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CO2 atmosphere-enhanced methanol aromatization over the NiO-HZSM-5 catalyst

机译：NiO-HZSM-5催化剂上的CO2气氛增强甲醇芳构化

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摘要

The aromatization of methanol over parent HZSM-5 and the modified NiO-HZSM-5 in a fixed-bed reactor was investigated under CO2 and N-2 flow. The as-prepared catalysts were characterized by H-2-TPR, XRD, BET, NH3-TPD, CO2-TPD and probe-molecule reaction. Compared with parent HZSM-5 in CO2 or N-2 flow and with NiO-HZSM-5 in N2 flow, NiO-HZSM-5 showed greatly improved aromatization activity and BTX (benzene, toluene and xylene) yield in CO2 atmosphere. This is attributed to the cooperation of acid sites with the activated CO2 (over NiO species), which not only can effectively promote dehydrogenation of alkanes to form olefin intermediates, but also can accelerate dehydrogenation in the conversion of olefin intermediates to aromatics. In particular, an optimized NiO-HZSM-5 with 2.0 wt% NiO loading showed 50.1% total aromatic yield and 35.5% BTX yield in CO2 atmosphere. It also showed high catalytic stability resulting from the restriction of coking due to its acidity, carbonaceous elimination by the activated CO2-reacting deposited coke, and the suppressed reduction of highly active NiO species by activated CO2.
机译：在CO2和N-2流量下，研究了固定床反应器中母体HZSM-5和改性NiO-HZSM-5上甲醇的芳构化作用。制备的催化剂通过H-2-TPR，XRD，BET，NH3-TPD，CO2-TPD和探针-分子反应进行表征。与在CO2或N-2气流中的母体HZSM-5和在N2气流中的NiO-HZSM-5相比，NiO-HZSM-5在CO2气氛中的芳构化活性和BTX（苯，甲苯和二甲苯）的收率大大提高。这归因于酸位与活化的CO2（超过NiO物种）的协作，这不仅可以有效地促进烷烃的脱氢以形成烯烃中间体，而且可以在烯烃中间体向芳烃的转化中加速脱氢。特别地，具有2.0重量％的NiO负载的优化的NiO-HZSM-5在CO 2气氛中显示出50.1％的总芳族产率和35.5％的BTX产率。由于其酸度限制焦化，通过活化的CO2反应沉积的焦炭去除碳以及通过活化的CO2抑制高活性NiO的还原，它还显示出高的催化稳定性。

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