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Partial oxidation of methane to oxygenates by oxygen transfer at novel lattice oxygen sites of palladium and ruthenium bimetal oxide

Ming Zhao, Yang Song, Daiki Higashikubo, Masanaru Moriyama, Hiroyuki Imai, Kyoko Bando, Atsushi Takagaki, Xiaohong Li

Molecular catalysis(2022)

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摘要
Alumina-supported bimetal oxide (PdRuOx) catalysts were prepared by galvanic displacement reduction method for partial oxidation of methane into oxygenates, and evaluated in a fixed-bed reactor at relatively low temperatures of 280-310 ?, using a mixture of NO and O-2 as the oxidant. The bimetal oxide catalysts exhibited high selectivity to HCHO. However, CO2 was dominantly obtained over two alumina-supported monometal oxide (PdO and RuO2) catalysts. Characterizations results showed that bimetal oxide-PdRuOx species with Pd-(O)-Ru active sites can selectively convert CH4 to HCHO through the transfer of its novel lattice oxygen. And in this process, CH3OH may play as an intermediate. Compared to oxidation with either O-2 and NO, the mixture oxidant of NO and O-2, acting as an oxygen shuttle through the gas-phase reaction of NO+(1)/2 O2 -> NO2, promoted the selective formation of HCHO.
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关键词
Methane,Selective oxidation,Formaldehyde,Bimetal oxide catalyst,Galvanic displacement reduction
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