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Identifier 000348356
Title Κινητική μελέτη της αντίδρασης των ατόμων Cl με οξικό οξύ στην αέρια φάση
Alternative Title Kinetic Study for the Gas Phase Reaction of Cl Atoms with Acetic Acid
Author Λάζος, Βαγγέλης Π.
Thesis advisor Παπαγιαννακόπουλος, Πάνος
Abstract In the present work, the reaction of chlorine atoms (Cl) with acetic acid (CH3C(O)OH) was investigated in the gas phase by using two independent experimental setups. In particular, the rate coefficient of the title reaction was determined as a function of pressure (P: 2×10-3 – 700 Torr) and temperature (T: 263 – 363 K). The continuous flow system of Very Low Pressure Reactor coupled with quadrupole mass spectrometry detection technique (VLPR-QMS, absolute rate coefficient determination) was employed in order to measure rate coefficients at the zero pressure limits (≈ 2 mTorr). In addition, the static system of Thermostated PhotoChemical Reactor equipped with Fourier Transformed Infrared spectroscopy for chemical mixtures analysis (TPCR-FT/IR, relative rate coefficient determination) was used at higher total pressures. Relative rate measurements performed in the presence of Nitrogen (N2), as a bath gas and excess of oxygen (O2), in order to suppress secondary chemistry complications originated by the primarily produced alkylradicals. The experimental results showed, that reaction rate coefficients are independent of pressure, and are very well represented by the Arrhenius expression, k(T)= (2.74±0.26)×10-12 exp(-1395±209/T) cm3 molecule-1 s-1, k(T=298 K)= (2.18±0.20)×10-14 cm3 molecule-1 s-1 . The quoted uncertainties are at 95% confidence level (2σ) and include systematic uncertainties. Final product analysis showed HCl formation in both experimental techniques used. The last observation combined with the non-pressure dependent rate coefficients measured in this work and their well representation by an Arrhenius expression provide with evidence that the reaction mechanism proceed via direct hydrogen abstraction. Finally, the difference in the reaction mechanism of acetic acid with Cl atoms and OH radicals was investigated, as well as the reactivity inversion of acetic acid towards the major atmospheric oxidants (ΟΗ and Cl), compared to majority of Volatile Organic Compounds, are discussed.
Language Greek
Subject Acetic Acid
Atmospheric Oxidation
Chlorine Reactivity
Gas Phase Chemistry
IR Spectroscopy
Kinetic Techniques
Mass Spectrometry
Pressure Dependence
Rate Coefficients
TPCR/FT-IR
Temperature Dependence
Tropsphere
VLPR/QMS
Ατμοσφαιρική οξείδωση
Εξάρτηση από τη θερμοκρασία
Εξάρτηση από την πίεση
Κινητικές τεχνικές
Οξικό οξύ
Οξύτητα ατόμων χλωρίου
Συντελεστές ταχύτητας
Φασματομετρία μάζας
Φασματοσκοπία υπερύθρου
Χημεία αέριας φάσης
Issue date 2009-06-30
Collection   School/Department--School of Sciences and Engineering--Department of Chemistry--Post-graduate theses
  Type of Work--Post-graduate theses
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