用于二甲醚水蒸气重整制氢金属铜基催化剂研究-工业催化专业论文.docx

ABSTRACTThe rapid consumption of fossil fuels and as-induced many kinds of environment pollution have driven extensive exploration of new energy alternatives. Hydrogen is a kind of clean and renewable energy, which is more suitable for future energy development. Dimethyl ether steam reforming (DME SR) is an effective way to produce hydrogen. For the production of hydrogen via DME SR, the development of highly efficient catalysts is crucial. Currently, the greatest challenge is to improve the catalytic performance of the catalysts, including low-temperature activity and selectivity. In this work, a kind of complex catalysts consisting of metal (CuZnAl or CuFe2O4) and solid acid (?-Al2O3) is employed for DME SR reaction, and systematically studied from several aspects, including the effect of calcination temperature, contents of active components, reaction conditions and active phase modifications. Multiple techniques such as BET, XRD, H2-TPR, N2O chemisorption and XAFS (including XANES and EXAFS) were employed for catalyst characterization. The structures and the properties of the catalysts are well correlated.Firstly, we performed thermodynamics analysis and drew a conclusion that DME SR reaction is not controlled by thermodynamics equilibrium and DME can be converted totally when reaction temperature is higher than 200 oC and S/C1.5. Besides, CH4 and C are thermodynamically favorable products; however, the appearance of them will decrease the hydrogen yield. Therefore, high selectivity is required for the catalysts to inhibit the formation of CH4 and C.Coprecipitation method was employed to prepare CuZnAl catalysts viahydrotalcite precursor, the effect of calcination temperature and contents of active components are investigated based upon catalytic test and characterization results. According to XRD and TPR results, the sample calcined at 500 oC which is more active has a proper interaction between Cu and carrier, besides, no CuAl2O4 was identified and the