Abstract
The increase in the rate of catalytic oxidation of CO on palladium nanosized coatings is measured when electric voltages of different polarities and magnitudes are applied to the coatings from an external source. Under the experimental conditions at 330°С, atmospheric pressure, and the initial composition of the mixture of 1.8% CO + 10.2% О2 + an Ar application of a positive voltage of +10 or +30 V to the coating leads to the CO oxidation rate increasing by 14 or 42%, respectively. Applying a negative voltage of –10 or –30 V results in less acceleration of oxidation by 4 or 12%. It is shown that the effect of the voltage supply does not depend on the particle size in the coating and increases linearly with increasing voltage. The quantum-chemical calculations of the heat of the association of CO and O2 with the simplest neutral or electrically charged palladium Pd2 clusters are calculated. It is found that the creation on Pd2 of a positive charge leads to a decrease in the difference between the heat of association of CO and O2 by 16.7 kcal/mol, while the creation on Pd2 of a negative charge leads to a smaller effect: a decrease in the specified difference by 10.6 kcal/mol. Based on the results of the calculations, an explanation is proposed for the increase in the rate of catalytic oxidation of CO on palladium electrically charged using an external voltage source is proposed.
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ACKNOWLEDGMENTS
The quantum-chemical calculations were performed using the supercomputer resources of the Joint Supercomputer Center, Russian Academy of Sciences.
Funding
The work was carried out as part of a state assignment of the Semenov Federal Research Center for Chemical Physics, Russian Academy of Sciences (topic 45.9, 0082-2014-0011, AAAA-A20-120013190076-0) and with financial support from the Russian Foundation for Basic Research (grant no. 20-03-00419).
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Grishin, M.V., Gatin, A.K., Slutskii, V.G. et al. Electric Stimulation of The Catalytic Activity of Palladium Nanosized Coatings during Oxidation with CO. Russ. J. Phys. Chem. B 15, 777–781 (2021). https://doi.org/10.1134/S1990793121050031
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DOI: https://doi.org/10.1134/S1990793121050031