Journal of Physical Chemistry p. 4772 - 4776 (1982)
Update date:2022-08-25
Topics:
Arakawa, R.
Rabinovitch, B. S.
The reaction probability per collision, Pc, for 1-methylcyclobutene activated at a hot seasoned fused silica surface has been measured under single collision conditions over the reactor temperature range Tr = 480-800 K.The initial thermal vibrational energy population distribution of the cyclobutene molecules was varied from Tc = 273 K to Tc 570 K.The reaction is isomerization to isoprene.Mixed samples of 1-methylcyclobutene and cyclobutene (which had been studied earlier) were used for internal comparison under the same conditions.These experiments provide a test of the relative suitability of various analytical forms for the collisional transition probability matrix P.Stochastic calculations with a Gaussian form provide the best overall fit to the data.The calculated average amount of energy (<ΔE'>E0) transferred from the hot molecules in a vibrational down transition from the reaction threshold energy level, E0, declined from 7220 to 3890 cm-1 with increase in surface temperature from 600 to 800 K.The experimental collisional efficiency, β1, declined from 0.39 to 0.035 over the combination temperature range Tr,Tc = 600,500 to 800,293.Strong collider behavior was observed with both 1-methylcyclobutene and cyclobutene for Tr less than 450 K.
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