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Effect of Noble Metals on the Strength of BrOnsted Acid Sites in Bifunctional Zeolites

机译:贵金属对双官能沸石强硬酸位点的影响

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摘要

1H magic angle spinning (MAS)NMR and FTIR spectroscopy with deuterated acetonitrile and pyridine as probe molecules, respectively, were used to study the strength of BrOnsted acid sites in Pt- and Ir-modified zeolites Y and Beta in comparison with the materials in their H,Na forms. For both types of zeolites, the following sequence of the acid strengths was found: zeolites in their H,Na form>Pt-modified zeolites>Ir-modified zeolites. As the 1HMASNMR signals of the bridging OH groups (Si(OH)Al) in the noble-metal-modified zeolites have the same spectroscopic properties as those observed in the materials in the H,Na forms, no direct influence of the noble metals on the nature of the hydroxyl protons or on the local structure of Si(OH)Al groups is expected. However, it is suggested that noble metals in these bifunctional zeolite catalysts are involved in charge transfer with neighboring framework atoms, which affects the mean framework electronegativity of the zeolites under study. This effect causes a variation of the acid strength of the Si(OH)Al groups similar to that observed for zeolites with different framework Al contents.
机译:1H魔法角纺(MAS)NMR和FTIR光谱分别与氘代乙腈和吡啶作为探针分子,用于研究PT-和IR-修饰的沸石Y和β中的正囊酸位点的强度与其中的材料相比h,na形式。对于两种类型的沸石,发现以下酸强度的顺序:其H中的沸石,Na形式> Pt-改性沸石> IR-改性沸石。作为贵金属改性沸石中的桥接OH基团的1HmasNMR信号(Si(OH)Al)具有与在H,Na形式中的材料中观察到的光谱性质相同的光谱性质,对贵金属没有直接影响预期羟基质子或羟基(OH)Al组局部结构的性质。然而,建议这些双官能沸石催化剂中的贵金属与相邻框架原子涉及电荷转移,这影响了研究的沸石的平均框架电负性。这种效果导致Si(OH)Al基团的酸强度的变化与具有不同框架Al含量的沸石观察到的Si(OH)Al基团的变化。

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