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  • Physical Chemistry  (7)
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  • 1
    Electronic Resource
    Electronic Resource
    A flash photolysis-resonance fluorescence kinetics study of ground-state sulfur atoms. II. Rate parameters for reaction of S(3P) with C2H4 (1972)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 4 (1972), S. 383-394 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Absolute rate constants for the reaction of S(3P) with ethylene were measured over an ethylene concentration range of 7, a total pressure of 50 to 400 torr, and a flash intensity range of 10. At 298°K, the bimolecular rate constant was found to be invariant over this range of variables and had a measured value of 4.96 × 10-13 cm3 molec-1 s-1. Over the temperature range of 218° to 442°K, the rate data could be fit to a simple Arrhenius equation of the form \documentclass{article}\pagestyle{empty}\begin{document}$$k_1 = (7.13 \pm 0.74) \times 10^{ - 12} {\rm exp}\left({\frac{{{\rm - 1}{\rm .58} \pm {\rm 0}{\rm .08 kcal/mole}}}{{RT}}} \right)$$\end{document} Units are cm3 molec-1 s-1. The dependence of the measured value of k1 on the concentration of the reaction product ethylene episulfide is discussed.
    Additional Material: 2 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550040403
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  • 2
    Electronic Resource
    Electronic Resource
    A flash photolysis-resonance fluorescence kinetics study of the reactions of ground-state sulfur atoms. V. Rate parameters for the reaction of S(3P)with cis-2-butene and tetramethylethylene (1973)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 5 (1973), S. 841-857 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Rate parameters for the reaction of ground-state atomic sulfur, S(3P), with the olefins cis-2-butene and tetramethylethylene have been determined over a temperature range of ∽280°K. A major finding of this study was that the rate constants for both reactions showed negative temperature dependencies. When k is expressed in the form of an Arrhenius equation, this necessarily leads to negative activation energies: k1 = (4.68 ± 0.70) × 10-12 exp (+0.23 ± 0.09 kcal/mole)/RT (219°-500°K) k2 = (4.68 ± 1.70) × 10-12 exp (+1.29 ± 0.23 kcal/mole)/RT (252°-500°K) Units are cm3 molec-1s-1. When a threshold energy of 0.0 kcal/mole is assumed for reaction (2), the temperature dependence of the preexponential term has a value of T-2. Making the usual simplifying assumptions, neither collision theory nor transition state theory leads to a preexponential factor with a strong enough negative temperature dependence. A comparison of these results with those derived from studies of the reactions of atomic oxygen, O(3P), with the same olefins shows that in both studies simple bimolecular processes were being examined. Also discussed are the possible experimental and theoretical ramifications of these new results.
    Additional Material: 5 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550050511
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  • 3
    Electronic Resource
    Electronic Resource
    Theoretical rate constant calculations for O(3P) with saturated hydrocarbons (1983)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 15 (1983), S. 705-719 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Theoretical rate constants have been calculated for O(3P) with five saturated hydrocarbons, CH4, C2H6, C3H8, iso-C4H10, and neo-C5H12. The method of choice is bond energy-bond order (BEBO) with activated complex theory (ACT). Because the BEBO method is empirical, O(3P) + CH4 is evaluated first, and the theoretical results are compared to more rigorous calculations and to the empirical transition state method. Comparisons are also made between predictions and experimental results. All of these comparisons show that the BEBO-ACT method gives results which are consistent with experiment and other theory. Because the method is successful, the other four cases are then considered. Ambiguity arises for the higher hydrocarbons from the problem of internal rotations in the activated complexes, and three cases are evaluated. Best agreement with experiment is obtained if the primary rotor(s) in the complexes are considered to be free. Predictions of rate constants are made from 500 to 2500 K. Throughout the discussion issues of theory which are common to any ACT calculation from any method of potential energy evaluation (LEP, LEPS, or ab initio quantum mechanics) are featured.
    Additional Material: 2 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550150803
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  • 4
    Electronic Resource
    Electronic Resource
    A flash photolysis resonance fluorescence kinetics study of ground-state sulfur atoms. III. Rate parameters for reaction of S(3P) with ethylene episulfide (1973)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 5 (1973), S. 149-153 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Absolute rate constants for the reaction of S(3P) with ethylene episulfide were measured over a C2H4S concentration range of 5, a total pressure of 20-200 tort, and a flash intensity range of ˜4. Over this range of variables, the bimolecular rate constant was found to be invariant. Because of limitations imposed by the physical properties of the reactant C2H4S, temperature variations were necessarily held to the range 298-355°K. The bimolecular rate constant was found to be invariant over this limited temperature range, having a value of (4.47 ± 0.26) × 10-11 cm3 molec.-1 sec-1. The possible influence of this reaction in studies of the S(3P)-ethylene system are discussed.
    Additional Material: 2 Tab.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550050113
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  • 5
    Electronic Resource
    Electronic Resource
    A flash photolysis-resonance fluorescence kinetics study of ground-state sulfur atoms. IV. Rate parameters for reaction of S(3P) with propene and 1-butene (1973)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 5 (1973), S. 375-384 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Using the technique of flash photolysis-resonance fluorescence, absolute rate constants have been measured for the reaction of S(3P) with propene and 1-butene. Variations in experimental conditions included the following: temperature (215-500°K); total pressure a factor of 10; olefin concentration, a factor of 6; flash intensity (S atom concentration), a factor of 10. It was found that over these variations in the experimental conditions only the temperature had a measureable effect on the bimolecular rate constant. The derived Arrhenius rate expressions for the reactions (2) and (3) were as follows: \documentclass{article}\pagestyle{empty}\begin{document}$$ k_2 = \left( {6.03 \pm 0.72} \right) \times 10^{ - 12} \exp \left( {\frac{{ - 0.38 \pm 0.09kcal/mol}}{{RT}}} \right) $$\end{document} temperature range 214-500°K \documentclass{article}\pagestyle{empty}\begin{document}$$ k_3 = \left( {7.41 \pm 1.15} \right) \times 10^{ - 12} \exp \left( {\frac{{ - 0.36 \pm 0.09kcal/mol}}{{RT}}} \right) $$\end{document} Units are cm3 molec-1 s-1.
    Additional Material: 2 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550050308
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  • 6
    Electronic Resource
    Electronic Resource
    The flash photolysis - shock tube technique using atomic resonance absorption for kinetic studies at high temperatures (1985)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 17 (1985), S. 315-326 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: A flash photolysis-shock tube technique is described for making kinetic measurements at high temperature. Coupled with sensitive atomic resonance absorption detection, this method allows bimolecular rate constants for atom-molecule reactions to be measured directly under conditions free from kinetic complications. Experiments were performed in the reflected shock regime, and the temperature and density were calculated using ideal shock wave theory in this initial work. Results for the reaction of atomic hydrogen with ammonia are presented to illustrate the potential of the technique. The values of the Arrhenius rate parameters found in these experiments, 900 K ≤ T ≤ 1850 K, were A = (1.14 ± 0.12) × 10-10 cm3 molecule-1 s-1 and Ea = 13,216 ± 242 cal mol-1. This result gives rate constants that are about five times larger than those from previous studies. Although corrections for nonidealities in the reflected shock region are anticipated and under investigation, the expected changes will be relatively small and thus the large discrepancy noted here will remain.
    Additional Material: 5 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550170308
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  • 7
    Electronic Resource
    Electronic Resource
    A flash photolysis-resonance fluorescence kinetics study of ground-state sulfur atoms: I. Absolute rate parameters for reaction of S(3P) with O2(3Σ). (1972)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 4 (1972), S. 367-382 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The flash photolysis-resonance fluorescence technique has been used to measure the reaction of ground-state sulfur atoms with molecular oxygen as a function of both temperature and total pressure. The most suitable source of S(3P) for this study was found to be COS in the presence of CO2, as a diluent gas and with the photolysis flash filtered so as to remove all radiation of wavelengths below 1650 Å. Under these conditions, it was found that over the temperature range of 252-423°K the rate data could be fit to a simple Arrhenius-type equation of the form \documentclass{article}\pagestyle{empty}\begin{document}$$k_1 = (2.24 \pm 0.27) \times 10^{ - 12} {\rm exp}\left({\frac{{{\rm - 0}{\rm .00} \pm {\rm 0}{\rm .10 kcal/mole}}}{{RT}}} \right)$$\end{document} Units are cm3 molec-1 s-1. The small A-factor for this reaction, the lack of any pressure dependence, and the direct observation of the production of O(3P) with increasing reaction time suggest that the S(3P) atom attacks the O2(3Σ) molecule end-on forming SOO which rapidly falls apart to form SO (3Σ) and O(3P).
    Additional Material: 4 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550040402
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