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采用共沉淀法制备Cu/ZnO催化剂、水热合成法制备H-β分子筛、通过物理包膜法制备了具有核壳结构的Cu/ZnO@H-β-P催化剂,并用于合成气制备液化石油气(LPG)反应。通过XRD、NH3-TPD、BET和SEM-EDS等手段对催化剂进行了表征,利用固定床连续反应装置对催化剂进行了活性评价。结果表明,Cu/ZnO@H-β-P催化剂是具有中孔的核壳结构材料,其协同作用打破了原有的热力学平衡,促进了甲醇→DME→LPG串联反应的连续进行。与物理混合的Mix-Cu/ZnO-H-β催化剂相比,Cu/ZnO@H-β-P催化剂的CO转化率和LPG选择性更高,空速和反应温度对催化剂活性影响明显,最佳空速和反应温度分别为2 400 h~(-1)和350℃。使用Cu/ZnO@H-β-P催化剂在最佳条件下进行合成气制备LPG反应,CO转化率达到了57.22%,LPG选择性达到了60.52%。
Cu / ZnO catalyst was prepared by co-precipitation method and H-β molecular sieve was prepared by hydrothermal synthesis method. Cu / ZnO @ H-β-P catalyst with core-shell structure was prepared by physical coating method and was used in synthesis gas to produce liquefied petroleum Gas (LPG) reaction. The catalysts were characterized by XRD, NH3-TPD, BET and SEM-EDS. The activity of the catalysts was evaluated by a fixed-bed continuous reactor. The results show that the Cu / ZnO @ H-β-P catalyst is a mesoporous core-shell structure material, and its synergistic effect breaks the original thermodynamic equilibrium and promotes the continuous progress of the methanol → DME → LPG tandem reaction. Compared with the physically mixed Mix-Cu / ZnO-H-β catalyst, the CO conversion and LPG selectivity of the Cu / ZnO @ H-β-P catalyst were higher. The space velocity and the reaction temperature had a significant effect on the catalyst activity. The best space velocity and reaction temperature were 2 400 h ~ (-1) and 350 ℃, respectively. The synthesis of LPG by Cu / ZnO @ H-β-P catalyst under the optimum conditions was used to prepare LPG. The CO conversion reached 57.22% and the LPG selectivity reached 60.52%.