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Co修饰碳纳米管促进的Cu-ZrO2催化剂上CO2加氢制甲醇

期刊名称：厦门大学学报 (自然科学版), 2008, 47(6): 765-771
时间：0
分类：O643.36[理学—物理化学;理学—化学]
作者机构：[1]厦门大学化学化工学院化学系,固体表面物理化学国家重点实验室．醇醚酯化工清洁生产国家工程实验室,福建厦门361005
相关基金：国家“973”项目（2005CB221403）,国家自然科学基金（20590364）,福建省科技重大专项（2005HZ01-3）资助
相关项目：能源发展中的若干关键化学科学基础问题

关键词： Co修饰多壁碳纳米管基复合材料, CuiZrj-x%(y%Co/CNT)催化剂, CO2加氢, 甲醇合成, Co-decorated MWCNT-based composite materials , CuiZrj-x % （y% Co/CNTs） catalysts, CO2 hydrogenation, methanol synthesis

中文摘要：

利用微波助多元醇化学还原沉积法，制备一类Co修饰的多壁碳纳米管（CNT）基复合材料（y％Co／CNT），进而用其作为添加剂，制备共沉淀型Y％Co／CNT促进的Cu—ZrO。催化剂，CuiZrj-x％（y％Co／CNT）．Co对CNT的修饰明显地提高了该催化剂对CO。加氢制甲醇的催化活性．在Cu1Zr1-10％（4．3％Co／CNT）催化剂上，5．0MPa，513K，V（H2）／V（C02）／V（N2）=69／23／8，GHSV=8000mE／（h·g）的反应条件下，CO2加氢的转化频率（TOF，即单位时间（s）内在单个表面活性金属Cu^0位上CQ加氢转化的分子数）达2．89×10^-3s^-1，是相同条件下非促进的原基质Cu，Zr，和单纯CNT促进的对应物Cu1Zr1—10％CNT上这个值（2．36×10^-3s^-1和2．40×10^-3s^-1）分别的1．22和1．20倍；在CO2加氢产物中甲醇的C-基选择性为～92％．时空产率达176mg／（h·g-cax．）．催化剂的表征研究显示，Co修饰CNT促进的催化剂对H2优良的吸附活化性能对CO2加氢转化频率（TOF）的显著提高起着重要作用．

英文摘要：

With the homemade Co-decorated multiwalled carbon nanotubes （y%Co/CNT） as promoter,a type of y%Co/CNT- promoted co- precipitated Cu-ZrOz catalysts, Cui Zrj-x% （y% Co/CNT）, were developed. Over a Cu1 Zr1-10% （4.3% Co/CNT） catalyst under reaction conditions of 5.0 MPa,513 K,V（ H2 ）/V（CO2 ）/V（N2 ）= 69/23/8 and GHSV= 8 000 mL/（h · g）, the observed turn- over frequency （TOF） of CO2 hydrogenation reached 2.89 × 10^-3s^-1. This value was 1.22 and 1.20 times that （2.36 × 10^-3s^-1 and 2.40 × 10^-3s^-1） of the CNT-free substrate Cu1Zr1 and the simple CNT-promoted counterpart Cu1Zr1-10 %CNT, respectively, under the same reaction conditions. The selectivity of methanol in the CO2 hydrogenation products reached - 92%, with corresponding STY reaching 176 mg-CH2OH/（h · g-cal. ）. Characterization of the catalysts revealed that the hydrogen adsorption capacity of the Co-decorated CNT-promoted Cu1 Zr1-based catalyst was considerably higher than that of the CNT-free substrate or the simple CNT-promoted counterpart. This would be favorable to generating a surface micro-environment with a high concentration of H-adspecies on the functioning catalyst,thus increasing the rate of surface CO2 hydrogenation reactions.