NiWS/-γAl_2O_3催化剂上吲哚加氢脱氮反应:H_2S和喹啉的影响  

Hydrodenitrogenation of indole over NiWS/γ-Al_2O_3 catalyst:Effects of H_2S and quinoline

作　　者：张奇[1] 刘春艳[1] 梁长海[1] 何德民[1] 关珺[1] 张秋民[1] 

机构地区：[1]大连理工大学煤化工研究设计所暨精细化工国家重点实验室,辽宁大连116012

出　　处：《燃料化学学报》2011年第5期361-366,共6页Journal of Fuel Chemistry and Technology

基　　金：新世纪优秀人才支持计划(NCET-07-0133)

摘　　要：在连续固定床微反装置上考察了吲哚(IND)和1,2-二氢吲哚(HIN)在NiWS/γ-Al2O3催化剂上加氢脱氮(HDN)的反应以及H2S和喹啉(Q)对其加氢脱氮反应的影响。结果表明,碱性含氮化合物HIN较吲哚对其自身的加氢脱氮反应抑制作用更为明显。H2S能够促进HIN的C(sp3)-N断裂,但抑制了邻乙基苯胺(OEA)的C(sp2)-N断裂;同时吲哚加氢反应途径也受到了抑制。喹啉的添加严重降低了吲哚加氢脱氮反应的转化率和脱氮率;喹啉对吲哚加氢反应和C-N键断裂反应均产生明显的抑制作用。喹啉的抑制作用主要源于喹啉及其中间产物1,2,3,4-四氢喹啉(THQ1)和5,6,7,8-四氢喹啉(THQ5)与吲哚及其中间产物的竞争吸附。Hydrodenitrogenation of indole and 1,2-dihydroindole were performed over a NiWS/γ-Al2O3 catalyst in a continuous fixed-bed microreactor; the effects of HzS, quinoline and its hydrodenitrogenation intermediates on the hydrodenitrogenation of indole were investigated. Compared with indole, 1,2-dihydroindole exhibits obvious self-inhibition effect on the hydrodenitrogenation. H2 S can promote C （ sp3 ） -N bond cleavage in 1,2- dihydroindole and slightly inhibit the hydrogenation reaction and C （sp2） -N bond cleavage in o-ethylaniline due to the competitive adsorption these species. The conversion of indole and denitrogenation efficiency are decreased seriously by adding quinoline into indole, indicating that quinoline inhibits the hydrogenation reaction pathway and C-N bond cleavage. This can be attributed to the stronger adsorption of quinotine and its intermediates such as 1,2,3,4-tetrahydro-quinoline and 5,6,7,8-tetrahydro-quinoline than that of indole.

关 键 词：NiWS/-γAl2O3 加氢脱氮 吲哚 H2S 喹啉 

分 类 号：O643.36[理学—物理化学]