Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions
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2007
Authors
Krstajić, Nedeljko V.Vračar, Ljiljana M.

Radmilović, Velimir R.

Neophytides, Stelios G.
Labou, Miranda
Jakšić, Jelena M.
Tunold, Reidar
Falaras, Polycarpos
Jakšić, Milan M.
Article (Published version)

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Magneli phases [A. Magneli, Acta Chem. Scand. 13 (1959) 5] have been introduced as a unique electron conductive and interactive support for electrocatalysis both in hydrogen (HELR) and oxygen (OELR) electrode reactions in water electrolysis and Low Temperature PEM Fuel Cells (LT PEM FC). The Strong Metal-Support Interaction (SMSI) that imposes the former implies: (i) the hypo-hyper-d-interbonding effect and its catalytic consequences, and (ii) the interactive primary oxide (M-OH) spillover from the hypo-d-oxide support as a dynamic electrocatalytic contribution. The stronger the bonding, the more strained appear d-orbitals, thereby the less strong the intermediate adsorptive strength in the rate determining step (RDS), and consequently, the faster the facilitated catalytic electrode reaction arises. At the same time the primary oxide spillover transferred from the hypo-d-oxide support directly interferes and reacts either individually and directly to contribute to finish the oxygen red...uction, or with other interactive species, like CO to contribute to the CO tolerance. In such a respect, the conditions to provide Au to act as the reversible hydrogen electrode have been proved either by its potentiodynamic surface reconstruction in a heavy water solution, or by the nanostructured SMSI Au on anatase titania with characteristic strained d-orbitals in such a hypo-hyper-d-interactive bonding (Au/TiO2). In the same context, some spontaneous tendency towards monoatomic network dispersion of Pt upon Magneli phases makes it possible to produce an advanced interactive supported electrocatalyst for cathodic oxygen reduction (ORR). The strained hypo-hyper-d-interelectronic and inter-d-orbital metal/hypo-d-oxide support bonding relative to the strength of the latter, has been inferred to be the basis of the synergistic electrocatalytic effect both in the HELR and ORR.
Keywords:
Hypo-hyper-d-d-bonding / Magneli phases / Monoatomic network / Primary oxide (M-OH) / Reversible H2/Au/TiO2 electrode / SMSI (strong metal-support interaction) / Spillover / Synergistic interactive electrocatalystsSource:
Surface Science, 2007, 601, 9, 1949-1966Publisher:
- Elsevier
Funding / projects:
- The present work has been supported by and carried out within EU Project ‘Apollon’, Contract Nr. ENK5-CT-2001-00572, EU Project NR. NNES-2001-00187, and the Project ‘Prometheas’, Contract Nr. ICA2-2001-10037. Partially (the ORR) this paper was supported by the Ministry of Science and Technologies of Republic Serbia, Belgrade
DOI: 10.1016/j.susc.2007.02.019
ISSN: 0039-6028
WoS: 000246550300008
Scopus: 2-s2.0-34247223113
Institution/Community
Tehnološko-metalurški fakultetTY - JOUR AU - Krstajić, Nedeljko V. AU - Vračar, Ljiljana M. AU - Radmilović, Velimir R. AU - Neophytides, Stelios G. AU - Labou, Miranda AU - Jakšić, Jelena M. AU - Tunold, Reidar AU - Falaras, Polycarpos AU - Jakšić, Milan M. PY - 2007 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5478 AB - Magneli phases [A. Magneli, Acta Chem. Scand. 13 (1959) 5] have been introduced as a unique electron conductive and interactive support for electrocatalysis both in hydrogen (HELR) and oxygen (OELR) electrode reactions in water electrolysis and Low Temperature PEM Fuel Cells (LT PEM FC). The Strong Metal-Support Interaction (SMSI) that imposes the former implies: (i) the hypo-hyper-d-interbonding effect and its catalytic consequences, and (ii) the interactive primary oxide (M-OH) spillover from the hypo-d-oxide support as a dynamic electrocatalytic contribution. The stronger the bonding, the more strained appear d-orbitals, thereby the less strong the intermediate adsorptive strength in the rate determining step (RDS), and consequently, the faster the facilitated catalytic electrode reaction arises. At the same time the primary oxide spillover transferred from the hypo-d-oxide support directly interferes and reacts either individually and directly to contribute to finish the oxygen reduction, or with other interactive species, like CO to contribute to the CO tolerance. In such a respect, the conditions to provide Au to act as the reversible hydrogen electrode have been proved either by its potentiodynamic surface reconstruction in a heavy water solution, or by the nanostructured SMSI Au on anatase titania with characteristic strained d-orbitals in such a hypo-hyper-d-interactive bonding (Au/TiO2). In the same context, some spontaneous tendency towards monoatomic network dispersion of Pt upon Magneli phases makes it possible to produce an advanced interactive supported electrocatalyst for cathodic oxygen reduction (ORR). The strained hypo-hyper-d-interelectronic and inter-d-orbital metal/hypo-d-oxide support bonding relative to the strength of the latter, has been inferred to be the basis of the synergistic electrocatalytic effect both in the HELR and ORR. PB - Elsevier T2 - Surface Science T1 - Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions EP - 1966 IS - 9 SP - 1949 VL - 601 DO - 10.1016/j.susc.2007.02.019 ER -
@article{ author = "Krstajić, Nedeljko V. and Vračar, Ljiljana M. and Radmilović, Velimir R. and Neophytides, Stelios G. and Labou, Miranda and Jakšić, Jelena M. and Tunold, Reidar and Falaras, Polycarpos and Jakšić, Milan M.", year = "2007", abstract = "Magneli phases [A. Magneli, Acta Chem. Scand. 13 (1959) 5] have been introduced as a unique electron conductive and interactive support for electrocatalysis both in hydrogen (HELR) and oxygen (OELR) electrode reactions in water electrolysis and Low Temperature PEM Fuel Cells (LT PEM FC). The Strong Metal-Support Interaction (SMSI) that imposes the former implies: (i) the hypo-hyper-d-interbonding effect and its catalytic consequences, and (ii) the interactive primary oxide (M-OH) spillover from the hypo-d-oxide support as a dynamic electrocatalytic contribution. The stronger the bonding, the more strained appear d-orbitals, thereby the less strong the intermediate adsorptive strength in the rate determining step (RDS), and consequently, the faster the facilitated catalytic electrode reaction arises. At the same time the primary oxide spillover transferred from the hypo-d-oxide support directly interferes and reacts either individually and directly to contribute to finish the oxygen reduction, or with other interactive species, like CO to contribute to the CO tolerance. In such a respect, the conditions to provide Au to act as the reversible hydrogen electrode have been proved either by its potentiodynamic surface reconstruction in a heavy water solution, or by the nanostructured SMSI Au on anatase titania with characteristic strained d-orbitals in such a hypo-hyper-d-interactive bonding (Au/TiO2). In the same context, some spontaneous tendency towards monoatomic network dispersion of Pt upon Magneli phases makes it possible to produce an advanced interactive supported electrocatalyst for cathodic oxygen reduction (ORR). The strained hypo-hyper-d-interelectronic and inter-d-orbital metal/hypo-d-oxide support bonding relative to the strength of the latter, has been inferred to be the basis of the synergistic electrocatalytic effect both in the HELR and ORR.", publisher = "Elsevier", journal = "Surface Science", title = "Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions", pages = "1966-1949", number = "9", volume = "601", doi = "10.1016/j.susc.2007.02.019" }
Krstajić, N. V., Vračar, L. M., Radmilović, V. R., Neophytides, S. G., Labou, M., Jakšić, J. M., Tunold, R., Falaras, P.,& Jakšić, M. M.. (2007). Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions. in Surface Science Elsevier., 601(9), 1949-1966. https://doi.org/10.1016/j.susc.2007.02.019
Krstajić NV, Vračar LM, Radmilović VR, Neophytides SG, Labou M, Jakšić JM, Tunold R, Falaras P, Jakšić MM. Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions. in Surface Science. 2007;601(9):1949-1966. doi:10.1016/j.susc.2007.02.019 .
Krstajić, Nedeljko V., Vračar, Ljiljana M., Radmilović, Velimir R., Neophytides, Stelios G., Labou, Miranda, Jakšić, Jelena M., Tunold, Reidar, Falaras, Polycarpos, Jakšić, Milan M., "Advances in interactive supported electrocatalysts for hydrogen and oxygen electrode reactions" in Surface Science, 601, no. 9 (2007):1949-1966, https://doi.org/10.1016/j.susc.2007.02.019 . .