メタンを還元剤とするNOx選択還元反応用Pd-Pt/硫酸化ジルコニア触媒の開発(<総説特集>実用化されつつある天然ガス利用プロセスの最前線)
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The deactivation of Pd ion-exchanged zeolite in the selective catalytic reduction of nitrogen oxides by methane was investigated. The deactivation was significantly promoted by the presence of water vapor. Characterization of deactivated catalysts by Raman spectroscopy, in situ infrared absorption spectroscopy, etc. proved that the agglomeration of dispersed Pd cations forming PdO was the principal cause of the deactivation. To simulate an actual combustion exhaust, a catalytic test was carried out in the presence of water vapor and sulfur dioxide. The result showed that only a trace amount of sulfur dioxide (3 ppm) almost completely deactivated the catalyst within several ten hours. Based on these results, employing sulfated zirconia (SZ), which possesses a strong solid acidity like zeolite, as a support, Pd-Pt/SZ, which is a novel catalyst, has been developed. On this catalyst, sulfur dioxide stabilized the activity. Comparison of activity in NO-CH_4-O_2, NO_2-CH_4-O_2, NO-O_2, NO_2-O_2, and CH_4-O_2 reactions showed that Pt catalyzed the oxidation of NO to NO_2 and Pd catalyzed the reaction of NO_2 with methane over the catalyst. The catalyst showed slow deactivation, but the addition of Fe to SZ significantly suppressed the deactivation. The promoted catalyst, Pd-Pt/Fe-SZ, maintained a NO_x conversion of practically applicable level (>70%) for more than 2000 h even in the presence of water vapor and sulfur dioxide.
- 一般社団法人日本エネルギー学会の論文
- 2007-04-20
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