燃料化学学报2018,Vol.46Issue(4):427-440,14.
铜钼组分对γ-Al2O3负载镍催化剂脂肪酸甲酯加氢脱氧性能的影响
Influence of Cu and Mo components ofγ-Al2O3supported nickel catalysts on hydrodeoxygenation of fatty acid methyl esters to fuel-like hydrocarbons
摘要
Abstract
In this work,series of Ni/γ-Al2O3catalysts with or without Cu and Mo components were prepared, characterized and tested for the hydrodeoxygenation of fatty acid methyl esters (FAME) to hydrocarbons. The effects of Cu and Mo loading, impregnation sequence with sequential impregnation and co-impregnation involved and reaction conditions on catalytic performance were investigated. According to the TG data, the spent 20Ni-6Cu/γ-Al2O3catalyst gives less weight loss than the spent 20Ni/γ-Al2O3catalyst, which indicates that the addition of copper inhibits the carbon deposits behavior on catalyst surface during reaction. For 20Ni-6Cu/γ-Al2O3and 20Ni-6Cu-nMo/γ-Al2O3(n=2, 5, 8 and 12) catalysts, NH3-TPD analysis shows that the addition of molybdenum phase has significant impact on the acid sites of γ-Al2O3. When the loading of molybdenum is 5%,a new acid site is observed corresponding to the medium strength acid site. The Cu and Mo modified catalysts demonstrate better catalytic performance than Ni/γ-Al2O3catalysts. Based on XPS results,Cu in the catalysts exists in the Cu2+and Mo in the catalysts has two states:Mo4+and Mo6+,and different impregnation sequences may influence the actual element composition of active phase on the surface of catalysts. In addition, the conversion of FAME and yield of alkane are related to the catalysts prepared with different impregnation sequence. Among all the catalysts, the trimetallic 20Ni-6Cu-5Mo/γ-Al2O3prepared by sequential impregnation (the former Ni and Cu impregnation, the latter Mo impregnation) exhibits optimal catalytic performance. Under appropriate reaction conditions 350℃,2.5 MPa, WSHV= 2.0 h-1, H2/oil ratio=1250 mL/mL, the conversion of FAME and yield of alkane are 98.4% and 94.2%.关键词
加氢脱氧/脂肪酸甲酯/镍基催化剂/γ-Al2O3Key words
hydrodeoxygenation/fatty acid methyl esters/Ni-based catalysts/γ-Al2O3分类
化学化工引用本文复制引用
景仲雨,张韬奇,商江伟,翟明路,杨浩,乔聪震,马新起..铜钼组分对γ-Al2O3负载镍催化剂脂肪酸甲酯加氢脱氧性能的影响[J].燃料化学学报,2018,46(4):427-440,14.基金项目
The project was supported by National Science and Technology Supporting Program(2013BAB11B02)and Science and Technology Development Project of Henan Province(152102210258). (2013BAB11B02)