镧氧化物对体相MoP加氢脱氮反应性能的影响  

Influence of Lanthanum Oxide on the Hydrodenitrogenation Performance of Bulk MoP

作　　者：徐艳春 李翔[1,2] 王安杰 遇治权[2] 陈永英 

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116024 [2]辽宁省高校石油化工技术与装备重点实验室,辽宁大连116024

出　　处：《石油学报（石油加工）》2018年第1期115-122,共8页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金(21473017和21673029);国家自然科学基金辽宁省联合基金(U1508205);辽宁省自然科学基金(201602158)项目资助

摘　　要：采用共沉淀法制备了体相MoP催化剂和La2O3改性的MoP催化剂,用XRD、N2物理吸附及TEM等手段对催化剂进行表征。以喹啉及其加氢中间体十氢喹啉(DHQ)为模型含氮化合物,研究了这些催化剂的加氢脱氮反应性能。结果表明,La2O3是MoP催化剂的有效助剂,同时促进了MoP的加氢活性和C—N键断裂活性,但抑制了DHQ的脱氢。当La/Mo摩尔比大于0.2时,增加La2O3含量能够显著提高催化剂的比表面积。La2O3含量过高主要生成LaPO4。La2O3改性的MoP催化剂的活性随La/Mo摩尔比增加而增加。当La/Mo摩尔比大于0.3(催化剂记为La-MoP(0.3))时,继续增加La2O3含量对催化剂活性影响不大。La-MoP(0.3)中活性相分散度高于MoP催化剂,并且活性相主要呈棒状,不同于MoP催化剂的卵石状。催化剂的性能与其比表面积或分散度之间没有直接联系。喹啉在这些催化剂上主要通过DHQ路径脱氮,引入La2O3对喹啉HDN反应的促进作用比对DHQ的HDN反应更为显著。Bulk MoP and La_2O_3-modified MoP catalysts were prepared by a co-precipitation method,and characterized by XRD and N2 physisorption methods.The hydrodenitrogenation(HDN)performances of the catalysts were studied using quinoline and decahydroquinoline(DHQ)as the model nitrogen-containing compounds.The results indicate that La_2O_3 is an effective promoter for the MoP HDN catalyst.It enhances both the hydrogenation activity and the C—N bond cleavage activity of MoP but inhibits the dehydrogenation of DHQ.At La/Mo molar ratio above 0.2,the specific surface area and the dispersion of the catalyst become higher with the increasing of La_2O_3 content.At high La/Mo molar ratio,LaPO4 is the major phase in the catalyst.Thus,the activity of the catalysts is increasing along with the La/Mo molar ratio.At the La/Mo ratio above 0.3(the catalyst is denoted as La-MoP(0.3)),the activity of the catalysts is almost not affected by further increasing the La_2O_3 content.The dispersion of active phase in La-MoP(0.3)is higher than that of MoP.Rod-like and pebble-shaped active phases are observed in La-MoP(0.3)and MoP,respectively.There is no relation between the HDN performances and specific surface areas and the dispersions of the La_2O_3-containing catalysts.The HDN of quinoline over the MoP catalysts occurs mainly through the DHQ pathway,and the HDN of quinoline is significantly enhanced by the addition of La_2O_3 than the HDN of DHQ.

关 键 词：加氢脱氮 MOP 镧氧化物 喹啉 助剂 

分 类 号：TE624.9[石油与天然气工程—油气加工工程]