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Microreactor for the Catalytic Partial Oxidation of Methane

机译:甲烷催化部分氧化的微反应器

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Fixed-bed reactors for the partial oxidation of methane to produce synthetic gas still pose hot-spot problems. An alternative reactor, which is known as the shell-and-tube-typed microreactor, has been developed to resolve these problems. The microreactor consists of a 1 cm outside-diameter, 0.8 cm inside-diameter and 11 cm length tube, and a 1.8 cm inside-diameter shell. The tube is made of dense alumina and the shell is made of quartz. Two different methods dip and spray coating were performed to line the tube side with the LaNi_xO_y catalyst. Combustion and reforming reactions take place simultaneously in this reactor. Methane is oxidized in the tube side to produce flue gases (CO_2 and H_2O) which flow counter-currently and react with the remaining methane in the shell side to yield synthesis gas. The methane conversion using the higher-loading catalyst spray-coated tube reaches 97% at 700℃, whereas that using the lower-loading catalyst dip-coated tube reaches only 7.78% because of poor adhesion between the catalyst film and the alumina support. The turnover frequencies (TOFs) using the catalyst spray-and dip-coated tubes are 5.75 x 10~(-5) and 2.24 x 10~(-5) mol/g_(cat) · s, respectively. The catalyst spray-coated at 900℃ provides better performance than that at 1250℃ because sintering reduces the surface-area. The hydrogen to carbon monoxide ratio produced by the spray-coated catalyst is greater than the stoichiometric ratio, which is caused by carbon deposition through methane cracking or the Boudouard reaction.
机译:用于将甲烷部分氧化以产生合成气的固定床反应器仍然存在热点问题。为了解决这些问题,已经开发出一种替代反应器,称为壳管式微反应器。微反应器由1厘米外径,0.8厘米内径和11厘米长的试管和1.8厘米内径的外壳组成。该管由致密氧化铝制成,外壳由石英制成。进行了两种不同的浸涂和喷涂方法,以在管侧衬以LaNi_xO_y催化剂。燃烧和重整反应在该反应器中同时发生。甲烷在管侧被氧化,产生烟道气(CO_2和H_2O),该烟道气逆流流动并与壳侧的剩余甲烷反应生成合成气。在700℃下,使用高负载催化剂喷涂管的甲烷转化率达到97%,而使用低负载催化剂浸涂管的甲烷转化率仅达到7.78%,这是因为催化剂膜与氧化铝载体之间的粘附性较差。使用催化剂喷涂管和浸涂管的周转频率(TOF)分别为5.75 x 10〜(-5)和2.24 x 10〜(-5)mol / g_(cat)·s。在900℃下喷涂的催化剂比在1250℃下喷涂的催化剂具有更好的性能,因为烧结会减少表面积。喷涂催化剂产生的氢与一氧化碳之比大于化学计量比,这是由于甲烷裂解或布杜德反应引起的碳沉积所致。

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