Copper-zeolites Prepared by Solid-state Ion Exchange-Characterization and Evaluation for the Direct Conversion of Methane to Methanol

被引:6
|
作者
Kvande, Karoline [1 ]
Prodinger, Sebastian [1 ]
Schlimpen, Fabian [2 ]
Beato, Pablo [3 ]
Pale, Patrick [2 ]
Chassaing, Stefan [2 ]
Svelle, Stian [1 ]
机构
[1] Univ Oslo, Ctr Mat Sci & Nanotechnol SMN, Dept Chem, Blindern 1033, N-0315 Oslo, Norway
[2] Univ Strasbourg, Inst Chim, Lab Synth React Organ & Catalyse LASYROC, CNRS,UMR 7177, 4 rue Blaise Pascal, F-67070 Strasbourg, France
[3] Topsoe AS, Haldor Topsoes 1, DK-2800 Lyngby, Denmark
关键词
Methane activation; Solid-state ion exchange; Cu-I; -zeolites; TO-METHANOL; GREEN CATALYSTS; OXIDATION; REDUCTION; CU-ZSM-5; STABILITY; CORE; XAS;
D O I
10.1007/s11244-022-01763-7
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Direct conversion of methane to methanol (MTM) over Cu-zeolites is a so-called "dream reaction " for the chemical industry. There is still a lot that can be done in order to optimize the reaction by e.g. achieving a deeper understanding of the reaction mechanism and the nature of the Cu-sites. In this study, we investigated a solid-state ion exchange method to incorporate Cu-I ions into zeolites (MOR, BEA, ZSM-5 and FAU), as a more scalable technique. The solid-state ion exchange led to a Cu/Al ration of about 0.8, however with a heterogeneous distribution of Cu. Regardless, Fourier transform-infrared spectroscopy still revealed that most Bronsted acid sites were exchanged in all four samples. Further, CH4-temperature programmed reaction experiments showed that some Cu-sites formed were reactive towards CH4, with Cu-I-MOR and Cu-I-FAU having the largest CH4 consumption. Ultimately, the Cu-I-zeolites were tested in the MTM reaction and proved capable of producing methanol, even without the presence of Bronsted sites. A MOR with lower Cu/Al ratio (0.30) was also tested for comparison, and as this sample obtained a much higher productivity than the Cu-I-MOR with high Cu-loading (0.10 vs. 0.03 mol(MeOH)/mol(Cu)), it was demonstrated that some fine-tuning is necessary to obtain the active Cu sites for methane activation.
引用
收藏
页码:1406 / 1417
页数:12
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