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Kinetics of hydrodeoxygenation of octanol over supported nickel catalysts: a mechanistic study

机译：支持镍催化剂上辛醇加氢脱氧的动力学：机械研究

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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 γ-Al _(2) O _(3) , SiO _(2) , 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 γ-Al _(2) O _(3) supported nickel catalysts decreased with increasing the nickel loading on γ-Al _(2) O _(3) . 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 γ-Al _(2) O _(3) and SiO _(2) 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 γ-Al _(2) O _(3) , and temperature and decreasing pressure and WHSV. The selectivity to products was strongly influenced by temperature, nickel loading on γ-Al _(2) O _(3) , pressure, and types of carrier gases (nitrogen and hydrogen). The selectivity to C _(7) hydrocarbons was favoured over catalysts with increased nickel loading on γ-Al _(2) O _(3) 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：在连续的下流式固定床反应器上，在γ-Al _（2）O _（3），SiO_（2）上，在连续的下流式固定床反应器中研究了1-辛醇的二辛糖醇的二辛族脂族醇的水冰氧基（HDO）。 HZSM-5负载的镍催化剂在488-533k的温度范围内。通过初期湿润浸渍方法制备负载的镍催化剂，并通过BET，XRD，TPR，TPD，H _（2）脉冲化学吸附，以及UV-可见光谱。支撑镍（或氧化镍）催化剂的表征揭示了分散的分散和氧化镍（或镍）的存在，这取决于镍负载的程度和载体的性质。随着γ-Al _（2）O _（3）上的镍负载增加，γ-Al _（2）O o _（3）负载镍催化剂的酸度降低。 N-庚烷，N-乙烷，二乙烯基醚，1-辛烷，庚烯，异构体，四癸烷和十六烷和十六烷被鉴定为1-辛醇的HDO产物。将C _（7）烃作为催化剂的主要产物，其具有活性金属位点，例如γ-Al _（2）O _（3）和SiO_（2）负载的镍催化剂。然而，C _（8）烃主要通过酸性催化剂形成，例如纯HZSM-5和HZSM-5负载的镍催化剂。 1-辛醇转化随着γ-Al _（2）O _（3）上的镍负载增加而增加，温度和降低压力和WHSV。对产物的选择性受温度的强烈影响，γ-Al _（2）O _（3），压力和载气（氮气和氢）的镍加载。对C _（7）烃的选择性在催化剂上有利于γ-Al _（2）O _（3）上升高的镍加载，在升高的温度和较低的压力下。基于不同催化剂的各种工艺条件下的产物分布描绘了HDO的综合反应机理。

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