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进一步证明 MFI 中存在双 Cu+ 位,该位作为室温下 C2H6 吸附的高效位。

Further evidence for the existence of a dual-Cu+ site in MFI working as the efficient site for C2H6 adsorption at room temperature.

机构信息

Department of Chemistry, Graduate School of Natural Science and Technology, Okayama University, 3-1-1 Tsushima, Kita-ku, Okayama 700-8530, Japan.

出版信息

Langmuir. 2013 Aug 6;29(31):9727-33. doi: 10.1021/la4018568. Epub 2013 Jul 23.

Abstract

We have recently clarified the following point: a dual-type site, which is composed of a pair of monovalent copper ions (Cu(+)) formed in a copper-ion-exchanged MFI-type zeolite (CuMFI), functions as the active center for strong ethane (C2H6) adsorption even at room temperature rather than a single-type site composed of a Cu(+) ion. However, the character of the dual-Cu(+) site in a CuMFI is not yet fully understood. In this study, we have elucidated the nature of the active sites for C2H6 based on infrared (IR) and calorimetric data. On the basis of the results obtained, we came to the conclusion that the dual-Cu(+) site composed of Cu(+) ions giving the adsorption energy of 100 kJ mol(-1) and the absorption band at 2151 cm(-1) for carbon monoxide (used as a probe molecule) at room temperature functions as an adsorption site for C2H6. We also evaluated, for the first time, the interaction between the dual-Cu(+) site and C2H6 energetically, by the direct measurement of heat of adsorption. The value of 67 kJ mol(-1) that we recorded was higher than that for the single-Cu(+) site in this sample and also for other samples, such as NaMFI and HMFI.

摘要

我们最近澄清了以下观点

双位点由在铜离子交换的 MFI 型沸石(CuMFI)中形成的一对单价铜离子(Cu(+))组成,即使在室温下也作为强乙烷(C2H6)吸附的活性中心,而不是由单个 Cu(+)离子组成的单一位点。然而,CuMFI 中的双 Cu(+)位点的性质尚未完全理解。在这项研究中,我们根据红外(IR)和量热数据阐明了 C2H6 的活性位性质。基于所获得的结果,我们得出结论,由在室温下给出 100 kJ mol(-1)的吸附能和在 2151 cm(-1)处的一氧化碳(用作探针分子)吸收带的 Cu(+)离子组成的双 Cu(+)位点作为 C2H6 的吸附位点。我们还首次通过直接测量吸附热对双 Cu(+)位点与 C2H6 之间的相互作用进行了能量评估。我们记录的值 67 kJ mol(-1)高于该样品中的单个 Cu(+)位点的值,也高于其他样品,如 NaMFI 和 HMFI。

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