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Effect of active impurities on the condensation of nanoparticles from supersaturated carbon vapor in the combined laser photolysis of C3O2 and H2S

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Abstract

The effect of active H2S, HS·, and atomic hydrogen impurities on the condensation of highly supersaturated carbon vapor obtained in the combined laser photolysis of a mixture of C3O2 and H2S diluted with argon was studied. The concentrations of carbon vapor, HS·, and atomic hydrogen obtained in the laser photolysis of the mixture were determined using the absorption cross sections of C3O2 and H2S molecules measured in this work and the measured amount of absorbed laser radiation. The time profiles of the sizes of growing nanoparticles synthesized in C3O2 + Ar and C3O2 + H2S + Ar mixtures were measured using the laser-induced incandescence (LII) method. An improved LII model was developed, which simultaneously took into account the heating and cooling of nanoparticles and the temperature dependence of the thermophysical properties of nanoparticles, as well as the cooling of nanoparticles by evaporation and thermal emission. The size distributions of carbon nanoparticles formed in the presence and absence of active impurities were determined with the use of a transmission electron microscope. The final average size of carbon nanoparticles was found to decrease from 12 to 9 nm upon the addition of H2S to the system, whereas the rate of nanoparticle growth decreased by a factor of 3, and the properties of nanoparticles changed. In particular, the translational energy accommodation coefficient for Ar molecules at the surface of carbon nanoparticles was found to decrease from 0.44 to 0.30. A comparison of the calculated total carbon balance at the early stage of nanoparticle formation with experimental data demonstrated that the reaction C + H2S → HCS· + H, which removes a portion of carbon vapor from the condensation process, has a determining effect on the carbon balance in the system. It was found that HS· and atomic hydrogen affect the carbon balance in the system only slightly. Thus, the experimentally observed decrease in the rate of nanoparticle growth and in the sizes of nanoparticles can be explained by a decrease in the concentration of free carbon upon the addition of H2S molecules to the system.

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Authors and Affiliations

  1. Institute of Thermal Physics of Extreme States, Russian Academy of Sciences, Moscow, 125412, Russia

    E. V. Gurentsov & A. V. Eremin

  2. Institut für Verbrennung und Gasdynamik, 47048, Duisburg, Germany

    C. Schulz

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  1. E. V. Gurentsov
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  2. A. V. Eremin
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  3. C. Schulz
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Correspondence to E. V. Gurentsov.

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Original Russian Text © E.V. Gurentsov, A.V. Eremin, C. Schulz, 2008, published in Kinetika i Kataliz, 2008, Vol. 49, No. 2, pp. 179–189.

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Gurentsov, E.V., Eremin, A.V. & Schulz, C. Effect of active impurities on the condensation of nanoparticles from supersaturated carbon vapor in the combined laser photolysis of C3O2 and H2S. Kinet Catal 49, 167–177 (2008). https://doi.org/10.1134/S002315840802002X

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