摘要
以生物柴油生产过程中副产的甘油为原料,通过催化氢解制备1,2-丙二醇是增长生物柴油产业链、提高其经济效益的有效途径.采用浸渍法制备了双金属磁性催化剂Ru-Cu/ Fe3 O4 -TiO2 ,利用X 射线衍射、X 射线光电子能谱、透射电子显微镜、N2 吸附等方法对催化剂进行了表征,考察了Ru/ Cu 摩尔比、反应温度、H2 压力、反应时间和催化剂用量等因素对催化剂性能的影响.结果表明,Ru-Cu/ Fe3 O4 -TiO2 双金属催化剂具有很高的催化活性和良好的1,2-丙二醇选择性.Cu 的加入没有明显改变Ru 的化学环境,但有效地提高了1,2-丙二醇的选择性,同时Ru 可改善Cu 在钛铁复合载体上的分散性,从而获得了平均金属粒径在5-9 nm 左右的催化剂.在Ru/ Cu 摩尔比1 ∶1. 6、反应温度200 ℃、H2 压力4. 0 MPa、反应时间10 h 的条件下,甘油转化率和1,2-丙二醇的选择性分别高达96. 12% 和86. 77%.反应后产物与催化剂可有效实现磁性分离,为该过程的工业化应用奠定了基础.
Hydrogenolysis of glycerol to 1,2-propanediol is one of the most promising routes which can effectively improve the eco-nomic benefit of biodiesel manufacturers. Several Ru-Cu bimetallic catalysts supported on titania-iron oxide were prepared by co-im-pregnation method. The as-prepared catalysts were characterized by X-ray diffraction,X-ray photoelectron spectroscopy,transmission electron microscopy,and N2 adsorption. The effects of Ru/Cu atomic ratio,reaction temperature,H2 pressure,reaction time and cata-lyst amount on the catalytic performance were investigated. The Ru-Cu/Fe3O4-TiO2 bimetallic catalyst showed high activity and good selectivity to 1,2-propanediol. The addition of Cu had no obvious effect on the chemical environment of Ru,but it markedly en-hanced the selectivity towards 1,2-propanediol. Ru could improve the dispersion of Cu on the titania-iron oxide support. The average metal particle size of the catalyst was about 5~9 nm. Under the optimized conditions( Ru/Cu=1:1. 6,200 ℃,4. 0 MPa,and 10 h),the conversion of glycerol and the selectivity to 1,2-propanediol reached 96. 12%and 86. 77%,respectively. The magnetic cata-lysts and reaction products could be easily separated by an external magnetic field,which was beneficial to the industrialization of this process.
出处
《化学研究与应用》
CAS
CSCD
北大核心
2016年第5期629-635,共7页
Chemical Research and Application
基金
国家自然科学基金项目(21302237)资助
重庆市基础与前沿研究计划项目(cstc2014jcyj A90004)资助
重庆科技学院研究生科技创新项目(YKJCX2014040)资助