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首页> 外文期刊>RSC Advances >Kinetics of hydrodeoxygenation of octanol over supported nickel catalysts: a mechanistic study
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Kinetics of hydrodeoxygenation of octanol over supported nickel catalysts: a mechanistic study

机译：负载型镍催化剂上辛醇加氢脱氧的动力学：机理研究

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The hydrodeoxygenation (HDO) of 1-octanol as a model aliphatic alcohol of bio-oil was investigated in a continuous down-flow fixed-bed reactor over gamma-Al2O3, SiO2, and HZSM-5 supported nickel catalysts in the temperature range of 488-533 K. The supported nickel catalysts were prepared by incipient wetness impregnation method and characterized by BET, XRD, TPR, TPD, H-2 pulse chemisorption, and UV-vis spectroscopy. Characterization of supported nickel (or nickel oxide) catalysts revealed existence of dispersed as well as bulk nickel (or nickel oxide) depending on the extent of nickel loading and the nature of the support. The acidity of gamma-Al2O3 supported nickel catalysts decreased with increasing the nickel loading on gamma-Al2O3. n-Heptane, n-octane, di-n-octyl ether, 1-octanal, isomers of heptene and octene, tetradecane, and hexadecane were identified as products of HDO of 1-octanol. The C-7 hydrocarbons were observed as primary products for catalysts with active metal sites such as gamma-Al2O3 and SiO2 supported nickel catalysts. However, C-8 hydrocarbons were primarily formed over acidic catalysts such as pure HZSM-5 and HZSM-5 supported nickel catalyst. The 1-octanol conversion increased with increasing nickel loading on gamma-Al2O3, and temperature and decreasing pressure and WHSV. The selectivity to products was strongly influenced by temperature, nickel loading on gamma-Al2O3, pressure, and types of carrier gases (nitrogen and hydrogen). The selectivity to C-7 hydrocarbons was favoured over catalysts with increased nickel loading on gamma-Al2O3 at elevated temperature and lower pressure. A comprehensive reaction mechanism of HDO of 1-octanol was delineated based on product distribution under various process conditions over different catalysts.
机译：在连续下流固定床反应器中，在γ-Al2O3，SiO2和HZSM-5负载的镍催化剂上，在温度范围为488的条件下，研究了作为生物油模型脂肪醇的1-辛醇加氢脱氧（HDO） -533K。负载的镍催化剂是通过初湿浸渍法制备的，并通过BET，XRD，TPR，TPD，H-2脉冲化学吸附和紫外可见光谱进行表征。负载型镍（或氧化镍）催化剂的表征表明，取决于镍的负载程度和载体的性质，分散镍和块状镍（或氧化镍）的存在。 γ-Al2O3负载的镍催化剂的酸度随γ-Al2O3上镍负载量的增加而降低。将正庚烷，正辛烷，二正辛醚，1-辛醛，庚烯和辛烯的异构体，十四烷和十六烷鉴定为1-辛醇的HDO产物。观察到C-7碳氢化合物是具有活性金属位点的催化剂（例如γ-Al2O3和SiO2负载的镍催化剂）的主要产物。但是，C-8烃主要在酸性催化剂（例如纯HZSM-5和HZSM-5负载的镍催化剂）上形成。 1-辛醇转化率随γ-Al2O3上镍负载量的增加，温度的升高以及压力和WHSV的降低而增加。产品的选择性受到温度，γ-Al2O3上镍的负载量，压力和载气类型（氮气和氢气）的强烈影响。与在高温和低压下，γ-Al2O3上镍负载量增加的催化剂相比，对C-7烃的选择性更有利。根据产物在各种工艺条件下在不同催化剂上的分布，描述了1-辛醇HDO的综合反应机理。

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