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H + CH{sub 2}CO {yields} CH{sub 3} + CO at high temperature : a high pressure chemical activation reaction with positive barrier.

Conference ·
OSTI ID:8910

The Laser Photolysis-Shock Tube (LP-ST) technique coupled with H-atom atomic resonance absorption spectrometry (ARAS) has been used to study reaction, H + CH{sub 2}CO {r_arrow} CH{sub 3} + CO, over the temperature range, 863-1400 K. The results can be represented by the Arrhenius expression, k = (4.85 {+-} 0.70) x 10{sup {minus}11} exp({minus}2328 {+-} 155 K/T) cm{sup 3} molecule{sup {minus}1} s{sup {minus}1}. The present data have been combined with the earlier low temperature flash photolysis-resonance fluorescence measurements to yield a joint three parameter expression, k = 5.44 x 10{sup {minus}14} T{sup 0.8513} exp({minus}1429 K/T) cm{sup 3} molecule{sup {minus}1} s{sup {minus}1}. This is a chemical activation process that proceeds through vibrationally excited acetyl radicals. However, due to the presence of a low lying forward dissociation channel to CH{sub 3} + CO, the present results refer to the high pressure limiting rate constants. Hence, transition state theory with Eckart tunneling is used to explain the data.

Research Organization:
Argonne National Lab., IL (US)
Sponsoring Organization:
US Department of Energy (US)
DOE Contract Number:
W-31109-ENG-38
OSTI ID:
8910
Report Number(s):
ANL/CHM/CP-95085
Country of Publication:
United States
Language:
English