催化炭膜制备及其强化甲醇水蒸气重整制氢反应

Fabrication of Catalytic Carbon Membranes and Their Intensification of Hydrogen Production Reaction from Methanol Steam Reforming

甲醇水蒸气重整(SRM)是重要的分布式制氢技术,然而受热力学平衡和动力学的限制,传统反应器的转化率和收率较低。本工作通过在反应过程中耦合催化炭膜,凭借其催化和分离联合作用实现强化SRM反应效果。采用红外光谱、X射线衍射、X光电子能谱、扫描电镜和泡压法等手段对膜材料的化学结构、微晶结构、化学元素、微观形貌和孔隙结构等进行了表征。考察了炭膜微结构、反应温度等因素对SRM反应的转化率和收率影响。结果显示:反应过程中耦合催化炭膜,显著强化了SRM反应效果;随反应温度升高,甲醇转化率增大,而氢气收率先升后降;当反应温度为240℃时,氢气收率比固定床反应器提高1.7倍。

Steam reforming of methanol (SRM) is an important distributed hydrogen production technology. However, the conversion and yield of traditional reactors are quite inferior due to the constraints of thermodynamic equilibrium and kinetics. Here, catalytic carbon membranes were integrated in the reaction process to strengthen SRM reaction by virtue of the combination effects of catalysis and separation. The chemical structure, microcrystal structure, chemical elements, microscopic morphology and porous structure of the membrane materials were characterized by means of infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscope and bubble pressure method, respectively. The effects of carbon membrane microstructure, reaction temperature and other factors on the conversion and yield of SRM reaction were investigated. The results show that the integration of catalytic carbon membranes during reaction process significantly enhances the efficiency of SRM reaction. As the reaction temperature increases, the methanol conversion increases, while the hydrogen yield first increases then decreases. When the reaction temperature is 240 ℃, the hydrogen yield is increased by 1.7 times compared to conventional fixed bed.