Abstract
A critical analysis of a recent paper by Robertson, Hils and Gallagher (RHG) on the mechanism of the thermal pyrolysis of silane is presented, with special attention to the nature of the initiation reaction and subsequent gas phase reactions. It is argued that exclusive initiation at the walls, as proposed by RHG is indeed the major mode of initiation at total reaction pressures below 1 Torr. However, homogeneous gas phase initiation via the pressure-dependent unimolecular reaction SiH 4 → SiH 2 + H 2 dominates at total reaction pressures above 100 Torr. Subsequent gas phase reactions are non-chain processes involving silylene and silene intermediates. Free radical chain reactions, as proposed by RHG, are not involved.
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