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首页> 外文期刊>Catalysis science & technology >Investigating the influence of acid sites in continuous methane oxidation with N2O over Fe/MFI zeolites
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Investigating the influence of acid sites in continuous methane oxidation with N2O over Fe/MFI zeolites

机译：研究酸网站的影响连续的甲烷与一氧化二氮氧化Fe / MFI沸石

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Methane oxidation using N2O was carried out with Fe-MFI zeolite catalysts at 300 degrees C. Methane conversion over Fe-ZSM-5, Fe-silicalite-1 and Fe-TS-1 indicates that Bronsted acidity is required to support the Fe-based alpha-oxygen active site for the important initial hydrogen abstraction step. Increasing the calcination temperature of Fe-ZSM-5 from 550 to 950 degrees C showed that the catalyst retained the MFI structure. However, at 950 degrees C the Bronsted and Lewis acid sites were altered significantly due to the migration of aluminium, which led to a significant decrease in catalytic performance. Over Fe-ZSM-5 the desired partial oxidation product, methanol was observed to undergo a reaction path similar to the methanol to olefin (MTO) process, which predominately produced ethene and subsequently produced coke. Methanol control experiments over Fe-silicalite-1, Fe-ZSM-5, Fe-TS-1 and H-ZSM-5 indicated that with the presence of Bronsted acidity the catalysts were more effective at forming ethene and subsequent aromatic species from DME, which resulted in an increased level of catalyst fouling. The implication of these observations is that the desorption of methanol is crucial to afford high mass balances and selectivity, however, Bronsted acid sites appear to slow this rate. These sites appear to effectively retain methanol and DME under reaction conditions, leading to low mass balances being observed. Our results confirm that to afford efficient and continuous methane oxidation by N2O, the catalytic active site must be Fe coordinated to Al.
机译：进行了甲烷氧化使用一氧化二氮Fe-MFI沸石催化剂在300摄氏度。甲烷在Fe-ZSM-5转换,Fe-silicalite-1和Fe-TS-1表明布仑斯惕酸度需要支持Fe-based alpha-oxygen重要的初始氢活性部位抽象的一步。Fe-ZSM-5温度从550到950摄氏度表明,保留了MFI催化剂结构。和路易斯酸的网站被显著改变由于铝的迁移,导致显著降低催化性能。在Fe-ZSM-5所需的部分氧化产品,甲醇进行观察类似于甲醇对烯烃的反应路径(MTO)过程,主要生产乙烯和随后生产可乐。在Fe-silicalite-1控制实验,Fe-ZSM-5, Fe-TS-1 H-ZSM-5表示布仑斯惕酸性催化剂的存在更有效地形成乙烯和吗随后的芳香物种从测距装置,导致了增加催化剂的水平污染。甲醇的解吸是至关重要的负担得起的高质量平衡和选择性,然而,布仑斯惕酸网站出现放缓率。甲醇和测距装置在反应条件下,导致低质量平衡被观察到。确认支付效率和结果一氧化二氮连续甲烷氧化的催化活性位点必须铁协调

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