硅源对蒸氨法制备Cu/SiO_2催化剂催化甲醇裂解制氢的影响  

Catalytic performance of methanol decomposition on Cu/SiO_2 catalyst with different silica sources prepared with ammonia evaporation method

作　　者：杜泽宇 朱明[1,2] 包喆宇 史大佑 陈晓蓉 许岩[1] 梅华 DU Ze-yu1, ZHU Ming1,2 , BAO Zhe-yu1 , SHI Da-you1, CHEN Xiao-rong1 , XU Yan1 , MEI Hua1,2(1. College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China; 2. Catalytic Hydrogenation Engineering Technology Research Center, Nuomeng Chem, Nanjing 210009, Chin)

机构地区：[1]南京工业大学化工学院,江苏南京210009 [2]南京(诺盟化工)催化氢化工程技术研究中心,江苏南京210009

出　　处：《燃料化学学报》2018年第6期692-699,共8页Journal of Fuel Chemistry and Technology

摘　　要：采用蒸氨法制备Cu/SiO_2催化剂,分别考察气相二氧化硅(SiO_2-aer)、硅胶(SiO_2-gel)和碱性硅溶胶(SiO_2-sol)对Cu/SiO_2催化剂催化甲醇裂解制氢性能的影响,并采用N2吸附-脱附、N2O化学吸附、电感耦合等离子体原子发射光谱法(ICP-AES)、X射线衍射(XRD)、H_2程序升温还原(H_2-TPR)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)等方法对催化剂进行表征。结果表明,硅源对Cu/SiO_2催化剂的活性具有较大影响。以碱性硅溶胶作为硅源制得的Cu/SiO_2-sol催化剂比表面积较大,活性中心粒径较小且分散均匀,这些使得其制氢性能优于其他两种硅源为载体所制备的催化剂。在反应温度280℃,反应压力1 MPa,甲醇质量空速0.6 h-1的条件下,相较于Cu/SiO_2-aer和Cu/SiO_2-gel催化剂,Cu/SiO_2-sol催化剂的甲醇转化率分别提高10%和7%,气相副产物CH_4和CO_2浓度也有所降低,该催化剂上的甲醇转化率和气体收率分别达到98.4%和96.7%。Cu/SiO2 catalysts were prepared via ammonia evaporation method,using fumed silica（ SiO2-aer）,silica gel（ SiO2-gel） and alkaline silica sol（ SiO2-sol） as the silica sources and their catalytic performance in methanol decomposition were investigated. The catalysts were characterized by N2 adsorption-desorption,N2O chemisorption,inductively coupled plasma atomic emission spectroscopy（ ICP-AES）, X-ray diffraction（ XRD）,H2 temperature programmed reduction（ H2-TPR）,transmission electron microscope（ TEM） and X-ray photoelectron spectroscopy（ XPS）. The results indicate that silica source can affect the decomposition activity of Cu/SiO2 catalysts. The Cu/SiO2-sol catalyst prepared with alkaline silica sol exhibits larger surface area,smaller active site size and more uniform dispersion of Cu. Therefore,it gives Cu/SiO2-sol a better decomposition performance than other catalysts. Methanol conversion on Cu/SiO2-sol is 10% higher than that on Cu/SiO2-aer,and 7% higher than that on Cu/SiO2-gel. Additionally,byproducts concentration on Cu/SiO2-sol is considerably lower than other catalysts. Under the reaction conditions of 280 ℃,1 MPa and 0. 6 h^-1 of WHSV,methanol conversion of 98.4% and gas yield of 96.7% can be achieved.

关 键 词：甲醇裂解 蒸氨法 CU/SIO2催化剂 

分 类 号：O643.88[理学—物理化学]