Effect of synthesis temperature on structure-activity-relationship over NiMo/γ-Al2O3 catalysts for the hydrodesulfurization of DBT and 4,6-DMDBT
Effect of synthesis temperature on structure-activity-relationship over NiMo/γ-Al2O3 catalysts for the hydrodesulfurization of DBT and 4,6-DMDBT
复制标题
合成温度对 NiMo/gamma-Al2O3 DBT 和 4,6-DMDBT 加氢脱硫催化剂构效关系的影响
DOI：
10.1016/j.fuproc.2017.03.003
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发表时间：
2017-06-15
影响因子：
7.5
通讯作者：
Fan, Ji-yuan
中科院分区：
文献类型：
--
作者：
Wang, Xi-long;Zhao, Zhen;Fan, Ji-yuan
以勃姆石溶胶为原料，通过调节陈化温度，合成了一系列具有不同结构和酸度的γ-Al（2）O（3）材料。以γ-Al 2 O3为载体制备了NiMo负载型催化剂，并以DBT和4，6-DMDBT为探针分子，考察了NiMo负载型催化剂的加氢脱硫性能。采用XRD、N2-物理吸附、Py-IR、UV-Vis DRS、激光拉曼光谱、H-2-TPR、XPS、HRTEM等方法对γ-Al_2O_3载体及相应的NiMo催化剂进行了表征。表征结果表明，NiMo/γ-363催化剂具有较大的孔径（12.0 nm）、开孔体积（0.86 cm（3）g（-1））、中等的酸性和适宜的MSI。NiMo/γ-363催化剂在所有WHSV下呈现最高的DBT和4，6-DMDBT转化率。NiMo/gamma-363催化剂具有最高的k（HDS）和TOF值，这是由于NiMo/gamma-363催化剂优异的织构性能、合适的酸性和MSI、适度的分散度、高的硫化度和良好的MoS 2晶粒堆积形态的协同作用。NiMo/γ-363催化剂上4，6-DMDBT HDS的最高HYD/DDS比（1.51）表明HYD途径是主要的反应途径。此外，还提出了NiMo/γ-Al_2 O_3系列催化剂上4，6-DMDBT加氢脱硫反应的可能反应网络。(C)2017爱思唯尔B. V.保留所有权利。
A series of gamma-A1(2)O(3) materials with different textural properties and acidities were synthesized from the boehmite sol by tuning the aging temperatures. NiMo supported catalysts were prepared by using gamma-Al2O3 as the supports, then the catalytic HDS performance were evaluated by using DBT and 4,6-DMDBT to be the probe molecules. The physico-chemical properties of gamma-Al2O3 supports and the corresponding NiMo catalysts were characterized by XRD, N-2-physisorption, Py-IR, UV-Vis DRS, laser Raman spectra, H-2-TPR, XPS, HRTEM methods. The characterization results showed that NiMo/gamma-363 catalyst possessed a large pore size (12.0 nm), open pore volume (0.86 cm(3) g(-1)), moderate acidity and appropriate MSI. The NiMo/gamma-363 catalyst presented the highest DBT and 4,6-DMDBT conversions at all the WHSVs. The NiMo/gamma-363 catalyst showed highest k(HDS) and TOF values of the 4,6-DMDBT HDS, which could be ascribed to the synergistic effect of excellent textural properties, appropriate acidity and suitable MSI of the NiMo/gamma-363 catalyst, moderate dispersion degree, high sulfidation degree and desirable stacking morphology of the MoS2 crystallites. The highest HYD/DDS ratio (1.51) of the 4,6-DMDBT HDS over the NiMo/gamma-363 catalyst indicated that the HYD pathway was the main reaction route. Furthermore, a possible reaction network for 4,6-DMDBT HDS over the series of NiMo/gamma-Al2O3 catalysts was proposed. (C) 2017 Elsevier B.V. All rights reserved.