reduction reaction than the C/Pt catalyst. The enhancement in the activity of Nb-TiO2/Pt is consequence of both: the interactions of Pt nanoparticles with the support and the energy shift of the surface d-states with respect to the Fermi level what changes the surface reactivity. © 2010 Elsevier B.V.",
publisher = "Elsevier",
journal = "Journal of Power Sources",
title = "Synthesis, characterization and electrocatalytical behavior of Nb-TiO2/Pt nanocatalyst for oxygen reduction reaction",
pages = "3968-3961",
number = "13",
volume = "195",
doi = "10.1016/j.jpowsour.2010.01.035",
url = "https://hdl.handle.net/21.15107/rcub_dais_3418"
}
Elezović, N. R., Babić, B. M., Gajić Krstajić, L., Radmilović, V. R., Krstajić, N.,& Vračar, L.. (2010). Synthesis, characterization and electrocatalytical behavior of Nb-TiO2/Pt nanocatalyst for oxygen reduction reaction. in Journal of Power Sources
Elsevier., 195(13), 3961-3968.
https://doi.org/10.1016/j.jpowsour.2010.01.035
https://hdl.handle.net/21.15107/rcub_dais_3418
Elezović NR, Babić BM, Gajić Krstajić L, Radmilović VR, Krstajić N, Vračar L. Synthesis, characterization and electrocatalytical behavior of Nb-TiO2/Pt nanocatalyst for oxygen reduction reaction. in Journal of Power Sources. 2010;195(13):3961-3968.
doi:10.1016/j.jpowsour.2010.01.035
https://hdl.handle.net/21.15107/rcub_dais_3418 .
Elezović, Nevenka R., Babić, Biljana M., Gajić Krstajić, Ljiljana, Radmilović, Velimir R., Krstajić, Nedeljko, Vračar, Ljiljana, "Synthesis, characterization and electrocatalytical behavior of Nb-TiO2/Pt nanocatalyst for oxygen reduction reaction" in Journal of Power Sources, 195, no. 13 (2010):3961-3968,
https://doi.org/10.1016/j.jpowsour.2010.01.035 .,
https://hdl.handle.net/21.15107/rcub_dais_3418 .
3
79
64
76