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  • Physical Chemistry  (50)
  • Wiley-Blackwell  (50)
  • American Meteorological Society
  • Annual Reviews
  • 1970-1974  (50)
  • 1
    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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  • 2
    Electronic Resource
    Electronic Resource
    The pyrolysis of 2-nitrosoisobutane and the bond dissociation energies of nitroso compounds (1974)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 6 (1974), S. 813-828 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Study of the reaction by very-low-pressure pyrolysis (VLPP) in the temperature range of 550-850°K yields for the high-pressure Arrhenius parameters \documentclass{article}\pagestyle{empty}\begin{document}$$\log {\rm }\,k_{\rm 1} = (15.6 \pm 0.5) - (36.0 \pm 1.0)/\theta {\rm \,(sec}^{{\rm - 1}})$$\end{document} where θ = 2.303RT in kcal/mole. These in turn yield for the high-pressure second-order recombination of tBu + NO, k-1 = (3.5 ± 1.7) × 109 1./mole·sec at 600°K. For the competing reaction l./mole·sec and E4 ≥ 4.2 kcal/mole. The bond dissociation energy DHo (tBu-NO) was determined to be (39.5 ± 1.5) kcal/mole, both from the equilibrium constant and from the activation energy of reaction (1), obtained from RRKM calculations. A ‘free-volume’ model for the transition state for dissociation is consistent with the data. A limited study of the system at 8-200 torr showed an extremely rapid inhibition by products and a very complex set of products.
    Additional Material: 3 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550060605
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  • 3
    Electronic Resource
    Electronic Resource
    Computational modeling of the mechanisms of the free radical-chain reaction of alkanes with oxygen. The oxidation of isobutane, n-butane, and isopentane (1972)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 4 (1972), S. 345-362 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: A general computational method for obtaining complete solutions of time-dependent kinetic equations has been developed and applied to free radical-initiated reactions of alkanes with oxygen. The method has been applied to the low-temperature, peroxide-initiated oxidations of isobutane and isopentane. Using available independently measured and estimated values for the rate constants and activation parameters for each of the 20 proposed reaction steps for the oxidation of isobutane, the rates and products have been calculated for both the liquid phase and gas phase in the range of 100°-155°C. The calculated rates and products of oxidation agree with published experimental values. The oxidation of isopentane was examined by a 32-reaction model. The rate constants were estimated using values for the appropriate rate steps in the oxidation of n-butane and isobutane. The calculation of the oxidation rate and products agree with our experiments.
    Additional Material: 7 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550040312
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  • 4
    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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  • 5
    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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  • 6
    Electronic Resource
    Electronic Resource
    A flash photolysis-resonance fluorescence study of the reaction of atomic hydrogen with molecular oxygen H + O2 + M → HO2 + M (1974)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 6 (1974), S. 401-416 
    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 H + O2 + M → HO2+M over a temperature range of 220-360°K. Over this temperature range, the data could be fit to an Arrhenius expression of the following form: \documentclass{article}\pagestyle{empty}\begin{document}$$k_{{\rm Ar}} = (6.75{\rm } \pm {\rm }1.1){\rm } \times {\rm }10^{ - 33} \exp {\rm }[685{\rm } \pm {\rm }128{\rm cal/mole]/}RT$$\end{document} The units for kAr are cm6/mole-s. At 300°K the relative efficiencies for the third-body gases Ar:He:H2:N2:CH4 were found to be 1.0:0.93:3.0:2.8:22. Wide variations in the photoflash intensity at several temperatures demonstrated that the reported rate constants were measured in the absence of other complex chemical processes.
    Additional Material: 5 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550060310
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  • 7
    Electronic Resource
    Electronic Resource
    The rate of the gas phase iodination of cyclobutane. The heat of formation of the cyclobutyl radicalThis work was supported, in part, by Grant No. AP 00353-07 of the Environmental Protection Agency, Air Pollution Control Administration. (1972)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 4 (1972), S. 487-495 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The gas phase iodination of cyclobutane was studied spectrophotometrically in a static system over the temperature range 589° to 662°K. The early stage of the reaction was found to correspond to the general mechanism \documentclass{article}\pagestyle{empty}\begin{document}$$\begin{array}{l} {\rm RH} + {\rm I} \cdot \mathop {{\rm \rightleftharpoons}}\limits^1 {\rm R} \cdot + {\rm HI} \\ {\rm R} \cdot + {\rm I}_{\rm 2} \mathop {{\rm \rightleftharpoons}}\limits^2 {\rm R} - {\rm I} + {\rm I} \cdot \\ \end{array}$$\end{document} where the Arrenius parameters describing k1 are given by log k1/M-1 sec-1 = 11.66 ± 0.11 - 26.83 ± .31/θ, θ = 2.303RT in kcal/mole. The measured value of E1, together with the fact that E-1 = 1 ± 1 kcal/mole, provides ΔHf,2980(c-C4H7.) = 51.14 ± 1.0 kcal/mole, and the corresponding bond dissociation energy, D(c-C4H7—H) = 96.8 ± 1.0 kcal/mole. A bond dissociation energy of 1.8 kcal/mole higher than that for a normal secondary C—H bond corresponds to one half of the extra strain energy in cyclobutene compared to cyclobutane and is in excellent agreement with the recent value of Whittle, determined in a completely different system. Estimates of ΔHf0 and entropy of cyclobutyl iodide are in very good agreement with the equilibrium constant K12 deduced from the kinetic data. Also in good agreement with estimates of Arrhenius parameters is the rate of HI elimination from cyclobutyl iodide.
    Additional Material: 2 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550040503
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  • 8
    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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  • 9
    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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  • 10
    Electronic Resource
    Electronic Resource
    Electronically excited oxygen atoms, O(21D2). A time-resolved study of the collisional quenching by the gases H2, D2, CH4, NO, NO2, N2O, and C3O2 using atomic absorption spectroscopy in the vacuum ultraviolet (1973)
    New York, NY : Wiley-Blackwell
    International Journal of Chemical Kinetics 5 (1973), S. 819-831 
    Details
    ISSN: 0538-8066
    Keywords: Chemistry ; Physical Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: Time-resolved atomic absorption spectroscopy in the vacuum ultraviolet has been employed to monitor electronically excited oxygen atoms, O(21D2), following their genera-tion by the flash photolysis of ozone in the Hartley band region. We report the first values for the absolute second-order rate constants describing the removal of the excited atom on collision with the molecules H2, D2, CH4, NO, NO2, N2O, and C3O2. Where possible, these data are considered within the context of restrictions arising from spin and orbital symmetry and are further discussed in tems of previously reported relative rate data derived from indirect measurements. Consideration is given to the importance of these rate con-stants in discussing processes taking place in the earth's atmosphere and in systems giving rise to chemical laser action.
    Additional Material: 5 Ill.
    Type of Medium: Electronic Resource
    URL: http://dx.doi.org/10.1002/kin.550050509
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