燃料化学学报2017,Vol.45Issue(11):1332-1339,8.
配合物的配位基团性质对CoMo/γ-Al2O3催化剂加氢脱硫性能的影响
Effect of coordinating groups of chelating agents on the hydrodesulfurization over CoMo/γ-Al2 O3 catalysts
摘要
Abstract
The modified CoMo/γ-Al2 O3 catalyst was prepared by addition of ethylene diamine ( EN ) , ethanolamine ( EA) , ethylene glycol ( EG) or malonic acid ( MA) . The effect of four bidentate molecules with different coordination groups on the dibenzothiophene HDS was compared. And the catalytic activity is determined in the sequence of CoMo ( EN )>CoMo ( EA )>CoMo ( EG )≈CoMo ( MA )>CoMo. For all catalysts, the direct desulfurization route is dominated, but with the increase of reaction temperature, the desulfurization by hydrogenation route become more apparent. Chelating agents facilitate the HDS reaction through hydrogenation route. CoMo ( EN) catalyst presents the highest hydrogenation ability. The catalysts were characterized by UV-vis, EA, XPS and HRTEM. The results show that NH2 group has a strong complexing interaction with Co2+. COOH group mainly has an electrostatic interaction with cobalt ion. Meanwhile, OH group hardly interacts with Co2+. It is noted that the HDS activity is directly related to the interaction between coordinating groups and Co2+. The combination of coordinating molecules with Co2+ leads to the effective formation of Co-Mo-S active center, and the carbonization of chelating decreases the interaction of the support with active phases, facilitating the formation of type II active phases which has a higher intrinsic catalytic activity.关键词
有机配合物/双齿配位分子/CoMo/γ-Al2O3/加氢脱硫/二苯并噻吩Key words
organic chelating agent/bidentate molecule/CoMo/γ-Al2 O3/hydrodesulfurization/dibenzothiophene分类
化学化工引用本文复制引用
韩文鹏,张晔,李学宽,唐明兴,周立公,吴明红,葛晖..配合物的配位基团性质对CoMo/γ-Al2O3催化剂加氢脱硫性能的影响[J].燃料化学学报,2017,45(11):1332-1339,8.基金项目
The project was supported by the National Natural Science Foundation of China (21473231) and National Natural Science Foundation of China(21603256).国家自然科学基金 (21473231),国家自然科学基金青年基金 (21603256)资助 (21473231)