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Specificity of the UPD of H to the structure of highly dispersed Pt on carbon support

Authorized Users Only
2007
Authors
Elezović, Nevenka
Babić, Biljana M.
Krstajić, Nedeljko
Gajić Krstajić, Ljiljana
Vračar, Ljiljana
Article (Published version)
Metadata
Show full item record
Abstract
Home-made carbon cryogel synthesized by sol-gel polycondensation and freeze-drying is used as support for preparation of highly dispersed Pt catalyst that is made by a modified polyol synthesis method in an ethylene glycol (EG) solution. Specific surface area of carbon support and Pt/C catalyst is determined from nitrogen adsorption isotherm. The adsorption isotherm demonstrates a significant mesoporosity of carbon support. Specific surface area of the carbon support, calculated by the BET equation, is found to be 573 m(2) g(-1). X-ray diffraction (XRD) results demonstrate a successful reduction of the Pt precursor to its metallic form, and transmission electron microscopy (TEM) images show very uniform Pt particle size distribution with mean particle size of about 2.7 +/- 0.7 nm of the catalyst. Potentiodynamic studies of the underpotential deposition of hydrogen (H-upd) on Pt/C electrode in 0.5 mol dm(-3) HClO4 aqueous solution in the temperature range from 274 to 318 K are made, and... thermodynamic state functions for the hydrogen adsorption are determined. The experimental results are analyzed assuming linear variation of the Gibbs energy of adsorption versus theta H-upd on the basis of the surface heterogeneity. The increase of Delta G(Hupd)(theta) with the surface coverage indicates the repulsive interactions between H-upd adatoms. From the temperature dependence of the Gibbs energy of adsorption, the enthalpy and the entropy of adsorption are calculated. The values of these functions are determined to be Delta H-Hupd(theta=0) = -5.6 kJ mol(-1) and Delta S-Hupd(theta=0) = 69.1 J mol(-1) K-1 The value of Delta H-Hupd(theta) allows determinations of the bond energy between electrode surface and H-upd that is found to be Ept-H = 223 kJ mol(-1) for theta = 0.

Keywords:
thermodynamic state functions / temperature effect / Pt/C catalyst / hydrogen adsorption / carbon cryogel / bond energy
Source:
International Journal of Hydrogen Energy, 2007, 32, 12, 1991-1998
Publisher:
  • Pergamon-Elsevier Science Ltd, Oxford
Funding / projects:
  • Sinteza, karakterizacija i primena nanostruktuiranih katalizatora na različitim nosačima u gorivnim spregovima, elektrolizi vode i elektroorganskoj sintezi (RS-142038)

DOI: 10.1016/j.ijhydene.2006.09.042

ISSN: 0360-3199

WoS: 000249739100051

Scopus: 2-s2.0-34547884723
[ Google Scholar ]
15
15
Handle
https://hdl.handle.net/21.15107/rcub_dais_12884
URI
http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5497
Collections
  • Radovi istraživača / Researchers’ publications (TMF)
Institution/Community
Tehnološko-metalurški fakultet
TY  - JOUR
AU  - Elezović, Nevenka
AU  - Babić, Biljana M.
AU  - Krstajić, Nedeljko
AU  - Gajić Krstajić, Ljiljana
AU  - Vračar, Ljiljana
PY  - 2007
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5497
AB  - Home-made carbon cryogel synthesized by sol-gel polycondensation and freeze-drying is used as support for preparation of highly dispersed Pt catalyst that is made by a modified polyol synthesis method in an ethylene glycol (EG) solution. Specific surface area of carbon support and Pt/C catalyst is determined from nitrogen adsorption isotherm. The adsorption isotherm demonstrates a significant mesoporosity of carbon support. Specific surface area of the carbon support, calculated by the BET equation, is found to be 573 m(2) g(-1). X-ray diffraction (XRD) results demonstrate a successful reduction of the Pt precursor to its metallic form, and transmission electron microscopy (TEM) images show very uniform Pt particle size distribution with mean particle size of about 2.7 +/- 0.7 nm of the catalyst. Potentiodynamic studies of the underpotential deposition of hydrogen (H-upd) on Pt/C electrode in 0.5 mol dm(-3) HClO4 aqueous solution in the temperature range from 274 to 318 K are made, and thermodynamic state functions for the hydrogen adsorption are determined. The experimental results are analyzed assuming linear variation of the Gibbs energy of adsorption versus theta H-upd on the basis of the surface heterogeneity. The increase of Delta G(Hupd)(theta) with the surface coverage indicates the repulsive interactions between H-upd adatoms. From the temperature dependence of the Gibbs energy of adsorption, the enthalpy and the entropy of adsorption are calculated. The values of these functions are determined to be Delta H-Hupd(theta=0) = -5.6 kJ mol(-1) and Delta S-Hupd(theta=0) = 69.1 J mol(-1) K-1 The value of Delta H-Hupd(theta) allows determinations of the bond energy between electrode surface and H-upd that is found to be Ept-H = 223 kJ mol(-1) for theta = 0.
PB  - Pergamon-Elsevier Science Ltd, Oxford
T2  - International Journal of Hydrogen Energy
T1  - Specificity of the UPD of H to the structure of highly dispersed Pt on carbon support
EP  - 1998
IS  - 12
SP  - 1991
VL  - 32
DO  - 10.1016/j.ijhydene.2006.09.042
UR  - https://hdl.handle.net/21.15107/rcub_dais_12884
ER  - 
@article{
author = "Elezović, Nevenka and Babić, Biljana M. and Krstajić, Nedeljko and Gajić Krstajić, Ljiljana and Vračar, Ljiljana",
year = "2007",
abstract = "Home-made carbon cryogel synthesized by sol-gel polycondensation and freeze-drying is used as support for preparation of highly dispersed Pt catalyst that is made by a modified polyol synthesis method in an ethylene glycol (EG) solution. Specific surface area of carbon support and Pt/C catalyst is determined from nitrogen adsorption isotherm. The adsorption isotherm demonstrates a significant mesoporosity of carbon support. Specific surface area of the carbon support, calculated by the BET equation, is found to be 573 m(2) g(-1). X-ray diffraction (XRD) results demonstrate a successful reduction of the Pt precursor to its metallic form, and transmission electron microscopy (TEM) images show very uniform Pt particle size distribution with mean particle size of about 2.7 +/- 0.7 nm of the catalyst. Potentiodynamic studies of the underpotential deposition of hydrogen (H-upd) on Pt/C electrode in 0.5 mol dm(-3) HClO4 aqueous solution in the temperature range from 274 to 318 K are made, and thermodynamic state functions for the hydrogen adsorption are determined. The experimental results are analyzed assuming linear variation of the Gibbs energy of adsorption versus theta H-upd on the basis of the surface heterogeneity. The increase of Delta G(Hupd)(theta) with the surface coverage indicates the repulsive interactions between H-upd adatoms. From the temperature dependence of the Gibbs energy of adsorption, the enthalpy and the entropy of adsorption are calculated. The values of these functions are determined to be Delta H-Hupd(theta=0) = -5.6 kJ mol(-1) and Delta S-Hupd(theta=0) = 69.1 J mol(-1) K-1 The value of Delta H-Hupd(theta) allows determinations of the bond energy between electrode surface and H-upd that is found to be Ept-H = 223 kJ mol(-1) for theta = 0.",
publisher = "Pergamon-Elsevier Science Ltd, Oxford",
journal = "International Journal of Hydrogen Energy",
title = "Specificity of the UPD of H to the structure of highly dispersed Pt on carbon support",
pages = "1998-1991",
number = "12",
volume = "32",
doi = "10.1016/j.ijhydene.2006.09.042",
url = "https://hdl.handle.net/21.15107/rcub_dais_12884"
}
Elezović, N., Babić, B. M., Krstajić, N., Gajić Krstajić, L.,& Vračar, L.. (2007). Specificity of the UPD of H to the structure of highly dispersed Pt on carbon support. in International Journal of Hydrogen Energy
Pergamon-Elsevier Science Ltd, Oxford., 32(12), 1991-1998.
https://doi.org/10.1016/j.ijhydene.2006.09.042
https://hdl.handle.net/21.15107/rcub_dais_12884
Elezović N, Babić BM, Krstajić N, Gajić Krstajić L, Vračar L. Specificity of the UPD of H to the structure of highly dispersed Pt on carbon support. in International Journal of Hydrogen Energy. 2007;32(12):1991-1998.
doi:10.1016/j.ijhydene.2006.09.042
https://hdl.handle.net/21.15107/rcub_dais_12884 .
Elezović, Nevenka, Babić, Biljana M., Krstajić, Nedeljko, Gajić Krstajić, Ljiljana, Vračar, Ljiljana, "Specificity of the UPD of H to the structure of highly dispersed Pt on carbon support" in International Journal of Hydrogen Energy, 32, no. 12 (2007):1991-1998,
https://doi.org/10.1016/j.ijhydene.2006.09.042 .,
https://hdl.handle.net/21.15107/rcub_dais_12884 .

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