Interactive supported electrocatalysts and spillover effect in electrocatalysis for hydrogen and oxygen electrode reactions
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The aim of the present paper has been to introduce the electron conductive and d-d-interactive individual and composite hypo-d-oxides of the increased altervalent capacity, or their suboxides (Magneli phases,), as catalytic supports and therefrom provide: (i) The Strong Metal-Support Interaction (SMSI) effect, and (ii) the Dynamic spillover interactive transfer of primary oxides (M-OH) for further electrode reactions, and thereby advance the overall electrocatalytic activity. The d-band has been pointed out as the bonding, adsorptive and catalytic orbital. In the same context, the phenomenon and significance of the d-d-correlations both in heterogeneous catalysis and electrocatalysis are displayed and inferred. Since hypo-d-oxides feature the exchange membrane properties, the higher the altervalent capacity, the higher the spillover effect. Potentiodynamic experiments have shown that the reversible peak of the primary oxide growth on Pt, Ru and Au supported upon hypo-d-oxides and subox...ides becomes distinctly increased in the charge capacity and shifts to remarkably more negative potential values, so that it starts even within the range of H-adatoms desorption, while its rfeduction extends until and merge with the UPD of hydrogen atoms. With wet tungstenia doped titania supported Pt catalyst in membrane cells these peaks dramatically increase in their charge capacity and reversibly become shrunk with a decreased moisture content in the feeding inert gas mixture, and vice versa. Such distinct potentiodynamic scans, in conjunction with some broaden complementary kinetic electrocatalytic improvements rising from the same hypo-d-oxide and/or suboxide interactive support effects, have been proved to be the best and comparable experimental evidence for the spillover effect of primary oxides.
Кључне речи:
Catalytic spillover / Electrocatalytic d-band / Hypo-hyper-d-d-interactive bonding / Intermetallic phases, altervalent capacity / Primary oxide (M-OH) / SMSI (Strong Metal-Support d-d-Interaction) / Surface oxide (M=O)Извор:
Chemical Industry and Chemical Engineering Quarterly, 2008, 14, 2, 119-136Издавач:
- Serbian Chemical Society
Финансирање / пројекти:
- Ministry of Science, Technologies and Development, Republic of Serbia, under Contract No. 142038.
- EU Project "Prometheas", Contract No. ICA2-2001-10037.
- IP7 EU Project "STRONGCAT" in Nanoscience and Nanotechnology.
DOI: 10.2298/CICEQ0802119J
ISSN: 1451-9372
WoS: 000262366800007
Scopus: 2-s2.0-49649105286
Институција/група
Tehnološko-metalurški fakultetTY - JOUR AU - Jakšić, Jelena M. AU - Lačnjevac, Časlav M. AU - Krstajić, Nedeljko V. AU - Jakšić, Milan M. PY - 2008 UR - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5562 AB - The aim of the present paper has been to introduce the electron conductive and d-d-interactive individual and composite hypo-d-oxides of the increased altervalent capacity, or their suboxides (Magneli phases,), as catalytic supports and therefrom provide: (i) The Strong Metal-Support Interaction (SMSI) effect, and (ii) the Dynamic spillover interactive transfer of primary oxides (M-OH) for further electrode reactions, and thereby advance the overall electrocatalytic activity. The d-band has been pointed out as the bonding, adsorptive and catalytic orbital. In the same context, the phenomenon and significance of the d-d-correlations both in heterogeneous catalysis and electrocatalysis are displayed and inferred. Since hypo-d-oxides feature the exchange membrane properties, the higher the altervalent capacity, the higher the spillover effect. Potentiodynamic experiments have shown that the reversible peak of the primary oxide growth on Pt, Ru and Au supported upon hypo-d-oxides and suboxides becomes distinctly increased in the charge capacity and shifts to remarkably more negative potential values, so that it starts even within the range of H-adatoms desorption, while its rfeduction extends until and merge with the UPD of hydrogen atoms. With wet tungstenia doped titania supported Pt catalyst in membrane cells these peaks dramatically increase in their charge capacity and reversibly become shrunk with a decreased moisture content in the feeding inert gas mixture, and vice versa. Such distinct potentiodynamic scans, in conjunction with some broaden complementary kinetic electrocatalytic improvements rising from the same hypo-d-oxide and/or suboxide interactive support effects, have been proved to be the best and comparable experimental evidence for the spillover effect of primary oxides. PB - Serbian Chemical Society T2 - Chemical Industry and Chemical Engineering Quarterly T1 - Interactive supported electrocatalysts and spillover effect in electrocatalysis for hydrogen and oxygen electrode reactions EP - 136 IS - 2 SP - 119 VL - 14 DO - 10.2298/CICEQ0802119J ER -
@article{ author = "Jakšić, Jelena M. and Lačnjevac, Časlav M. and Krstajić, Nedeljko V. and Jakšić, Milan M.", year = "2008", abstract = "The aim of the present paper has been to introduce the electron conductive and d-d-interactive individual and composite hypo-d-oxides of the increased altervalent capacity, or their suboxides (Magneli phases,), as catalytic supports and therefrom provide: (i) The Strong Metal-Support Interaction (SMSI) effect, and (ii) the Dynamic spillover interactive transfer of primary oxides (M-OH) for further electrode reactions, and thereby advance the overall electrocatalytic activity. The d-band has been pointed out as the bonding, adsorptive and catalytic orbital. In the same context, the phenomenon and significance of the d-d-correlations both in heterogeneous catalysis and electrocatalysis are displayed and inferred. Since hypo-d-oxides feature the exchange membrane properties, the higher the altervalent capacity, the higher the spillover effect. Potentiodynamic experiments have shown that the reversible peak of the primary oxide growth on Pt, Ru and Au supported upon hypo-d-oxides and suboxides becomes distinctly increased in the charge capacity and shifts to remarkably more negative potential values, so that it starts even within the range of H-adatoms desorption, while its rfeduction extends until and merge with the UPD of hydrogen atoms. With wet tungstenia doped titania supported Pt catalyst in membrane cells these peaks dramatically increase in their charge capacity and reversibly become shrunk with a decreased moisture content in the feeding inert gas mixture, and vice versa. Such distinct potentiodynamic scans, in conjunction with some broaden complementary kinetic electrocatalytic improvements rising from the same hypo-d-oxide and/or suboxide interactive support effects, have been proved to be the best and comparable experimental evidence for the spillover effect of primary oxides.", publisher = "Serbian Chemical Society", journal = "Chemical Industry and Chemical Engineering Quarterly", title = "Interactive supported electrocatalysts and spillover effect in electrocatalysis for hydrogen and oxygen electrode reactions", pages = "136-119", number = "2", volume = "14", doi = "10.2298/CICEQ0802119J" }
Jakšić, J. M., Lačnjevac, Č. M., Krstajić, N. V.,& Jakšić, M. M.. (2008). Interactive supported electrocatalysts and spillover effect in electrocatalysis for hydrogen and oxygen electrode reactions. in Chemical Industry and Chemical Engineering Quarterly Serbian Chemical Society., 14(2), 119-136. https://doi.org/10.2298/CICEQ0802119J
Jakšić JM, Lačnjevac ČM, Krstajić NV, Jakšić MM. Interactive supported electrocatalysts and spillover effect in electrocatalysis for hydrogen and oxygen electrode reactions. in Chemical Industry and Chemical Engineering Quarterly. 2008;14(2):119-136. doi:10.2298/CICEQ0802119J .
Jakšić, Jelena M., Lačnjevac, Časlav M., Krstajić, Nedeljko V., Jakšić, Milan M., "Interactive supported electrocatalysts and spillover effect in electrocatalysis for hydrogen and oxygen electrode reactions" in Chemical Industry and Chemical Engineering Quarterly, 14, no. 2 (2008):119-136, https://doi.org/10.2298/CICEQ0802119J . .