Chemisorption study of hydrogen and methane by 1H MAS NMR and conversion of methane in the presence of ethylene on Ag-Y zeolite

被引:46
作者
Baba, T
Sawada, H
Takahashi, T
Abe, M
机构
[1] Tokyo Inst Technol, Grad Sch Sci & Engn, Dept Appl Chem, Meguro Ku, Tokyo 1528552, Japan
[2] Japan Energy Analyt Res Ctr Co Ltd, Toda, Saitama 3350026, Japan
关键词
H-1 MAS NMR; Ag-Y; hydrogen chemisorption; methane conversion; ethylene;
D O I
10.1016/S0926-860X(01)00904-8
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
H-1 MAS NMR showed that hydrogen dissociatively adsorbs on Ag-Y and generates acidic protons and silver-hydride species (Ag-n-H). The peak due to Ag-n-H was observed at -0.1 ppm together with peaks due to acidic protons in the supercages (3.9 ppm) and in the socialite cages (4.7 ppm). The hydrogen chemisorption on Ag-Y is reversible. Thus, the peaks at 3.9 and -0.1 ppm disappeared by evacuating the Ag-Y at 313 K, and the intensities of these peaks recovered by re-exposing the evacuated sample to hydrogen at 313 K. Adsorption of methane on Ag-Y at 423 K also gave rise to the peak due to Ag-n-H, indicating that heterolytic dissociation of CH4 proceeds on Ag-n-Y. ZO(-)Ag(n)(+) + CH4 --> Ag-n-H + ZO(delta-)CH(3)(delta+) The reaction of CH4 with C2H4 proceeded to give C3H6 on Ag-n-Y at 673 K. These results demonstrate that methane is easily activated on Ag-Y. (C) 2002 Elsevier Science B.V All rights reserved.
引用
收藏
页码:55 / 63
页数:9
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