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活性形貌对CuO/ZnO/Al2O3催化加氢反应的影响
引用本文:秦霏,颜万鑫,纳薇,叶海船,高文桂,王华.活性形貌对CuO/ZnO/Al2O3催化加氢反应的影响[J].精细化工,2019,36(5).
作者姓名:秦霏  颜万鑫  纳薇  叶海船  高文桂  王华
作者单位:;1.云南省复杂有色金属资源清洁利用国家重点实验室;2.昆明理工大学冶金与能源工程学院
基金项目:国家自然科学基金项目(面上项目,重点项目,重大项目)
摘    要:以硝酸铜、硝酸锌等为原料,采用沉淀-沉积法制备了载体是介孔Al_2O_3的CuO/ZnO/Al_2O_3催化剂,通过改变焙烧时间可得到不同活性组分形貌(团簇球状和棒状)的催化剂,并用于CO/CO_2加氢反应。通过XRD、BET、N_2吸附-脱附、TEM、H_2-TPR、CO_2-TPD、NH_3-TPD和FTIR对催化剂进行了表征与测试。结果表明,活性组分(CuO/ZnO)形貌的改变影响了催化剂的Cu O晶粒尺寸、比表面积、孔径及其还原性能,且对催化剂的酸性位点和碱性位点的相对数量影响较大。团簇球状催化剂中活性组分的分散度高、易还原、碱性位多、酸性位少,有利于甲醇的生成;而棒状催化剂中孔道不均匀、碱性位少、酸性位多,更有利于二甲醚(DME)的生成。活性测试结果表明,团簇球状催化剂表现出高甲醇选择性(95.05%)和低DME选择性(4.18%);棒状催化剂的产物选择性与团簇球状相反,表现出高DME选择性(75.41%)和低甲醇选择性(12.81%)。

关 键 词:介孔Al2O3  CuO/ZnO/Al2O3催化剂  CO/CO2加氢反应  活性组分形貌  产物调控  催化技术
收稿时间:2018/9/17 0:00:00
修稿时间:2019/1/15 0:00:00

Effect of Active Morphology on Catalytic Hydrogenation of CuO/ZnO/ Al2O3
QIN Fei,YAN Wan Xin,NA Wei,Ye Hai-chuan,GAO Wen-gui and WANG Hua.Effect of Active Morphology on Catalytic Hydrogenation of CuO/ZnO/ Al2O3[J].Fine Chemicals,2019,36(5).
Authors:QIN Fei  YAN Wan Xin  NA Wei  Ye Hai-chuan  GAO Wen-gui and WANG Hua
Affiliation:Kunming University of Science and Technology,Kunming University of Science and Technology,Kunming University of Science and Technology,Kunming University of Science and Technology,Kunming University of Science and Technology
Abstract:CuO/ZnO/Al2O3 catalysts with mesoporous Al2O3 as support were prepared by precipitation-deposition method using cupric nitrate and zinc nitrate as raw materials. Catalysts possessing different active component morphologies (globular clusters and rod-like structure) were obtained by changing calcination time and used for CO/CO2 hydrogenation reaction. The catalysts were characterized and tested by XRD, BET, N2 adsorption-desorption, TEM, H2-TPR, CO2-TPD, NH3-TPD and FTIR. The results showed that the morphology of the active components affects the CuO grain size, specific surface area, pore size and reduction performance of the catalyst and has a great influence on the relative quantity of acid sites and basic sites of the catalysts. The catalyst with globular clusters has high dispersion of active components, easy to reduce, more basic sites and less acid sites, which is favorable for the formation of methanol. While the rod-like catalyst has uneven pores, less basic sites and more acid sites, which is more conducive to the formation of dimethyl ether (DME). The activity test results revealed that the catalyst with globular clusters exhibited high methanol selectivity (95.05%) and low DME selectivity (4.18%). The rod-like catalyst displayed the opposite trend with high DME selectivity (75.41%) and low methanol selectivity (12.81%).
Keywords:Mesoporous Al2O3  CuO/ZnO/Al2O3 catalysts  CO/CO2 hydrogenation  Morphology of active component  Product selective regulation
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