On the possibility of AgZSM-5 zeolite being a partial oxidation catalyst for methane.
A silver-ion-exchanged HZSM-5 zeolite sample (Ag(H)ZSM-5) evacuated at 573 K exhibited prominent catalytic behavior in the partial oxidation of CH(4) at temperatures above 573 K, exceeding the performance of Ag/SiO(2)Al(2)O(3) and Ag/SiO(2) catalysts. From the infrared (IR) and X-ray absorption fine structure (XAFS) spectra, as well as the dioxygen adsorption measurement, it was concluded that the simultaneous existence of Ag(+) ions and small clusters of Ag particles leads to the partial oxidation of methane. Taking the magnitude of the formation enthalpy (per oxygen atom) of Ag(2)O (DeltaH=26 kJ/mol) into consideration, we propose the interpretation that the dioxygen activated on small Ag metal clusters formed in ZSM-5 elaborates a surface oxide layer on small Ag clusters and the thus-formed species is simultaneously and easily decomposed at 573 K or above, and the oxygen activated in this way on the Ag metal spills over and can react with methane that has been activated by the Ag(+) ions exchanged in ZSM-5, resulting in the high catalytic activity of the Ag(H)ZSM-5 sample in the partial oxidation of methane. This interpretation is also well evidenced by XAFS and IR data. It is anticipated that this material has the potential to be a promising catalyst in the conversion of natural gas into higher value-added chemicals and fuels.
Kuroda
Yasushige
Y
Department of Fundamental Materials Science, Graduate School of Natural Science and Technology, Okayama University, Tsushima, Okayama 700-8530, Japan. kuroda@cc.okayama-u.ac.jp
Mori
Toshinori
T
Sugiyama
Hiroyuki
H
Uozumi
Yoshinori
Y
Ikeda
Katsuhiro
K
Itadani
Atsushi
A
Nagao
Mahiko
M