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  • 1980-1984  (11)
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  • 1
    Electronic Resource
    Electronic Resource
    Shock-induced kinetics of the disilane decomposition and silylene reactions with trimethylsilane and butadiene (1982)
    s.l. : American Chemical Society
    Organometallics 1 (1982), S. 1217-1220 
    Details
    ISSN: 1520-6041
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/om00069a020
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  • 2
    Electronic Resource
    Electronic Resource
    Kinetics of the high-temperature thermal decomposition of silanes and alkylsilanes (1983)
    s.l. : American Chemical Society
    Organometallics 2 (1983), S. 1891-1894 
    Details
    ISSN: 1520-6041
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/om50006a038
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  • 3
    Electronic Resource
    Electronic Resource
    Mechanism and kinetics of the homogeneous gas-phase thermal decomposition of methylgermane (1981)
    s.l. : American Chemical Society
    Journal of the American Chemical Society 103 (1981), S. 5740-5746 
    Details
    ISSN: 1520-5126
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1021/ja00409a021
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  • 4
    Electronic Resource
    Electronic Resource
    Kinetics and mechanism of the germane decomposition (1980)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 12 (1980), S. 661-670 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The homogeneous gas-phase thermal decomposition kinetics of germane have been measured in a single-pulse shock tube between 950 and 1060 K at pressures around 4000 torr. The initial decomposition is GeH4 → GeH2 + H2 in its pressure-dependent regime, with log kGeH4(4000) = 13.83 ± 0.78 - 50,750 ± 3570 cal/2.303RT. RRKM calculations suggest that the high-pressure Arrhenius parameters are log k GeH4(M → ∞) = 15.5 - 54,300 cal/2.303RT. Extrapolations to static system pyrolysis conditions (T ∼ 600 K, P ∼ 200 torr) give homogeneous reaction rates which are much slower than those observed, hence the static system pyrolysis of germane must be predominantly heterogeneous. Shock-initiated pyrolysis reaction stoichiometry is 2 mol H2 per mole GeH4, suggesting that the subsequent decomposition of germylene is essentially quantitative. Investigations of the hydrogen product yields for pyrolysis of GeD4 in øCH3 further indicate that the germylene decomposition reaction is mainly GeH2 → H2 + Ge, but that a small amount of reaction to H atoms may also occur.
    Additional Material: 1 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550120907
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  • 5
    Electronic Resource
    Electronic Resource
    The gas-phase decomposition of methylsilane. Part I. Mechanism of decomposition under shock-tube conditions (1984)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 16 (1984), S. 7-21 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The gas-phase decompositions of methylsilane and methylsilane-d3 have been investigated in a single-pulse shock tube at 4700 torr total pressure in the temperature range of 1125-1250 K. For CH3SiD3 at 1200 K three primary steps occur in the homogeneous decomposition with efficiencies in parentheses: \documentclass{article}\pagestyle{empty}\begin{document}$$ {\rm CH}_{\rm 3} {\rm SiD}_{\rm 3} \mathop {\longrightarrow} \limits^1 {\rm CH}_{\rm 3} {\rm SiD} + {\rm D}_{\rm 2} \left( {0.71} \right) $$\end{document}, \documentclass{article}\pagestyle{empty}\begin{document}$$ {\rm CH}_{\rm 3} {\rm SiD}_{\rm 3} \mathop {\longrightarrow} \limits^2 {\rm CH}_{\rm 4} + {\rm SiD}_{\rm 2} \left( {0.15} \right) $$\end{document}, and \documentclass{article}\pagestyle{empty}\begin{document}$$ {\rm CH}_{\rm 3} {\rm SiD}_{\rm 3} \mathop {\longrightarrow} \limits^3 {\rm CH}_{\rm 2} \raise1pt\hbox{=\kern-3.45 pt=} {\rm SiD}_{\rm 2} \left( {0.14} \right) $$\end{document}. For CH3SiH3 at 1200 K the primary CH4 elimination efficiency is 0.09 while the total primary H2 elimination efficiency is 0.91. Minor product formations of C2H4, acetylene, dimethylsilane, and SiH4 are discussed.
    Additional Material: 4 Tab.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550160104
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  • 6
    Electronic Resource
    Electronic Resource
    The gas-phase decomposition of methylsilane. Part III. Kinetics (1984)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 16 (1984), S. 31-39 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The homogeneous gas-phase decomposition kinetics of methylsilane and methylsilane-d3 have been investigated by the comparative-rate-single-pulse shock-tube technique at total pressures of 4700 torr in the 1125-1250 K temperature range. Three primary processes occur: CH3SiH3 → CH3SiH + H2 (1), CH3SiH3 → CH4 + SiH2 (2), and CH3SiH3 → CH2 = SiH2 + H2 (3). The high-pressure rate constants for the primary processes in CH3SiH3 obtained by RRKM calculations are log (k1 + k3) (s-1) = 15.2 - 64,780 Cal/θ and log k2 (s-) = 14.50 - 67,600 → 2800 Cal/θ. For CH3SiD3 these same rate constants are log k1 (s-) = 14.99 - 64,700 cal/θ log k2 (s-) = 14.68 - 66,700 → 2000 cal/θ, and log k3 (s-) = 14.3 - 64,700 cal/θ.
    Additional Material: 1 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550160106
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  • 7
    Electronic Resource
    Electronic Resource
    The gas-phase decomposition of methylsilane. Part II. Mechanisms of decomposition under static system conditions (1984)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 16 (1984), S. 23-30 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The static system pyrolysis of methylsilane (T ∼ 700 K, PT ∼ 150 torr), pure and in the presence of ethylene, propylene, and acetylene, has been investigated. It is proposed that in the uninhibited system, the major products (silane and dimethylsilane) are produced by free radical processes, and that the free radicals are formed at the walls from methylsilylenes. In the presence of olefins, the free radicals are trapped to form methylsilane adducts. In acetylene, trapping of methylsilylenes prevents free radical production and eliminates the free radical produced products of the pure and the olefin inhibited systems. Rates of initiation correlate with rates of reactant loss in acetylene inhibited systems, and with rates of hydrogen formation in olefin inhibited systems. Rough estimates of primary dissociation process yields give for the 1,1-H2 elimination φ1,1 ≅ 0.78, for the 1,2-H elimination φ1,2 ≅ 0.16, and for the methane elimination φCH4 ≅ 0.06 at 700 K. Deuteration lowers initial step kinetics by about 15%.
    Additional Material: 1 Tab.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550160105
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  • 8
    Electronic Resource
    Electronic Resource
    Shock-initiated decomposition of tetramethylgermane and the reaction of methyl radicals with toluene (1982)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 14 (1982), S. 279-289 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The shock-initiated decomposition of tetramethylgermane (1078-1242 K) has been found to involve successive elimination of methyl radicals with the rate constant k1 for the first step given by \documentclass{article}\pagestyle{empty}\begin{document}$$ \log k_{\rm 1} {\rm}(s^{- 1}) = {\rm}(17.00 \pm 0.35) - (77.0 \pm 1.9)\theta {\rm kcal/mol} $$\end{document} In the presence of excess toluene the products were CH4 (major), C2H4, and C2H6. Results relevant to the reaction of methyl radicals with toluene compared to methyl radical recombination are discussed.
    Additional Material: 3 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550140308
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  • 9
    Electronic Resource
    Electronic Resource
    Mechanism and kinetics of the shock-tube decomposition of vinylsilane (1984)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 16 (1984), S. 289-305 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The shock-induced thermal decompositions of vinylsilane and vinylsilane-d3 (0.2% on argon) have been studied in the temperature range of 1085-1275 K, and at total pressures of about 3100 torr. In systems without silylene traps, some induced decomposition occurs which is attributed to the silylene chain sequence VSiH → C2H2 + SiH2, S̈iH2 + VSiH3 ⇄ VSiH2SiH3 → VSiH2S̈iH + H2, VSiH2S̈iH → VSiH + S̈iH2. In the presence of silylene traps (butadiene and acetylene), the overall decomposition kinetics are log k(VSiH3, s-1) = 14.95 - 63,268 cal/2.303RT and log k(VSiD3, s-1) = 15.14 - 64,815 cal/2.303RT. Three primary processes contribute to the decomposition: 1,1-H2 elimination, 1,2-H2 elimination, and ethylene elimination. Two mechanisms are proposed, one for exclusive primary process formation of C2H4, and the other for both primary and secondary formation routes. Modeling studies are reported which show that both mechanisms can be made compatible with the rate and product yield data within experimental errors.
    Additional Material: 1 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550160402
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  • 10
    Electronic Resource
    Electronic Resource
    The kinetics and mechanism of the shock induced gas phase decomposition of ethylsilane (1984)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 16 (1984), S. 1371-1383 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The decomposition kinetics of ethylsilane under shock tube conditions (PT ca. 3100 torr, T ≃ 1080-1245 K), both in the absence and presence of silylene trapping agents (butadiene and acetylene) are reported. Arrhenius parameters under maximum butadiene inhibition are: log k(C2H5SiH3) = 15.14-64,769 ± 1433 cal/2.303 RT; log k(C2H5SiD3) = 15.29-66,206 ± 1414/2.303 RT. The uninhibited reaction is subject to silylene induced decomposition (63% lowest T -- 24% highest T). Major reaction products are ethylene and hydrogen, consistent with two dominant primary dissociation reactions: C2H5SiD3 → C2H5SiD + D2, φ ≃ 0.66; C2H5SiD3 → CH3CH = SiD2 + HD, φ ≃ 0.30. Minor products suggest several other less important primary processes: alkane elimination, φ ≃0.02, and free-radical production via simple bond fission, φ ≃0.02. An upper limit for the activation energy of the decomposition, C2H5SiH → C2H4 + SiH2, of E 〈 30 ± 4 kcal is established, and speculations on the mechanism of this decomposition (concerted or stepwise) with conclusions in favor of the stepwise path are made. Computer modeling studies for the reaction both in the absence and presence of butadiene are shown to be in good agreement with the experimental observations.
    Additional Material: 1 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550161109
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