Isotope effect in gas-surface vibrational energy transfer

Wei, Yuan; Tosa, R.; Chao, Kai; Rabinovitch, B. S.

doi:10.1016/0009-2614(82)83454-4

Chemical Physics Letters

1982

DOI: 10.1016/0009-2614(82)83454-4

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Isotope effect in gas-surface vibrational energy transfer

Yuan Wei¹,

R. Tosa²,

Kai Chao³

et al.

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1984

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Cited by 7 publications

References 19 publications

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Gas/wall collision efficiencies in very low pressure pyrolysis experiments

Dick¹,

Gilbert²,

King³

1984

Int J of Chemical Kinetics

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A readily applicable empirical formula is obtained for the collisional efficiency for energy transfer between a highly vibrationally excited reactant and a seasoned (usually quartz) wall, in terms of the molecular weight, potential well depth and dipole moment of the reactant. This expression is used to examine corrections due to nonunit wall collision efficiency in the high-pressure rate parameters obtained from very low-pressure pyrolysis experiments. It is found that these corrections are up to ca. 2 5 kJ/mol in the high-pressure activation energy and a factor of ca. 2 in the high-pressure frequency factor, for molecules with molecular weight less than ca. 100 and where experiments are carried out at temperatures exceeding 1000 K.

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Gas/wall collision efficiencies in very low pressure pyrolysis experiments

Dick¹,

Gilbert²,

King³

1984

Int J of Chemical Kinetics

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High temperature collisional energy transfer in highly vibrationally excited molecules: Isotope effects in tert‐butyl chloride systems

Brown

King

Gilbert

1984

Int J of Chemical Kinetics

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The average downward collisional energy transfer (<ΔEdown>) is obtained for highly vibrationally excited tert‐butyl chloride, both undeuterated and per‐deuterated, with Kr, N2, CO2, and C2H4 bath gases, at ca. 760 K. Data are obtained using the technique of pressure‐dependent very low‐pressure pyrolysis. Reactant internal energies to which the data are sensitive are in the range 200–250 kJ mol−1. For C4H9Cl, the <ΔEdown> values (cm−1) are 255 (Kr), 265 (N2), 440 (CO2), and 585 (C2H4), and for C4D9Cl, 245 (N2), 370 (CO2), and 540 (C2H4). The uncertainties in these values are ca. 20% (40% for Kr); the uncertainties in the deuteration ratios are 10–15%. The value for Kr is in agreement with theoretical predictions of a biased random walk model for internal energy change in monatomic/substrate collisions. The effect of deuteration of <ΔEdown> is also in accord with that predicted by a modification of the theory. Extrapolated highpressure rate coefficients for the thermal decomposition of reactant are 1013.6 exp(‐187 kJ mol−1/RT) s−1 (C4H9Cl) and 1014.2 exp(−196 kJ mol−1/RT) s−1 (C4D9Cl), in accord with other studies and the expected isotope effect.

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Collisional energy transfer in the decomposition of 2-methyloxetane and 3-methyloxetane, II. Gas/wall collisions

Zalotai

Bérces

Márta

1990

React Kinet Catal Lett

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Isotope effect in gas-surface vibrational energy transfer

Cited by 7 publications

References 19 publications

Gas/wall collision efficiencies in very low pressure pyrolysis experiments

Gas/wall collision efficiencies in very low pressure pyrolysis experiments

High temperature collisional energy transfer in highly vibrationally excited molecules: Isotope effects in tert‐butyl chloride systems

Collisional energy transfer in the decomposition of 2-methyloxetane and 3-methyloxetane, II. Gas/wall collisions

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