TY - JOUR
T1 - Partial oxidation of methane to oxygenates by oxygen transfer at novel lattice oxygen sites of palladium and ruthenium bimetal oxide
AU - Zhao, Ming
AU - Song, Yang
AU - Higashikubo, Daiki
AU - Moriyama, Masanaru
AU - Imai, Hiroyuki
AU - Bando, Kyoko
AU - Takagaki, Atsushi
AU - Li, Xiaohong
N1 - Funding Information:
This work was supported by the under the CREST program, Grant Number JPMJCR16P2. The XAFS measurements were performed under the approval of the Photon Factory Program Advisory Committee (Proposal Nos. 2020G039, 2019G070 and 2017G083). We also acknowledge the collaboration of Mr. Akira Takatsuki (TIA-AIST) for the TEM analysis.
Publisher Copyright:
© 2022
PY - 2022/8
Y1 - 2022/8
N2 - 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 °C, using a mixture of NO and O2 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 O2 and NO, the mixture oxidant of NO and O2, acting as an oxygen shuttle through the gas-phase reaction of NO+1/2 O2→NO2, promoted the selective formation of HCHO.
AB - 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 °C, using a mixture of NO and O2 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 O2 and NO, the mixture oxidant of NO and O2, 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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U2 - 10.1016/j.mcat.2022.112449
DO - 10.1016/j.mcat.2022.112449
M3 - Article
AN - SCOPUS:85133293469
SN - 2468-8231
VL - 528
JO - Molecular Catalysis
JF - Molecular Catalysis
M1 - 112449
ER -