二甲醚水蒸气重整制氢双功能催化剂研究.doc

  二甲醚水蒸气重整制氢双功能催化剂研究# 龙旭，李靖，郭瑞，刘昭铁，刘忠文** （陕西师范大学化学与化工学院，应用表面与胶体化学教育部重点实验室，西安 710062） 5 10 15 20 25 30 35 40 摘要：二甲醚水蒸气重整（SRD）制氢作为质子交换膜燃料电池（PEMFC）汽车氢源的关键在 于开发高效、高选择性的催化剂。为此，本文采用络合分解法制备了一系列 Cu/ZnO/Al2O3 复合氧化物，较为系统地考察了络合剂、溶剂和 Cu/Zn/Al 摩尔比等制备条件对 Cu/ZnO/Al2O3 结构及其还原性能的影响，并研究了所制备 Cu/ZnO/Al2O3 与商品 ZSM-5 分子筛(Si/Al=25) 机械混合物作为双功能催化剂的 SRD 反应性能。XRD、低温 N2 吸脱附及 H2-TPR 表征结果表明， 溶剂和络合剂是影响 Cu/ZnO/Al2O3 结构、织构和还原性能的关键因素。SRD 反应结果表明， 水为溶剂、丙三醇为络合剂制备的 Cu/ZnO/Al2O3 与 ZSM-5 组成的双功能催化剂具有较好的低 温活性，可解释为 Cu/ZnO/Al2O3 的还原性能及比表面积的差异。 关键词：工业催化；二甲醚；氢；水蒸汽重整；ZSM-5 分子筛；Cu/ZnO/Al2O3 中图分类号：O 643 Investigation on the bifunctional catalyst for the steam reforming of dimethyl ether Long Xu, Li Jing, Guo Rui, Liu Zhaotie, Liu Zhongwen (Key laboratory of Applied Surface and Colloid Chemistry (MOE), School of Chemistry & Chemical Engineering, Shaanxi Normal University, Xi'an 710062) Abstract: A series of Cu/ZnO/Al2O3 oxides were prepared by a complex-combustion method, and the effect of paraperation parameters, e.g., complex agent, solvent, and the molar ratio of the metal cations (nCu/nZn/nAl), on the texture, structure, and reduction behaviour of the oxides were sysmetically investigated. Characterization results of XRD, H2-TPR and N2 adsorption/desorption indicate that solvent and complex agent are important factors influencing the structural and reductive properties of the oxides. The physical mixture of the thus prepared Cu/ZnO/Al2O3 and a commercial ZSM-5 zeolite (Si/Al=25) was subjected to the steam reforming of dimethyl ether (SRD), and the properties of the mixded oxide had a significant impact on the performance of SRD over the bifunctional catalyst. Moreover, the functional catalyst containing Cu/ZnO/Al2O3 prepared by using water as a solvent and glycerin as a complex agent gave higher catalytic activity at low reaction temperatures. These reaction results were reasonably explained as the variation in BET surface areas and reduction behavior of the Cu/ZnO/Al2O3. Keywords: Industrial catalysis; di