Catalytic deoxygenation of methyl laurate as a model compound to hydrocarbons on nickel phosphide catalysts: Remarkable support effect

Catalytic deoxygenation of methyl laurate as a model compound to hydrocarbons on nickel phosphide catalysts: Remarkable support effect
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月桂酸甲酯作为模型化合物在磷化镍催化剂上催化脱氧制烃:显着的支撑效果

DOI:
10.1016/j.fuproc.2013.08.010
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发表时间:
2014-02
影响因子:
7.5
通讯作者:
Tian Shasha
Tian Shasha
中科院分区:
工程技术1区
文献类型:
--
作者:
Shi Heng;Chen Jixiang;Yang Yan;Tian Shasha

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本文研究了磷化镍催化剂上月桂酸甲酯脱氧制C11和C12烃的载体效应。以Ni/P比为1.0的前驱体为原料,采用H2-TPR法在SiO2、CeO 2、TiO 2和SAPO-11上生成Ni 2 P,在γ-Al 2 O3上生成Ni 3 P和Ni 12 P5,在HY上生成Ni 12 P5和Ni 2 P。Ni_2P/SiO_2催化剂中Ni位的电子密度较低,可能存在Ni_3P和Ni_(12)P_5相,也可能存在还原态CeO_2或TiO_2向Ni_2P的电子转移。在573-613 K和3.0 MPa下,月桂酸甲酯的转化率和C11、C12烃的选择性依次为Ni 2 P/SiO2> Ni 3 P-Ni 12 P5/Al 2 O3> Ni 2 P/TiO 2> Ni 2 P/SAPO-11 > Ni 2 P-Ni 12 P5/HY > Ni 2 P/CeO 2,C11/C12摩尔比的顺序为:Ni 2 P/CeO 2> Ni 3 P-Ni 12 P5/Al 2 O3> Ni 2 P/SiO2> Ni 2 P/SAPO-11 > Ni 2 P/TiO 2> Ni 2 P-Ni 12 P5/HY。载体的作用主要是由于载体的酸性和还原性。催化剂的活性、烃类选择性和脱氧途径与Ni位的表面密度、Ni位的电子性质、Ni_2 P晶粒尺寸以及Ni位与酸位或氧空位的协同作用有关。
This work investigated the support effect on the deoxygenation of methyl laurate to C11 and C12 hydrocarbons over nickel phosphide catalysts. By the H2-TPR method from the precursors with Ni/P ratio of 1.0, Ni2P was produced on SiO2, CeO2, TiO2and SAPO-11, while Ni3P and Ni12P5were formed on γ-Al2O3, and Ni12P5and Ni2P were formed on HY. Ni2P/SiO2had lower electron density of Ni site than other catalysts, where either there were the Ni3P and Ni12P5phases or there was the electron transfer from reduced CeO2or TiO2to Ni2P. At 573–613 K and 3.0 MPa, the conversion of methyl laurate and the selectivity to C11 and C12 hydrocarbons tended to decrease in the sequence of Ni2P/SiO2> Ni3P-Ni12P5/Al2O3> Ni2P/TiO2> Ni2P/SAPO-11 > Ni2P-Ni12P5/HY > Ni2P/CeO2, whereas the C11/C12 molar ratio followed in the order of Ni2P/CeO2> Ni3P-Ni12P5/Al2O3> Ni2P/SiO2> Ni2P/SAPO-11 > Ni2P/TiO2> Ni2P-Ni12P5/HY. The effect of supports mainly results from their acidity and reducibility. The catalyst activity, the selectivity to hydrocarbons and the deoxygenation pathway are correlated with the surface density of Ni site, the electron property of Ni site, the Ni2P crystallite size and the synergism between the Ni site and the acid site or the oxygen vacancy.
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发表时间: 2009-06
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