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Catalytic conversion of dimethyl ether to lower olefins: Process and catalyst deactivation studies.

机译:二甲醚催化转化为低级烯烃的研究:工艺和催化剂失活研究。

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Coal or natural-based synthesis gas can be converted to dimethyl ether in a single-stage, liquid phase process. The process described here converts dimethyl ether to hydrocarbons, especially lower olefins. Thus, a novel process of producing lower olefins from coal via dimethyl ether has been introduced. The superior process advantages as well as its competitive economics quite clearly identifies this process to be quite promising when conducted on an industrial scale.; The process feasibility of dimethyl ether conversion has been evaluated and the range of products of this process have been identified. The effect of key operating parameters like temperature, partial pressure of dimethyl ether, and space velocity of dimethyl ether have been addressed and these parameters have been optimized to maximize the yield of lower olefins. The effect of the acidity (number of acidic sites and their distribution) of the zeolite catalyst on the product distribution has also been evaluated. The effect of operating times on dimethyl ether conversion, as well as on the coking contents of the zeolite catalysts is evaluated. Lastly, the economic analysis of this process is conducted to determine if this process is feasible to be conducted on an industrial scale.; This process uses dimethyl ether as the raw material, ZSM-5 type zeolite as the catalyst and a laboratory scale, once-through fixed-bed reactor as the mode of operation. Lower olefin selectivities, as high as 75-80 wt.%, have been achieved by dimethyl ether conversion over zeolite catalysts in a fixed bed reactor. These high selectivities can be accomplished by operating at higher temperatures, and low partial pressures as well as high space velocities of dimethyl ether. The lower olefin selectivity is further enhanced by utilizing a ZSM-5 zeolite with high silica to alumina ratios of 150. The zeolite catalysts investigated show remarkable thermal stability at extended periods of time on stream. Dimethyl ether conversion was maintained at 100%, and no appreciable changes in the product distribution were noticed when operating for as much as 60 hours on stream. The coking loadings on partially deactivated catalysts was evaluated and the change in the structure of the deactivated catalyst was examined by infra-red and x-ray diffraction techniques. The economic analysis of this dimethyl ether process indicate that olefins like ethylene, propylene, and butenes can be produced at prices that are comparable or cheaper than those of existing processes.
机译:煤或基于天然气的合成气可以在单级液相过程中转化为二甲醚。本文所述的方法将二甲醚转化为烃,尤其是低级烯烃。因此,已经引入了一种通过煤通过二甲醚生产低级烯烃的新方法。优越的工艺优势及其竞争经济性很清楚地表明,这种工艺在工业规模上进行时很有希望。已评估了二甲醚转化的工艺可行性,并确定了该工艺的产品范围。已经解决了关键操作参数(例如温度,二甲醚分压和二甲醚的空速)的影响,并且对这些参数进行了优化,以最大程度地降低低级烯烃的收率。还评估了沸石催化剂的酸度(酸性位点的数量及其分布)对产物分布的影响。评价了操作时间对二甲醚转化率以及对沸石催化剂的焦化含量的影响。最后,对该过程进行经济分析,以确定该过程在工业规模上是否可行。该工艺以二甲醚为原料,ZSM-5型沸石为催化剂,实验室规模,一次通过固定床反应器为操作方式。在固定床反应器中,通过二甲醚在沸石催化剂上的二甲醚转化已经实现了较低的烯烃选择性,高达75-80重量%。这些高选择性可以通过在较高温度,较低的分压以及较高的二甲醚的空速下进行操作来实现。通过使用高二氧化硅与氧化铝之比为150的ZSM-5沸石,可以进一步提高较低的烯烃选择性。所研究的沸石催化剂在延长的生产时间内显示出显着的热稳定性。二甲醚的转化率保持在100%,当连续运行60小时时,产品分布没有明显变化。评估了部分失活的催化剂上的焦化负荷,并通过红外和X射线衍射技术检查了失活的催化剂结构的变化。该二甲醚工艺的经济分析表明,可以以与现有工艺相当或便宜的价格生产烯烃,如乙烯,丙烯和丁烯。

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