期刊
CATALYSIS LETTERS
卷 138, 期 1-2, 页码 14-22出版社
SPRINGER
DOI: 10.1007/s10562-010-0380-6
关键词
Methanol; Methane activation; Cu-ZSM-5; mu-Oxo dicopper cluster; UV-Vis spectroscopy; FT-IR with pivalonitrile and NO
资金
- ACTS-ASPECT [053.62.006]
A series of Cu-ZSM-5 zeolites was prepared by varying nature of the charge compensating cation, copper precursor, copper loading, and pH. The materials were tested for the oxidation of methane to methanol using oxygen. A linear relationship between the amount of methanol produced over Cu-ZSM-5 zeolites from methane and oxygen and a UV-Vis-NIR DRS charge transfer band at 22,700 cm(-1) is reported irrespective of the synthesis route used. The absolute intensity of the 22,700 cm(-1) band is always low, indicating a low number of active sites in the samples. In all studied Cu-ZSM-5 zeolites at least two copper species were present: (a) Cu-O clusters dispersed on the outer surface of ZSM-5 and (b) highly dispersed copper-oxo species inside the channels, a minority fraction in the sample. By relating catalytic activity to FT-IR data of adsorbed pivalonitrile, visualizing Cu-O particles on the outer surface of the zeolite, and subsequently adsorbed NO, indicative of the Cu-O species inside the zeolite channel, it was concluded that Cu-O species on the outer surface are not involved in the oxidation reaction, while copper inside the channels are responsible for the selective conversion of methane to methanol.
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