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Microporous crystalline silicoaluminophosphates: Effect of synthesis conditions on the physicochemical and catalytic properties in the reaction of methanol to C-2-C-4 olefins conversion

机译:微孔晶体硅铝磷酸盐:合成条件对甲醇转化为C-2-C-4烯烃的反应中物理化学和催化性能的影响

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摘要

Effect of the synthesis parameters (reaction mixture composition, crystallization temperature and duration) on the physicochemical and catalytic properties of microporous crystalline silicoaluminophosphates (SAPOs) has been studied. Methods for the directional control of phase composition, degree of crystallinity, morphology and size of SAPO crystals crystallized from colloidal silicoaluminophosphate sols stabilized in tetraethylammoniun hydroxide solution as a template have been developed. It has been determined that the use of more severe synthesis conditions (increase in temperature and duration of crystallization) leads to the formation of larger crystals and a growth in the concentration of medium strength sites in the samples, which causes a rapid deactivation of the samples in the reaction of methanol conversion to C-2-C-4 olefins. Crystallization under milder conditions (a decrease in pH and temperature) promotes the acid formation of CHA/AEI intergrowth crystals exhibited a high and steady performance in the methanol conversion for more than 8 h at a total yield of olefins of 95 wt %.
机译:研究了合成参数(反应混合物组成,结晶温度和持续时间)对微孔晶体硅铝磷酸盐(SAPOs)的理化和催化性能的影响。已经开发了定向控制相组成,结晶度,形态和尺寸的方法,该方法以在四乙基铵氢氧化物溶液中稳定的胶态硅铝磷酸盐溶胶为模板结晶而成的SAPO晶体。已确定使用更严格的合成条件(温度和结晶持续时间的增加)会导致形成更大的晶体,并导致样品中中等强度位点的浓度增加,从而导致样品快速失活在甲醇反应中转化为C-2-C-4烯烃。在较温和的条件下(pH和温度降低)结晶会促进酸的形成​​,CHA / AEI共生晶体在甲醇转化中表现出高且稳定的性能,超过8小时,烯烃的总收率为95 wt%。

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