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首页> 美国卫生研究院文献>Wiley-Blackwell Online Open >A Systematic Study of Isomorphically Substituted H‐MAlPO‐5 Materials for the Methanol‐to‐Hydrocarbons Reaction
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A Systematic Study of Isomorphically Substituted H‐MAlPO‐5 Materials for the Methanol‐to‐Hydrocarbons Reaction

机译：同构取代的H-MAlPO-5材料在甲醇制烃反应中的系统研究

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摘要

Substituting metals for either aluminum or phosphorus in crystalline, microporous aluminophosphates creates Brønsted acid sites, which are well known to catalyze several key reactions, including the methanol to hydrocarbons (MTH) reaction. In this work, we synthesized a series of metal‐substituted aluminophosphates with AFI topology that differed primarily in their acid strength and that spanned a predicted range from high Brønsted acidity (H‐MgAlPO‐5, H‐CoAlPO‐5, and H‐ZnAlPO‐5) to medium acidity (H‐SAPO‐5) and low acidity (H‐TiAlPO‐5 and H‐ZrAlPO‐5). The synthesis was aimed to produce materials with homogenous properties (e.g. morphology, crystallite size, acid‐site density, and surface area) to isolate the influence of metal substitution. This was verified by extensive characterization. The materials were tested in the MTH reaction at 450 °C by using dimethyl ether (DME) as feed. A clear activity difference was found, for which the predicted stronger acids converted DME significantly faster than the medium and weak Brønsted acidic materials. Furthermore, the stronger Brønsted acids (Mg, Co and Zn) produced more light alkenes than the weaker acids. The weaker acids, especially H‐SAPO‐5, produced more aromatics and alkanes, which indicates that the relative rates of competing reactions change upon decreasing the acid strength.
机译：用金属代替晶体或微孔铝磷酸盐中的铝或磷会产生布朗斯台德酸位点，众所周知，布朗斯台德酸位点可催化几个关键反应，包括甲醇制烃（MTH）反应。在这项工作中，我们合成了一系列具有AFI拓扑结构的金属取代的铝磷酸盐，其主要不同之处在于其酸强度，其分布范围从高布朗斯台德酸度（H‐MgAlPO‐5，H‐CoAlPO‐5和H‐ZnAlPO ‐5）到中等酸度（H‐SAPO‐5）和低酸度（H‐TiAlPO‐5和H‐ZrAlPO‐5）。该合成旨在生产具有均一特性（例如形态，微晶尺寸，酸位密度和表面积）的材料，以隔离金属取代的影响。广泛的特性验证了这一点。使用二甲醚（DME）作为进料，在450°C的MTH反应中测试了材料。发现了明显的活性差异，为此，所预测的强酸转化DME的速度明显快于中等和弱布朗斯台德酸性材料。此外，与弱酸相比，较强的布朗斯台德酸（Mg，Co和Zn）可生产更多的轻质烯烃。较弱的酸，尤其是H-SAPO-5，产生更多的芳烃和烷烃，这表明竞争反应的相对速率随酸强度的降低而变化。

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