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机构地区:[1]大连理工大学精细化工国家重点实验室,辽宁大连116012 [2]辽宁省高校石油化工技术与装备重点实验室,辽宁大连116012
出 处:《石油学报(石油加工)》2010年第2期171-176,共6页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:国家自然科学基金重点基金(20333030);国家自然科学基金青年基金(20503003);国家自然科学基金(20773020);辽宁省中青年学科带头人和教育部博士点专项基金项目资助
摘 要:采用分步浸渍法制备了Ti O2改性的Ni-Mo/MCM-41加氢脱硫(HDS)催化剂,并以质量分数为0.8%的二苯并噻吩的十氢萘溶液作为模型化合物,考察了Ti O2及其引入顺序对Ni-Mo/MCM-41 HDS反应催化活性的影响。紫外/可见漫反射光谱(UV-Vis)、程序升温还原(TPR)以及NH3-TPD结果表明,Ti O2的引入对Ni-Mo/MCM-41催化剂活性物种配位状态及其还原性能和酸性影响不显著。由HDS反应结果可以看出,引入Ti O2虽然抑制了Ni-Mo/MCM-41的直接脱硫反应路径(DDS)的活性,但显著提高了其加氢反应路径(HYD)活性,进而提高了总的HDS反应活性。先引入Ni-Mo活性组分然后引入Ti O2能更有效地提高催化剂HDS反应活性。根据反应产物组成分析,Ti O2可能主要通过提高Ni-Mo/MCM-41硫化物酸性来提高催化剂的HYD和HDS活性。TiO2 modified Ni-Mo/MCM-41 hydrodesulfurization (HDS) catalysts were prepared by a consecutive impregnation method, and the effects of TiO2 as well as its introduction order on the HDS performance of Ni-Mo/MCM-41 were studied by using a model fuel of decalin containing 0.8% DBT. The UV-Vis, TPR and NH3-TPD results indicated that both the coordination states, the reducibility as well as the surface acidity of the oxidic precursor of Ni-Mo/MCM-41 were not remarkably affected by the introduction of TiO2. The HDS results showed that the addition of TiO2 suppressed the direct desulfurization pathway (DDS) activity of Ni-Mo/MCM-41, but significantly enhanced its hydrogenation pathway (HYD) activity, leading to an enhanced global HDS activity. The promoting effect was more pronounced when TiO2 was introduced after the impregnation of Ni-MO over MCM-41. On the base of the product compositions, it is suggested that the improved HYD and HDS activities of TiO2-containing Ni-Mo/MCM-41 catalysts may be attributed to the enhanced acidity of the sulfides.
关 键 词:加氢脱硫 Ni—Mo TIO2 MCM-41 二苯并噻吩 分步浸渍
分 类 号:TE624.9[石油与天然气工程—油气加工工程]
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