New catalysts for hydroprocessing: Transition metal carbides and nitrides
New catalysts for hydroprocessing: Transition metal carbides and nitrides
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DOI：
10.1021/j100044a025
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发表时间：
1995-11
期刊：
影响因子：
--
通讯作者：
S. Ramanathan;S. Oyama
中科院分区：
文献类型：
--
作者：
S. Ramanathan;S. Oyama
通过氧化物前体与反应气体（碳化物为 20% CH{sub 4}/H{sub 2}，氮化物为 100% NH{sub 3}）的程序升温反应，制备了一系列中等表面积的钼、钨、钒、铌和钛的过渡金属碳化物和氮化物。样品的相纯度和组成通过 X 射线衍射光电子能谱 (XPS) 确定，而表面性质通过 N{sub 2} BET 和 CO 化学吸附测量确定。在三相滴流床反应器中测试了催化剂在加氢脱氮（HDN）、加氢脱硫和加氢脱氧中的活性，特别是加氢脱氧。催化测试使用含有 3000 ppm 硫（二苯并噻吩）、2000 ppm 氮（喹啉）、500 ppm 氧（苯并呋喃）、20 wt% 芳族化合物（四氢化萘）和余量脂肪族化合物（十四烷）的模型液体进料混合物进行。发现碳化物和氮化物对喹啉的 HDN 具有活性，活性遵循组 6 > 组 5 > 组 4 的顺序。值得注意的是，Mo{sub 2}C 显示出比商业硫化 Ni-Mo/Al{sub 2} O{sub 3} 催化剂（壳 324）更优异的面 HDN 活性。废催化剂的 XRD 分析表明整体结构没有变化，而 XPS 结果显示催化剂的表面区域几乎没有硫的掺入，表明这些材料对硫具有耐受性。 42 条参考文献，11 个图，7 个标签。« 更少
A series of moderate surface area transition metal carbides and nitrides of molybdenum, tungsten, vanadium, niobium, and titanium were prepared by temperature-programmed reaction of the oxide precursor with a reactant gas (20% CH{sub 4}/H{sub 2} for the carbides and 100% NH{sub 3} for the nitrides). The phase purity and composition of the samples were established by X-ray diffraction photoelectron spectroscopy (XPS), while surface properties were determined by N{sub 2} BET and CO chemisorption measurements. The catalysts were tested in three-phase trickle-bed reactor for their activity in hydrodenitrogenation (HDN), hydrodesulfurization, and hydrodeoxygenation, with particular emphasis on HDN. The catalytic tests were carried out using a model liquid feed mixture containing 3000 ppm sulfur (dibenzothiophene), 2000 ppm nitrogen (quinoline), 500 ppm oxygen (benzofuran), 20 wt% aromatics (tetralin), and balance aliphatics (tetradecane). The carbides and nitrides were found to be active for HDN of quinoline with activity following the order group 6 > group 5 > group 4. Notably, Mo{sub 2}C showed superior areal HDN activity than a commercial sulfided Ni-Mo/Al{sub 2} O{sub 3} catalyst (shell 324). The XRD analysis of the spent catalysts indicated no change in the bulk structure, while XPS results showed little incorporation of sulfur in the surface regionmore » of the catalysts, suggesting that these materials are tolerant of sulfur. 42 refs., 11 figs., 7 tabs.« less