Abstract Iridium catalyst using different zirconium modified-SBA-15 supports were tested in the HDT of tetralin and typical sulfur and nitrogen compounds present in diesel feed. The zirconium modified-SBA-15 supports were synthesized by sol-gel method using two sources of zirconium, zirconyl chloride and zirconium (IV) propoxide. Regarding XRD, N2 adsorption isotherms and TEM, we obtained better textural and structural properties using the alkoxide, especially when lactic acid was added in order to decrease the hydrolysis rate of zirconium propoxide. In addition, XPS and DRUV-Vis demonstrated that zirconium was incorporated mainly as tetrahedral Zr4+ species NH3-TPD showed that higher acidity is observed when tetrahedral Zr4+ species are present. Iridium dispersion was determined by TEM and H2-chemisorption and reducibility by XPS and TPR. Among the catalysts prepared, the catalyst synthesized using zirconium propoxide and lactic acid presented the highest dispersion, lowest cluster size and lowest reduction temperature. Consequently, this was the most active catalyst for the hydrogenation of tetralin, the HDN of indole and quinoline and the HDS of dibenzothiophene (DBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT). The presence of Zr+4 had a remarkable effect on the dispersion and reducibility capacity of the iridium actives species. In addition, the presence of moderate acidity in this material gives the best catalyst for HDN and HDS in the studied conditions. The inhibition effect of the sulfur and nitrogen compounds over tetralin hydrogenation was studied using individual feeds and a mixture feed. We observe that 4,6-DMDBT and quinoline were the most refractory compounds and they showed the highest inhibition effect. Tetralin hydrogenation was stronger inhibited when using the mixture feed compared with the individual feeds. This can be explained in terms of the competition between the different compounds that retard the rate of hydrogenation of tetralin. However, a high conversion of tetralin was achieved even when 300 ppm of S or N was added. The most active catalyst synthesized by direct synthesis using propoxide and lactic acid was stable after several catalytic cycles making this material as potential catalyst for HDT reaction at mild conditions.

中文翻译：

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模型柴油进料在 Ir 改性 Zr-SBA-15 催化剂上的 HDT

摘要 在四氢化萘和柴油原料中存在的典型硫和氮化合物的 HDT 中测试了使用不同锆改性 SBA-15 载体的铱催化剂。锆改性的 SBA-15 载体是通过溶胶-凝胶法合成的，使用两种锆来源，即氯化锆和丙氧化锆 (IV)。关于 XRD、N2 吸附等温线和 TEM，我们使用醇盐获得了更好的结构和结构特性，特别是当添加乳酸以降低丙醇锆的水解速率时。此外，XPS 和 DRUV-Vis 表明，锆主要以四面体 Zr4+ 物质的形式掺入。NH3-TPD 表明，当存在四面体 Zr4+ 物质时，观察到更高的酸度。铱的分散性由 TEM 和 H2 化学吸附测定，还原性由 XPS 和 TPR 测定。在制备的催化剂中，使用丙氧化锆和乳酸合成的催化剂表现出最高的分散度、最低的团簇尺寸和最低的还原温度。因此，这是氢化四氢萘、吲哚和喹啉的 HDN 以及二苯并噻吩 (DBT) 和 4,6-二甲基二苯并噻吩 (4,6-DMDBT) 的 HDS 的最活性催化剂。Zr+4 的存在对铱活性物质的分散和还原能力有显着影响。此外，在所研究的条件下，这种材料中中等酸性的存在为 HDN 和 HDS 提供了最佳催化剂。使用单独的进料和混合进料研究硫和氮化合物对萘满氢化的抑制作用。我们观察到 4, 6-DMDBT和喹啉是最难处理的化合物，它们显示出最高的抑制作用。与单独的进料相比，当使用混合进料时，四氢萘氢化受到更强的抑制。这可以从阻碍四氢萘氢化速率的不同化合物之间的竞争来解释。然而，即使添加 300 ppm 的 S 或 N，也能实现四氢化萘的高转化率。通过使用丙氧化物和乳酸直接合成合成的活性最高的催化剂在经过几个催化循环后是稳定的，这使得该材料成为在温和条件下进行 HDT 反应的潜在催化剂。这可以从阻碍四氢萘氢化速率的不同化合物之间的竞争来解释。然而，即使添加 300 ppm 的 S 或 N，也能实现四氢化萘的高转化率。通过使用丙氧化物和乳酸直接合成合成的活性最高的催化剂在经过几个催化循环后是稳定的，这使得该材料在温和条件下成为 HDT 反应的潜在催化剂。这可以从阻碍四氢萘氢化速率的不同化合物之间的竞争来解释。然而，即使添加 300 ppm 的 S 或 N，也能实现四氢化萘的高转化率。通过使用丙氧化物和乳酸直接合成合成的活性最高的催化剂在经过几个催化循环后是稳定的，这使得该材料成为在温和条件下进行 HDT 反应的潜在催化剂。