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For investigating the pyrolysis of 1,3-butadiene (1,3-C 4 H 6 ) and 2-butyne (2-C 4 H 6 ), reactive gas mixtures highly diluted with argon as bath gas were prepared. The experiments were carried out in a high purityshock tube device over a temperature range of about 1500–1800 K at total pressures between 1.2 and 1.9 bar. The time-dependentformation of H-atoms was measured behind reflected shock waves by using the very sensitive method of atomic resonance absorptionspectrometry (ARAS). A detailed chemical kinetic reaction mechanism consisting of 33 elementary reactions and 26 species wasused to model the experimentally obtained H-atom profiles. From kinetic modelling, with help of sensitivity and reaction fluxanalysis, it was concluded that reaction R 1 2-C 4 H 6  ↔ 2-C 4 H 5  + H is crucial for the observed formation of H-atoms during the thermal decomposition of both investigated species and withinthe investigated range of temperatures and pressures. Moreover, at temperatures above about 1650 K, the decay of propargylradicals (C 3 H 3 ) turns out to contribute significantly to the amount of produced H-atoms. The following rate expressions were obtained forthree reactions (R 1–R 3) – among them the isomerisation from 2-butyne to 1,3-butadiene – important with respect to the formationof H-atoms within the investigated parameter range. The uncertainties are estimated to be ±30%:

Formation of H-atoms in the Pyrolysis of 1,3-butadiene and 2-butyne: A Shock Tube and Modelling Study