HZSM-5双功能催化剂的制备及催化CO2加氢合成二甲醚.pdfVIP

学兔兔 石 油 化 工 2015年第44卷第4期 PETRoCHEMICAL TECHNoL0GY ·44l· 焙烧态类水滑石／HZSM一5双功能催化剂的 制备及催化CO2加氢合成二甲醚 常琴琴，赵 博，杨 萌，刘 艳，刘恩周，樊 君 (西北大学化工学院，陕西西安710069) [摘要]采用并流共沉淀法制备了不同ZrO 含量的CuO—ZnO—A1 O，一ZrO 类水滑石前体，焙烧后与HZSM一5分子筛物理混 合得到CuO—ZnO—A1 O，一ZrO ／HZSM一5双功能催化剂，采用XRD、N：物理吸附、H 一TPR等技术对催化剂的物相、结构 特征及还原性进行了表征，考察了催化剂对CO 加氢直接合成二甲醚(DME)反应的催化性能。实验结果表明，所有前体试样 均具有结晶相为Cu，Zn A1 (OH)。 ·4H：O的水滑石结构，ZrO：的加入改善了催化剂的还原性和活性，DME合成速率主要取决 于甲醇的合成速率。在533 K、3．0 MPa、 (H2)：n(CO )=3：1、GHSV=2 400 h 的反应条件下，当n(ZrO2)：n(AI2O3+ ZrO )=0．10时，催化剂的反应性能最佳，CO 转化率达25．87％，DME选择性达48．15％；反应30 h后，催化剂仍表现出较 高的活性及稳定性。 [关键词]类水滑石前体；HZSM一5分子筛；双功能催化剂；锆助剂；二氧化碳加氢；二甲醚 [文章编号]1000—8144(2015)04—0441—06 [中图分类号]TQ 032．4 [文献标志码]A Synthesis of Dimethyl Ether from CO ／H on Bifunctional Calcined Hydrotalcite．．Like Precursors／HZSM．．5 Catalysts Chang Qinqin，Zhao Bo，Yang Meng，Liu Yan，Liu Enzhou，Fan Jun (School of Chemical Engineering，Northwest University，Xi’an Shaanxi 710069，China) [Abstract]A series of CuO—ZnO-A12 O3一ZrO2 hydrotalcite—like precursors with different ZrO2 content were prepared through CO—precipitation and then were calcinated．The products were physically mixed with HZSM-5 to prepared catalysts for the synthesis of dimethyl ether(DME)by the hydrogenation of CO2．The catalysts were characterized by means of XRD，N2 physisorption and H2-TPR．The results showed that the catalysts exhibited hydrotalcite—like structure with Cu3Zn3A12(OH)16·4H2O phase． The addition of ZrO2 improved the reducibility and activity of the catalysts．The experimental results in— dicated that the DME synthesis rat