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作 者:姚云龙 遇治权[1,2] 孙志超 刘颖雅[1,2] 王安杰 YAO Yunlong;YU Zhiquan;SUN Zhichao;LIU Yingya;WANG Anjie(State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, China;Liaoning Key Laboratory of Petrochemical Technology and Equipment, Dalian University of Technology, Dalian 116024, China)
机构地区:[1]大连理工大学精细化工国家重点实验室,辽宁大连116024 [2]大连理工大学辽宁省省级高校石油化工技术与装备重点实验室,辽宁大连116024
出 处:《大连理工大学学报》2020年第5期477-485,共9页Journal of Dalian University of Technology
基 金:国家自然科学基金资助项目(21972014,21603024,21872014,U1508205);科技部政府间国际科技创新合作重点专项(2016YFE0109800);中央高校基本科研业务费专项资金资助项目(DUT19GJ205)。
摘 要:通过程序升温还原制备了非负载过渡金属磷化物(MoP、Ni3P、Ni12P5、Ni2P、Fe2P、FeP、Co2P和CoP),以异丙醇为溶剂,在固定床反应器中考察其在糠醛选择性加氢反应中的催化性能.MoP表现出最佳的催化活性,糠醛转化率和2-甲基呋喃选择性分别为96.9%和91.5%.通过NH3程序升温脱附、N2物理吸附脱附、透射电子显微镜和X射线光电子能谱等表征手段对MoP催化剂进行表征.2-甲基呋喃的高选择性与糠醛在金属位点上适宜的加氢性能以及P的引入提高了糠醇氢解能力有关.研究了反应条件(反应温度、反应压力和接触时间)对催化性能的影响,并考察了糠醛在MoP上加氢脱氧性能的稳定性,发现MoP催化剂表面积碳会导致反应活性逐渐下降.Unsupported transition metal phosphides,including MoP,Ni3P,Ni12P5,Ni2P,Fe2P,FeP,Co2P and CoP are prepared by temperature-programmed reduction method,and their catalytic performance in selective hydrogenation of furfural is tested in a fixed bed reactor using isopropanol as the solvent.Among them,MoP exhibits the highest catalytic performance,with furfural conversion of 96.9%and selectivity to 2-methylfuran of 91.5%.The MoP catalyst is characterized by means of NH3 temperature-programmed desorption,N2 adsorption-desorption,transmission electron microscope,and X-ray photoelectron spectroscopy.The high yield to 2-methylfuran is attributed to the appropriate hydrogenation ability of the metal sites and to the enhanced hydrogenolysis ability of furfural alcohol by the introduction of phosphorous species.The effects of temperature,pressure,and contact time on the catalytic performance of MoP are investigated.It is found that MoP catalyst undergoes gradual deactivation in the course of the selective hydrogenation,probably because of coke formation.
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