Preparation of Ru-Sn/Y Zeolite Catalysts with Various Precursors and Their Application to Acetic Acid (Methyl Acetate) Formation from Methanol Alone
Naoki MIMURA†, Satomi OGUNI††, Tetsu YAMAKAWA* and Sumio SHINODA
Institute of Industrial Science, The University of Tokyo; 4-6-1, Komaba, Meguro-ku, Tokyo 153-8505 Japan
† Present address National Institute of Advanced Industrial Science and Technology (AIST); Tsukuba West, Tsukuba-shi 305-8569 Japan
†† Present address Automotive Coatings Technical Center, PPG Japan Ltd.; 1-11 Aza-Nakayama, Oaza Hagi, Otowa-cho, Hoi-gun, Aichi 441-0201 Japan
New preparation methods for Ru-Sn/Y zeolites, which catalyze acetic acid (methyl acetate) formation from methanol alone in the gas-solid phase, were investigated. When SnX2 (X=Cl, Br, I) was impregnated on a [Ru (NH3)6]3+/Y zeolite from the methanol solution at the ratio of [Sn]/[Ru]=1.0, the higher activity was obtained with X possessing the higher electronegativity (Cl>Br>I). The larger methyl acetate formation was observed by using a Ru precursor with chloride ligands, [RuCl2(NH3)4]+, and SnCl2. Introducing SnCl2 as a vapor afforded 14 and 10 times smaller amounts of Sn species on the [Ru (NH3)6]3+/Y and [RuCl2(NH3)4]+/Y, respectively. Nevertheless, the activities were almost the same for the former (3.1%→2.9%) and somewhat increased for the latter (6.2%→8.4%), suggesting the formation of more active species.
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