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Characterization of the location of coke deposited on spent HZSM-5 zeolite by special temperature-programmed oxidation and isothermal oxidation methods
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2017-08-24 , DOI: 10.1016/j.apcata.2017.08.023
Xiaochao Xian , Chao Ran , Chenglong Nai , Peng Yang , Shuo Zhao , Lichun Dong

The location of coke deposited on HZSM-5 zeolite catalyst during the supercritical catalytic cracking (400 °C, 4.0 MPa) of n-dodecane was systematically characterized by special temperature-programmed oxidation (TPO) and isothermal oxidation methods, and a steric hindrance model describing the interactions of the coke deposited on different locations was proposed to support the methods theoretically. Accord to the results, the sharp shoulder peak that appears on the TPO profile at high temperature range (> 700 °C) with low concentration of oxygen in the oxygen/nitrogen mixed carrier gas (≤ 2.0 Vol.%) can be ascribed to the characteristic peak representing the oxidation of the coke blocked in micropores, while the appearance of the CO peak during the isothermal oxidation at high temperature (≥ 550 °C) using air as carrier gas provides another method to detect the coke blocked in micropores. Through checking whether the characteristic sharp shoulder peak of the TPO profile appears or not as expected according to the steric hindrance model during the re-oxidation of several samples with different coke content and spatial distribution, which were prepared by partial oxidation of the spent catalyst using TPO and isothermal oxidation methods, the special TPO and isothermal oxidation methods combined with their theoretical support of the steric hindrance model were proved to be self-consistent in the characterization of the location of coke. The location information of coke was further verified by the typical method of nitrogen adsorption-desorption analyses of a series of partially oxidized samples prepared by TPO method.



中文翻译:

通过特殊的程序升温氧化和等温氧化方法表征沉积在废HZSM-5沸石上的焦炭的位置

n的超临界催化裂化(400°C,4.0 MPa)过程中沉积在HZSM-5沸石催化剂上的焦炭的位置通过特殊的程序升温氧化(TPO)和等温氧化方法对十二碳烷进行了系统表征,并提出了描述沉积在不同位置的焦炭相互作用的空间位阻模型,以从理论上支持该方法。根据结果​​,在高温范围(> 700°C)且氧气/氮气混合载气中的氧气浓度较低(≤2.0 Vol。%)时,TPO轮廓上出现的尖峰峰可以归因于代表被阻塞在微孔中的焦炭氧化的特征峰,而在高温(≥550°C)下使用空气作为载气等温氧化过程中出现的CO峰则提供了另一种检测被阻塞在微孔中的焦炭的方法。通过检查几个焦炭含量和空间分布不同的样品的再氧化过程中,根据空间位阻模型,根据空间位阻模型检查TPO轮廓的特征性尖峰峰是否按预期出现,这些样品是通过使用废催化剂进行部分氧化而制得的。 TPO和等温氧化方法,特殊的TPO和等温氧化方法,结合其对空间位阻模型的理论支持,被证明在焦炭位置表征中是自洽的。焦炭的位置信息通过典型的氮吸附-解吸分析方法(通过TPO方法制备的一系列部分氧化的样品)进一步验证。

更新日期:2017-08-24
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