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Symposium (International) on Combustion | 1988

Rate constant for the reaction of O(3P) with H2 by the flash photolysis—shock tube and flash photolysis—resonance fluorescence techniques; 504K≤T≤2495K

J. W. Sutherland; Joe V. Michael; A.N. Pirraglia; F.L. Nesbitt; R. B. Klemm

The rate constant for the reaction, O ( P 3 ) + H 2 → O H + H , ( 1 ) was measured over the temperature range of 504K to 2495 K by two independent experimental methods. The flash photolysis-shock tube (FP-ST) technique, combined with atomic resonance absorption spectroscopy (ARAS), was used over the temperature range 880K to 2495K. The results from the FP-ST work, expressed in simple Arrhenius form, are: k 1 ( T ) = ( 3.1 ± 0.2 ) × 10 − 10 exp ⁡ ( − 13620 ± 170 / R T ) c m 3 molecule − 1 s − 1 , where the units of R in this and succeeding expressions are cal mole −1 K −1 . The flash photolysis-resonance fluorescence (FP-RF) technique was utilized to measure rate constants from 504K to 923K. Results from the FP-RF experiments, also expressed in simple Arrhenius form, are: k 1 ( T ) = ( 7.2 ± 0.4 ) × 10 − 11 exp ⁡ ( − 10430 ± 70 / R T ) c m 3 molecule − 1 s − 1 . These kinetic results for the reaction of O( 3 P) with H 2 exhibit non-Arrhenius behavior. This conclusion is confirmed by the recent kinetic data of Presser and Gordon (297K≤T≤471K). The combined results from these three data sets are expressed by the three parameter fit: k 1 ( T ) = 8.4 × 10 − 20 T 2.67 exp ⁡ ( − 6290 / R T ) c m 3 molecule − 1 s − 1 . The estimated error in this expression is about ±30% over the entire temperature range, 297K to 2495K. Rate constants for reaction (1) from recent ab initio calculations are in excellent agreement with these experimental results.


Journal of Chemical Physics | 1988

The kinetics and thermodynamics of the reaction H+NH3⇄NH2+H2 by the flash photolysis–shock tube technique: Determination of the equilibrium constant, the rate constant for the back reaction, and the enthalpy of formation of the amidogen radical

J. W. Sutherland; Joe V. Michael

Equilibrium constants K1 for the reaction H+NH3⇄NH2+H2 were measured over the temperature range 900 to 1600 K using a flash photolysis–shock tube apparatus. The experimental values of K1 ranged from 1.0 at 900 K to 2.2 at 1620 K with an estimated experimental error of about ±10%. The value obtained from the third law analysis for the enthalpy of formation of the amidogen radical, ΔH0f298 (NH2), is 45.3 kcal/mol (ΔH0f0 =46.0). The corresponding value for the bond dissociation energy, D0(NH2–H), is 107 kcal/mol. These values are in good agreement with the data tabulated in the revised JANAF tables (1982), with those derived from new measurements of the photoionization threshold for the amidogen radical, and with those from independent measurements of the rate constants of the forward and back reactions. The Arrhenius rate expression derived for reaction (−1), NH2+H2→NH3+H, is k−1(T)=5.38×10−11 exp(−6492/T) cm3 molecule−1 s−1 for the temperature range 900–1620 K. The estimated error in k−1(T) is about ±25%.


Symposium (International) on Combustion | 1991

Rate constants for the reaction, O(3P)+H2O¶OH+OH, over the temperature range 1053 K to 2033 K using two direct techniques

J. W. Sutherland; Patricia M. Patterson; R. Bruce Klemm

The rate constant for the reaction of O( 3 P) with H 2 O (reaction (1)) was measured over the temperature range 1288 K≤T≤2033 K using the flash photolysis-shock tube technique and at 1053, 1090 and 1123 K using the flash photolysis-resonance fluorescence method. The photolytic source for O( 3 P) atoms was nitric oxide. The results were given by the Arrhenius expression: k 1 (T)=(9.2±0.9)×10 −11 exp(−19100±300 cal mol −1 /RT) cm 3 molecule −1 s −1 The present results were equally well fit to the three parameter expression: k 1 (T)=4.93×10 −18 T 2.02 exp(−13400 cal mol −1 /RT) cm 3 molecule −1 s −1 . Uncertainties in the Arrhenius expressions are given at the one standard deviation level and the mean deviation of the data from each expression is ±16%. Corresponding rate constants for the reverse reaction (reaction (−1)) were computed from the known values of the equilibrium constant and were fitted to the Arrhenius equation: k −1 (T)=(8.9±0.9)×10 −12 exp(−2100±300 cal mol −1 /RT) cm 3 molecule −1 s −1 . These direct experimental results for k −1 (T) and k 1 (T) are compared with previously reported experimental measurements and with available theoretical expressions.


Journal of Chemical Physics | 1979

Aerosol formation on the flash photolysis of SO2/gas mixturesa)

Laurence D. Fogel; J. W. Sutherland

A long‐lived transient absorption observed on the flash photolysis of SO2/gas mixtures at λ?190 nm has been identified as resulting from light scattering by H2SO4 aerosols. No detectable signals were monitored on photolysis at λ?270 nm, indicating that the aerosol precursors originated from the promotion of SO2 into its second singlet level and into its dissociation continuum. The SO3 that was formed was hydrated immediately to yield H2SO4 vapor in a highly supersaturated state and heteromolecular homogeneous nucleation to produce H2SO4 aerosols ensued. This nucleation was quenched rapidly as the acid vapor was consumed by further nucleation, by condensation, and by vapor diffusion to the cell walls. A model was formulated in which the condensations of the H2SO4 and the H2O vapors on the growing droplets were considered kinetically negligible and the particles grew by coagulation; simultaneously, they were lost by tranquil gravitational settling and by diffusion to the cell walls. Computer simulations dem...


Current topics in shock waves 17th international symposium on shock waves and shock tubes | 2008

High temperature study of the reaction of O(3P)+NH3

Patricia M. Patterson; J. W. Sutherland; R. B. Klemm

Values of the rate constant for the reaction O(3P)+NH3 were determined by compring calculated O atom profiles with those obtained experimentally in the temperature range 2069‐2459K. Oxygen atoms were generated by thermal decomposition of N2O. The results were combined with those from previous direct studies (448‐1790K) to given the following expression 448‐2459K:     k2(T)=2.27×10−18 T2.19 exp(−3061/T) cm3 molecule−1 s−1 An overall uncertainty of ±25% is estimated for this expression.


The Journal of Physical Chemistry | 1989

A flash photolysis-shock tube kinetic study of the H atom reaction with O sub 2 : H + O sub 2 rightleftharpoons OH + O (962 K le T le 1705 K) and H + O sub 2 + Ar yields HO sub 2 + Ar (746 K le T le 987 K)

A.N. Pirraglia; J. V. Michael; J. W. Sutherland; R. B. Klemm


The Journal of Physical Chemistry | 1991

Direct rate constant measurements for atomic hydrogen + methane .fwdarw. methyl + hydrogen, 897-1729 K, using the flash photolysis-shock tube technique

M. J. Rabinowitz; J. W. Sutherland; Patricia M. Patterson; R. B. Klemm


The Journal of Physical Chemistry | 1986

Rate constant for the reaction, atomic hydrogen + ammonia, over the temperature range, 750-1777 K

J. V. Michael; J. W. Sutherland; R. B. Klemm


The Journal of Physical Chemistry | 1986

Rate constant for the O(3P) + CH4 .fwdarw. OH + CH3 reaction obtained by the flash photolysis-shock tube technique over the temperature range 760 .ltoreq. T .ltoreq. 1760 K

J. W. Sutherland; J. V. Michael; R. B. Klemm


Journal of Physical Chemistry A | 1997

Rate Constants for the Thermal Dissociation of N2O and the O(3P) + N2O Reaction

Stuart K. Ross; J. W. Sutherland; Szu-Cherng Kuo; R. Bruce Klemm

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R. B. Klemm

Brookhaven National Laboratory

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Patricia M. Patterson

Brookhaven National Laboratory

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M. J. Rabinowitz

Brookhaven National Laboratory

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R. Bruce Klemm

Brookhaven National Laboratory

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Joe V. Michael

Brookhaven National Laboratory

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A.N. Pirraglia

Brookhaven National Laboratory

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F.L. Nesbitt

Brookhaven National Laboratory

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Laurence D. Fogel

Brookhaven National Laboratory

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Szu-Cherng Kuo

Brookhaven National Laboratory

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