Kinetic studies were carried out for the gas-phase reaction ND(a1 Δ) + H2 → products (1) at room temperature (T = 300 K) at total pressure of 10 Torr in a flow reactor using pulsed laser photolysis of DNCO at a wavelength of 193 nm to generate ND(a 1 Δ) reagents in combination with time-resolved pulsed-vacuum-ultraviolet-laser-induced fluorescence spectroscopy for H and D atom product detection. From a pseudo-first-order analysis of the formation rate of H and D atom reaction products, a rate constant k1 = (3.8 ± 0.3) × 10−1212 cm3 molecule−1 s−1 has been determined. For the H and D atom producing reaction channels ND(a1 Δ) + H2 → NDH + H (2) and ND(a1 Δ) + H2 → NH2 + D (3) the product branching ratios ΓH = k2/k1 = 0.84 ± 0.06 and ΓD = k3/k1 = 0.16 ± 0.06 could be obtained. In addition, the primary quantum yield for D atom formation in the 193 nm DNCO photolysis could be determined to be φD (193 nm) = 0.24 ± 0.03.
Research on Chemical Intermediates – Springer Journals
Published: Jan 1, 2005
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