Laser powered homogeneous pyrolysis of ethyne, propyne, and propadiene initiated by methyl radicals: formation and degradation of hydrocarbons at 800–950 K
Literature Information
Karlheinz Hoyermann, Bettina Jürges
Applying laser heating by fast vibrational–translational energy transfer in a quasi-wall-free reactor the pyrolysis of ethyne (C2H2), propyne (p-C3H4), and propadiene (a-C3H4) was studied experimentally at 0.13 bar in the medium temperature range of 800–950 K with respect to the degradation and formation of hydrocarbons. The radical/hydrocarbon chemistry was chemically induced via CH3 radicals produced by the fast thermal dissociation of di-tert-butyl-peroxide DTBP ((tert-C4H9O)2 → 2 CH3 + 2 CH3COCH3). Complete analysis of the product yields was achieved by means of GC-MS with special attention to isomeric product and benzene formation. The product distribution, the temperature dependence and the underlying reaction schemes were analyzed by kinetic models developed for high temperature alkane oxidation/pyrolysis and aromatic formation in premixed ethene and ethyne flames. The primary attack of the unsaturated hydrocarbons by CH3 radicals in the studied temperature range occurs via the addition to the double/triple bond and via hydrogen atom abstraction, leading to different classes of radicals. For the reaction system C2H2 + CH3 high yields of C6H6 with a marked negative temperature dependence were observed. A semi-quantitative description of the C6H6 yield was obtained by a reaction sequence of successive addition of C2H2 to the radicals C2H3 (from C2H2 + H) and C4H5, being consistent with recent discussed reaction networks. For the reaction systems p-C3H4 + CH3 and a-C3H4 + CH3 only qualitative agreement between measured and modelled product yields was found, pointing to a lack of reliable data of the reactions of p-C3H4/a-C3H4/C3H3/H. Modified mechanisms are presented for the radical rich reaction systems C2H2 + CH3, p-C3H4 + CH3, and a-C3H4 + CH3 experimentally studied.
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Source Journal
Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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