Autor: |
Giesen, Andreas, Herzler, Jürgen, Roth, Paul |
Zdroj: |
Physical Chemistry Chemical Physics (PCCP); July 19, 2002, Vol. 4 Issue: 15 p3665-3668, 4p |
Abstrakt: |
The reaction of Fe-atoms with CO2 was studied in the temperature range of 1330 K T 2650 K at pressures between 1.0 and 1.6 bar in a shock wave reactor. Resonance absorption spectroscopy was applied for time-resolved measurement of Fe-atoms, O-atoms, and CO-molecules in initial gas mixtures containing Fe(CO)5 and CO2, highly diluted in argon. The experiments showed at early reaction time an Fe-consumption and a simultaneous CO formation which was interpreted by reaction R2 (explained below): The rate coefficient was determined to be k2 = 1014.51 ± 0.10 exp(−15 000 ± 400 K/T) cm3 mol−1 s−1. At higher temperatures and longer reaction times a quasi stationary Fe-atom concentration level was observed which could not be explained by (R2) only. Therefore secondary reactions were considered in a simplified reaction mechanism, enabling the simulation of the complete Fe, O, and CO concentration profiles. For the major secondary reaction (R3, explained below): a rate coefficient of k3 = 1015.59 ± 0.46 exp(−23 000 ± 1700 K/T) cm3 mol−1 s−1 was determined, which is regarded more like a fitting parameter than an elementary reaction. |
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