摘要
The influence of the synthesis method parameters used to prepare nickel-based catalysts on the catalytic performance for the glycerol steam reforming reaction was studied.A series of Al2O3-supported Ni catalysts were synthesized,with nickel loading of 8 wt%,using the incipient wetness,wet impregnation,and modified equilibrium deposition filtration methods.The catalysts＇ surface and bulk properties were determined by inductively coupled plasma（ICP）,N2 adsorption-desorption isotherms（BET）,X-ray diffraction（XRD）,scanning electron microscopy（SEM）,transmission electron microscopy（TEM）,and temperature-programmed reduction（TPR）.Used catalysts were characterized by techniques such as elemental analysis and SEM in order to determine the level of carbon that was deposited and catalyst morphology.The results indicated that the synthesis method affected the textural,structural and surface properties of the catalysts,differentiating the dispersion and the kind of nickel species on alumina＇s surface.The formation of nickel aluminate phases was confirmed by the XRD and TPR analysis and the β-peak of the Ni/Al-edf catalyst was higher than in the other two catalysts,indicating that the nickel aluminate species of this catalyst were more reducible.Both Ni/Al-wet and Ni/Al-edf catalysts showed increasing CO2 selectivities and approximately constant CO selectivities for temperatures above 550℃,indicating that these catalysts successfully catalyze the water gas shift reaction.It was also confirmed that the Ni/Al-edf catalyst had the highest values for glycerol to gaseous products conversion,hydrogen yield,allyl alcohol,acetaldehyde,and acetic acid selectivities at 650℃ and the lowest carbon deposition of the catalysts tested.The correlation of the catalysts＇ structural properties,dispersion and reducibility with catalytic performance reveals that the EDF method can provide catalysts with higher specific surface area and active phase＇s dispersion,that are easier to reduce,more active and selective
研究了制备参数对用于甘油蒸汽重整反应的Ni基催化剂性能的影响.采用过量浸渍法、等体积浸渍法和改进的平衡沉积过滤(EDF)法制备了一系列Al2O3负载的8 wt%Ni催化剂,运用X射线衍射(XRD)、电感耦合等离子体光谱仪、N_2吸附-脱附、扫描电镜(SEM)、透射电镜和H2程序升温还原(TPR)表征了催化剂的表面和体相性质;采用CHN分析仪和SEM表征了使用后催化剂以测定其表面沉积的碳及其形貌.结果表明,制备方法对所制催化剂的织构、结构和表面性质影响很大,导致氧化铝表面Ni物种的分散和种类的不同.即使XRD和TPR结果证实形成了铝酸镍晶相,但Ni/Al-edf催化剂中β峰的贡献大于其它两个催化剂的,表明在这种情况下铝酸镍更容易还原.在550 ℃以上CO_2选择性增加和CO选择性不变,表明Ni/Al-wet和Ni/Al-edf催化剂可成功催化水汽变换反应.另外,650 ℃时Ni/Al-edf催化剂上甘油生成气相产物的转化率、氢气产率以及烯丙醇、乙醛和乙酸选择性最高,且它在所有催化剂中的积炭量也最低.将催化剂结构性质、分散度和还原性与其催化性能相关联,发现EDF法制得的催化剂比表面积和活性相分散度更高,更易被还原,因而其活性和生成H_2的选择性更高,也更抗积碳.
基金
Financial support by the program THALIS implemented within the framework of Education and Lifelong Learning Operational Programme
co-financed by the Hellenic Ministry of Education,Lifelong Learning and Religious Affairs and the European Social Fund,for the project 'Production of Energy Carriers from Biomass by Products
financial support provided by the Committee of the Special Account for Research Funds of the Technological Educational Institute of Western Macedonia(ELKE,TEIWM)
