燃料化学学报2018,Vol.46Issue(1):75-83,9.
金属助剂对Ni/SiO2催化剂苯甲醚加氢脱氧性能的影响
Influence of metallic promoters on the performance of Ni/SiO2 catalyst in the hydrodeoxygenation of anisole
摘要
Abstract
Ni/SiO2 and Ni-based bimetallic Ni30 M/SiO2 catalysts ( with a Ni/M atomic ratio of 30; M = Fe, Co, Cu, Zn and Ga) were prepared by the impregnation method and characterized by the means of H2-TPR, XRD, H2 chemisorption, NH3-TPD and N2 sorption;the effect of M promoters on the structure and performance Ni-based catalysts in the hydrodeoxygenation of anisole was investigated. The results indicated that the metallic promoters have a significant influence on the reducibility of nickel species, due to the interaction between M and Ni species, although the sizes of Ni-M bimetallic crystallites in Ni30 M/SiO2 are similar to that of Ni crystallite in Ni/SiO2 . Because of the interaction between Ni and M and the enrichment of certain M promoters on the surface of Ni-M bimetallic particles, the adsorption quantity of H2 on Ni30 M/SiO2 is lower than that on Ni/SiO2 . In addition, the Ni30 M/SiO2 catalysts also have more acid sites ( especially the weak ones) than Ni/SiO2 . For the hydrodeoxygenation of anisole under 300 ℃, 0. 1 MPa, weight hourly space velocity ( WHSV) of anisole of 1. 0 h-1 and H2/anisole molar ratio of 25, the Ni30 M/SiO2 catalysts exhibit lower anisole conversion than Ni/SiO2 , probably due to the lower H2 uptakes on the bimetallic catalysts. However, Ni30 Ga/SiO2 and Ni30 Zn/SiO2 give much higher selectivities to BTX (benzene, toluene and xylene) (81. 7% and 76. 8%, respectively) than Ni/SiO2(71. 5%). Meanwhile, Ni30 Zn/SiO2 exhibits higher activity in methyl transfer and lower activity in C-C bond hydrogenolysis than other catalysts; owing to the high oxophilicity of Zn, from the aspects of increasing carbon yield and reducing H2 consumption, Ni30 Zn/SiO2 is probably an appropriate catalyst in hydrodeoxygenation.关键词
镍基催化剂/金属助剂/苯甲醚/加氢脱氧/C-C键氢解/甲烷化Key words
Ni-based catalyst/metallic promoter/anisole/hydrodeoxygenation/hydrogenolysis/methanation分类
化学化工引用本文复制引用
李风旭,王晓菲,郑莹,陈吉祥..金属助剂对Ni/SiO2催化剂苯甲醚加氢脱氧性能的影响[J].燃料化学学报,2018,46(1):75-83,9.基金项目
The project was supported by the National Natural Science Foundation of China (21576193).国家自然科学基金(21576193)资助 (21576193)