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FTIR study of the relation, between extra-framework aluminum species and the adsorbed molecular water, and its effect on the acidity in ZSM-5 steamed zeolite

机译:FTIR研究骨架外铝物种与吸附的分子水之间的关系,及其对ZSM-5蒸汽沸石中酸度的影响

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The infrared spectroscopy study of zeolite samples, obtained by steam treatment at 560‑960 °C of the ZSM‑5 catalyst (framework Si/Al ratio of 13), suggests an association between adsorbed molecular water and extra‑framework aluminum hydroxyls generated after treatment. Moreover, infrared spectroscopy of adsorbed pyridine shows the reduction of the densities of Br?nsted and Lewis sites, when treatment temperature rises, with contradicts the frequently accepted mechanism of the transformation of two bridged Si‑OH‑Al groups for each Lewis site generated. The gradual conversion of the octahedral extra-framework aluminum (Lewis‑associated) in polymeric species with low acidity is the most probable cause of this behavior. On the other hand, the apparent decline of the acid Br?nsted strength, with the increase in the temperature of the hydrothermal treatment, has two possible causes: a) the decreasing accessibility, of the pyridine molecular probe to bridged Si-OH-Al groups with the strongest Br?nsted acidity, inside the channels, and b) the gradual transformation of these groups into extra framework species of weak acidity.
机译:沸石样品的红外光谱研究是在560‑960°C的ZSM‑5催化剂(骨架Si / Al之比为13)下通过蒸汽处理获得的,表明吸附的分子水与处理后产生的骨架外铝羟基之间的关联。此外,吸附吡啶的红外光谱显示,当处理温度升高时,布朗斯台德和路易斯位点的密度降低,这与通常为每个路易斯位点产生的两个桥连的Si-OH-Al基团的转化机理相反。低酸度的聚合物中八面体骨架外铝(刘易斯缔合)的逐渐转化是这种现象的最可能原因。另一方面,随着水热处理温度的升高,酸布朗斯台德强度的明显下降有两个可能的原因:a)吡啶分子探针与桥连的Si-OH-Al的可及性降低。通道内部具有最强布朗斯台德酸度的基团; b)这些基团逐渐转变为弱酸度的额外骨架物种。

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