Potential for C-H Activation in CH4 Utilizing a CuMFI-Type Zeolite as a Catalyst
Potential for C-H Activation in CH4 Utilizing a CuMFI-Type Zeolite as a Catalyst
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DOI：
10.1021/jp807008t
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发表时间：
2009-04
影响因子：
3.7
通讯作者：
Atsushi Itadani;H. Sugiyama;Masashi Tanaka;T. Ohkubo;T. Yumura;Hisayoshi Kobayashi;Y. Kuroda
中科院分区：
文献类型：
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作者：
Atsushi Itadani;H. Sugiyama;Masashi Tanaka;T. Ohkubo;T. Yumura;Hisayoshi Kobayashi;Y. Kuroda
我们发现，铜离子交换MFI(Mobil Five)型分子筛的离子交换容量为112%(CuMFI-112)，即使在室温下也表现出与CH4的特异性相互作用。与钠离子交换MFI的吸附量、与MFI中钠离子的相互作用以及其他类型的铜离子交换沸石的吸附量相比，所观察到的性质是非常显著的。铜离子在MFI中的特异性是显而易见的。该体系最显著的特征是在300K下吸附甲烷后，在2661和2619 cm−-1处出现明显的红外吸收峰，以及300K下吸附甲烷前后CuMFI的X射线吸收精细结构谱的变化，表明该体系中存在实质性和特异性的相互作用。在密度泛函理论的基础上，利用由CuMF10元环组成的Cu−AlSi91O151H66团簇模型进行了计算。
We have found that a copper ion-exchanged MFI (Mobil Five)-type zeolite, having an ion exchange capacity of 112% (CuMFI-112), exhibits a specific interaction with CH4, even at room temperature. The observed properties are very remarkable compared with those found in the adsorbed amount of sodium ion-exchanged MFI and in the interaction with the sodium ion in MFI as well as in the adsorbed amounts for other types of copper ion-exchanged zeolites. The specificity of Cu+ in MFI is clearly evident. The most remarkable feature of the present system is the distinct appearance of infrared bands (IR) at 2661 and 2619 cm−1 due to adsorbed CH4 at 300 K and the change in the X-ray absorption fine structure spectra of CuMFI before and after CH4 adsorption at 300 K, indicating the existence of substantial and specific interaction in this system. In addition, calculations based on the density functional theory were carried out by utilizing a Cu−AlSi91O151H66 cluster model, which is made up of a 10-membered ring of CuMF...