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The photochemical removal of methane was investigated in N_2 or air using a head-on or side-on type 172 nm Xe_2 excimer lamp at atmospheric pressure. No photolysis of CH_4 was observed in N2 because C...H_4 does not absorb 172 nm photons. On the other hand, 34% of CH_4 (1000 ppm) was decomposed in air after 30 min photoirradiation using the head-on lamp. When the side-on type lamp with a larger irradiation area was used, the removal rate of CH_4 was increased by a factor of about 6. In the 172 nm photolysis of CH_4 in air, not only the O(^3P,^1D) + CH_4 reactions but also the O_3 + CH_4 reaction can take part in the initial oxidation of CH_4. The contribution of O(^1D) was examined by reducing the total pressure to suppress the collisional quenching of O(^1D) by the buffer N_2/O_2 gases. The contribution of O_3 was studied by observing the O_3 + CH_4 reaction. It was found that the O(^1D) + CH_4 reaction plays a major role in the initial stage of the oxidation of CH_4 under 172 nm VUV irradiation. Major oxidation pathways from CH_4 to CO_2 under 172 nm VUV photolysis in air are discussed.続きを見る
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