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作 者:姚敏[1] 王燕娣 卢美贞[1] 计建炳[1] 刘学军[1] YAO Min;WANG Yan-di;LU Mei-zhen;JI Jian-bing;LIU Xue-jun(Zhejiang Province Key Laboratory of Biofuel Utilization Technology,Biodiesel Laboratory of China Petroleum and Chemical Industry Federation,School of Chemical Engineering,Zhejiang University of Technology,Hangzhou 310014,China)
机构地区:[1]浙江工业大学石油和化工行业生物柴油技术工程实验室浙江省生物燃料利用技术研究重点实验室化学工程学院
出 处:《燃料化学学报》2019年第12期1450-1457,共8页Journal of Fuel Chemistry and Technology
摘 要:采用NiMoP浸渍液中添加乙二醇(EG)的方式制备了不同EG含量的NiMoP(x)/Al2O3催化剂,为研究EG及其含量对该系列催化剂催化性能和活性相结构的影响,用二苯并噻吩(DBT)和喹啉(Q)为模型化合物,考察了催化剂的加氢脱硫(HDS)和加氢脱氮(HDN)性能。结果表明,在EG添加量较低的情况下(EG/Ni物质的量比分别为0、0.5、1、2、3),EG能够明显提高催化剂对DBT和Q的HDS和HDN活性,其中,HDN活性提高幅度大于HDS,且随着EG含量提高,催化剂的HDS和HDN活性进一步提高。通过TEM分析和XPS分析可知,EG有助于增加催化剂中MoS2颗粒的堆积层数和片层长度,且随着EG含量增加,堆积层数和片层长度都有所增加;EG有助于提高Mo表面原子浓度,对Ni表面原子浓度影响较小,但明显提高了Mo和Ni硫化程度。TG表征说明,EG在氧化铝和催化剂表面存在多种相互作用方式,并且存在与活性组分相互作用的耐高温有机物种。The PdMoP/γ-Al2O3 catalyst was prepraed through loading the Pd, Mo, and P elements on the γ-Al2O3 support by incipient impregnation method and characterized by XRD, NH3-TPD, XPS, Py-FTIR, nitrogen physisorption and STEM-EDS. The catalytic performance of PdMoP/γ-Al2O3 in the hydrodeoxygenation of soybean oil methyl ester to alkane biodiesel was invetigqated and the operation conditions were optimized. The results show that a combination of Pd, Mo and P elements can effectively adjust the catalyst acidity;Mo can reduce strong acidity, whereads P can enhance weak acidity, leading to a decrease in the B/L ratio of weak acid sites and a slight increase in the B/L ratio of strong acid sites. The optimized hydrodeoxygenation conditions are 315 ℃, 1.5 MPa, WHSV = 0.5 h-1, and V(hydrogen)/V(esters) = 1100;under such conditions, the conversion of soybean oil methyl esters reaches 98.4% and the C15-18 alkane yield is 91.5%.
关 键 词:加氢脱氧 PdMoP/γ-Al2O3催化剂 酸性调节 大豆油甲酯 烷烃类生物柴油
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