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Monitoring the Location,Amount,and Nature of Carbonaceous Deposits on Aged Zeolite Ferrierite Crystals by Using STEM-EELS

机译:使用STEM-EELS监测老化的沸石镁碱沸石晶体上含碳沉积物的位置,数量和性质

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摘要

By the use of electron energyloss spectroscopy performed ina scanning transmissin electron microscope (STEM-EELS) detailed spatial information is obtasined concerning the amount and nature of carbonaceous deposits formed indise the cryatals of the zeolite ferrierite (FER) during the reactin of n-butene to isobutene In all cases gradients in coke concentratin over the cryatal have been observed adn quantified An extensive accumulation of coke is observed at the entrance of the eight-membered-ring (MR) pores while less coke is present at the entrances of the ten-MR channels At a higher coke content further filling up to the complete micropore systwm occurs adn the eigh-MR pores become fully blocked The ten-MR channele remain partialy accessible for n-butene with alkyl-aromatic pecies deposited near the inlets of these channels With regard to the selective transformation of n-butene into isobutene this supoorts the view that the cataytic action takes place in the pore mouths of the ten-MR channels Overall it is demonstrated theat te major benefit of STEM-EELS is the possibility to simultaneously determine the position -resolved amount and nature fo carbonaceous deposits on intact zeolite crystals.
机译:通过使用在扫描透射电子显微镜(STEM-EELS)中进行的电子能量损失光谱分析,关于在正丁烯与硅的反应过程中沸石镁碱沸石(FER)的晶状体中形成的碳质沉积物的数量和性质的详细空间信息变得模糊不清。异丁烯在所有情况下,都可以观察到并量化了晶状体上焦炭浓度的梯度,并且在八元环(MR)孔的入口处观察到大量积炭,而十MR孔处的焦炭较少。较高焦炭含量的通道会进一步填充至完整的微孔系统,并且eigh-MR孔变得完全被堵塞。十MR通道对于正丁烯仍然部分可及,且烷基-芳香族化合物沉积在这些通道的入口附近。将正丁烯选择性转化为异丁烯的观点认为,催化作用发生在十MR的孔口中通道总体而言,STEM-EELS的主要优势在于可以同时测定完整沸石晶体上碳质沉积物的位置分辨量和性质。

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