THE VAPOR PHASE PHOTOLYSIS OF HEXAFLUOROACETONE IN THE PRESENCE OF METHANE AND ETHANE

1955 ◽  
Vol 33 (5) ◽  
pp. 743-749 ◽  
Author(s):  
P. B. Ayscough ◽  
J. C. Polanyi ◽  
E. W. R. Steacie

The photolytic decomposition of hexafluoroacetone by light of wavelength 3130 Å has been used to produce trifluoromethyl radicals for a study of their reactions with methane and ethane. It has been shown that these radicals abstract hydrogen with greater facility than do methyl radicals. The activation energies for the two reactions[Formula: see text]and[Formula: see text]are found to be 10.3 ± 0.5 kcal./mole and 7.5 ±0.5 kcal./mole respectively, if one can assume zero activation energy for the recombination of trifluoromethyl radicals.

1959 ◽  
Vol 37 (9) ◽  
pp. 1462-1468 ◽  
Author(s):  
A. R. Blake ◽  
K. O. Kutschke

The pyrolysis of di-t-butyl peroxide has been reinvestigated and used as a source of methyl radicals to study the abstraction reaction between methyl radicals and formaldehyde. At low [HCHO]/[peroxide] ratios the system was simple enough for kinetic analysis, and a value of 6.6 kcal/mole was obtained for the activation energy. At higher [HCHO]/[peroxide] ratios the system became very complicated, possibly due to the increased importance of addition reactions.


1956 ◽  
Vol 34 (2) ◽  
pp. 103-107 ◽  
Author(s):  
P. B. Ayscough ◽  
E. W. R. Steacie

A study of the reactions of trifluoromethyl radicals, produced by the photolysis of hexafluoroacetone, with propane, n-butane, and isobutane has been made. The rate constants of the hydrogen-abstraction reactions have been determined at temperatures between 27 °C and 119 °C and the activation energies found to be 6.5 ± 0.5, 5.1 ± 0.3, and 4.7 ± 0.3 kcal./mole respectively. These values are compared with those obtained for the reactions with methane and ethane, and with the corresponding reactions of methyl radicals.


1960 ◽  
Vol 38 (11) ◽  
pp. 2128-2135 ◽  
Author(s):  
S. J. W. Price ◽  
K. O. Kutschke

The reactions of C2F5 radicals, produced by the photolysis of (C2F5)2CO, with methane and hydrogen have been studied. Assuming zero activation energy for 2C2F5 → C4F10 the activation energies for C2F5 + CH4 → C2F5H + CH3 and C2F5 + H2 → C2F5H + H are 10.6 kcal/mole and 11.9 kcal/mole respectively. The present results have been correlated with data on the reactions of CF3, C3F7, and CH3 radicals with H2, D2, CH4, and C2H6. Taking Erecombination ≈ 0 in all cases and assuming the frequency factor for the recombination reaction varies little from radical to radical, the order of ease of hydrogen abstraction from a given substrate is CF3 > C2F5 > C3F7 > CH3. Similarly the ease of hydrogen abstraction from a substrate by a given fluorinated radical is C2H6 > H2 > CH4 > D2. A calculation based on very limited data indicates the reaction CH3 + C2F5COC2F5 → CH3COC2F5 + C2F5 may occur with an activation energy of approximately 7 kcal/mole.


1963 ◽  
Vol s3-104 (68) ◽  
pp. 413-439
Author(s):  
D. J. GOLDSTEIN

Methods are proposed for the estimation of the rate, activation energy, heat, and affinity of staining of histological sections, and approximate results are given for the staining of mucin, mast-cell granules, chromatin, cytoplasmic ribonucleic acid (RNA), cartilage matrix, and other structures by azure A. The half-staining time t½ is the time taken by a substrate under given staining conditions to achieve half the intensity of staining it would reach at equilibrium, and is approximately equal to the time taken to stain in a given, fairly dilute dyebath to the same intensity as at equilibrium in a dyebath of half the given concentration. The activation energy E of staining is given by E = ln t½(1)/t½(2) x RT1T2/(T2-T1), where t½(1) and t½(2) are the half-staining times at absolute temperatures T1 and T2 respectively, and R is the gas constant. The activation energy of staining reflects the effect of temperature on rate of staining, and may be regarded as an index of substrate permeability. Half-staining times and activation energies of staining with azure A increase in the order mucin, mast-cell granules, chromatin, RNA, and interstitial cartilage matrix. Times of half-destaining and activation energies of destaining also are probably largely determined by substrate permeability. Differential staining dependent on differences in rate of staining may be enhanced by the use of chilled and stirred dyebaths, and by the use of dyes of large particle size. The heat of dyeing δH, sometimes regarded as the sum of the heats of formation of the various dye-substrate bonds, approximately equals RT1T2/(T2-T1)x ln [D]1/[D]2, where [D]1 and [D]2 are the concentrations of dyebath giving equal intensity of staining of the substrate at equilibrium at temperatures T1 and T2. Approximate figures for δH in kcal/mole for staining with dilute azure A are: mucin, -8; chromatin and cartilage matrix, -7; cytoplasmic RNA, -5.5; mast-cell granules, - 2 to - 4. The higher the value of -δH the more is staining inhibited by a rise in temperature of the dyebath. The affinity of a dye for a substrate may be regarded as the standard free energy change accompanying the staining process, which under certain conditions is given approximately by δF° = - RT ln τ /(1-τ)[D], where τ is the fraction of available staining sites in the substrate occupied by dye when the substrate is at equilibrium with a dyebath of concentration [D]. Differential staining of substrates with a high affinity for the dye is facilitated by the use of dilute dye solutions. Approximate values of δF° for staining with azure A at 4° C and pH 4.0, in kcal/mole, are: cartilage matrix, -3.8 (orthochromasia) and - 5.3 (metachromasia); mast-cell granules, -4 (orthochromasia) and -4.4 (metachromasia); RNA, -3.1; mucin, between - 2.7 and -3.4; chromatin, -3.1; thyroid colloid, -2.3; Xenopus poison gland secretion, -2.3 It is suggested that part of the high affinity of sulphate groups for basic dyes is due to an increase in entropy during staining, resulting from dispersion of a large hydration shell surrounding the sulphate groups before attachment of the dye.


1957 ◽  
Vol 35 (10) ◽  
pp. 1216-1224 ◽  
Author(s):  
G. O. Pritchard ◽  
E. W. R. Steacie

The photolytic and thermal decomposition of azomethane in the presence of hexafluoroacetone produces small amounts of fluorinated products, mainly fluoroform. The mechanism of this and related reactions is discussed. It is concluded that the proposed reaction.[Formula: see text]has an activation energy of about 6 kcal./mole, with a steric factor of about 10−5.


1965 ◽  
Vol 43 (7) ◽  
pp. 1961-1967 ◽  
Author(s):  
M. G. Jacko ◽  
S. J. W. Price

The pyrolysis of trimethylthallium has been studied in a toluene carrier flow system from 458 to 591 °K using total pressures from 5.6 to 33.0 mm. The progress of the reaction was followed by measuring the amount of methane, ethane, ethylene, and ethylbenzene formed and, in 21 runs, by direct thallium analysis. All preparative and kinetic work was carried out in total darkness where possible. A shielded 10 W lamp was used when some illumination was necessary.The decomposition is approximately 80% heterogeneous in an unconditioned vessel and 14–27% heterogeneous in a vessel pretreated with hot 50% HF for 10 min. The reaction proceeds by the simple consecutive release of three methyl radicals. The rate constant depends only slightly on the total pressure in the system so that the activation energy of the homogeneous process, 27.4 kcal/mole, may be equated to D[(CH3)2Tl—CH3].


1959 ◽  
Vol 37 (4) ◽  
pp. 672-678 ◽  
Author(s):  
S. Toby ◽  
K. O. Kutschke

Azomethane was photolyzed in the presence of up to 30 mole per cent formaldehyde and formaldehyde-d2 at temperatures from 80 °C to 180 °C. The value of the activation energy for the abstraction reaction with methyl radicals was found to be 6.2 kcal mole−1 for CH2O and 7.9 kcal mole−1 for CD2O. The results indicated that the formyl radical was stable over the temperature range studied.


1950 ◽  
Vol 28b (7) ◽  
pp. 395-402 ◽  
Author(s):  
M. K. Phibbs ◽  
B. deB. Darwent

The reactions of methyl radicals, produced by the photochemical decomposition of dimethylmercury, with cyclopropane, ethylene oxide, methanol and dimethyl ether have been investigated between 100° and 250 °C. The following activation energies (kcal. mole−1) for the abstraction of hydrogen from the compounds by methyl radicals were found: cyclopropane, 10.2; ethylene oxide 9.6; methanol, 8.2; and dimethyl ether, 8.0. The probability factors have been shown to be about 10−4 for all the compounds investigated.


1955 ◽  
Vol 33 (1) ◽  
pp. 31-38 ◽  
Author(s):  
P. Ausloos ◽  
E. W. R. Steacie

Azomethane has been photolyzed in the presence of CH3CHO and CH3CDO, and the results compared with the direct photolysis of the aldehydes. The activation energies found were 6.8 and 7.8 kcal./mole, respectively, for the reactions[Formula: see text]The results furnish evidence that only an acyl hydrogen is captured. Evidence has also been found for the occurrence of wall reactions and the disproportionation reaction[Formula: see text]


1970 ◽  
Vol 48 (22) ◽  
pp. 3601-3604 ◽  
Author(s):  
S. H. Jones ◽  
E. Whittle

The reaction between CF3 radicals and ethylene oxide was studied in the range 60–228 °C using CF3I as a radical source. For the reactions,[Formula: see text]we obtain[Formula: see text]where θ = 2.3 RT kcal mole−1Published data of Phibbs and Darwent on the reaction[Formula: see text]have been re-calculated and it is suggested that both the original and re-calculated values of the activation energy E5 are too low. The Arrhenius parameters for the reactions of CF3 and CH3 radicals with ethylene oxide are compared with those for related reactions.


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