Stepwise Methane-to-Methanol Conversion on CuO/SBA-15

被引:42
作者
Le, Ha V. [1 ]
Parishan, Samira [2 ]
Sagaltchik, Anton [3 ]
Ahi, Hamideh [3 ,4 ]
Trunschke, Annette [4 ]
Schomaecker, Reinhard [2 ]
Thomas, Arne [1 ]
机构
[1] Tech Univ Berlin, Inst Chem Funct Mat, BA2,Hardenbergstr 40, D-10623 Berlin, Germany
[2] Tech Univ Berlin, Inst Chem Tech Chem, TC8,Str 17 Juni 124, D-10623 Berlin, Germany
[3] Tech Univ Berlin, BasCat UniCat BASF Joint Lab, EW K 01,Hardenbergstr 36, D-10623 Berlin, Germany
[4] Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany
关键词
copper; heterogeneous catalysis; mesoporous materials; oxidation; supported catalysts; ACTIVE-SITE; EXCHANGED ZEOLITES; COPPER; OXIDATION; CLUSTERS; OXIDE; MORDENITE; CU-ZSM-5; OXYGEN; ZSM-5;
D O I
10.1002/chem.201801135
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The direct partial oxidation of methane to methanol is a challenging scientific and economical objective to expand the application of this abundant fuel gas as a major resource for one-step production of value-added chemicals. Despite substantial efforts to commercialize this synthetic route, to date no heterogeneous catalyst can selectively oxidize methane to methanol by O-2 with an economically acceptable conversion. Cu-exchanged zeolites have been recently highlighted as one of the most promising bioinspired catalysts toward the direct production of methanol from methane under mild conditions. In this work, Cu-based catalysts were prepared using mesoporous silica SBA-15 as an alternative support and their activity for this conversion was investigated. The results demonstrate that highly dispersed CuO species on SBA-15 are able to react with methane and subsequently produce methanol with high selectivity (>84%) through water-assisted extraction. Furthermore, it was confirmed that the main intermediate formed after interaction of the catalyst with methane is a methoxyl species, which can be further converted to methanol or dimethyl ether on extraction with water or methanol, respectively.
引用
收藏
页码:12592 / 12599
页数:8
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