摘要
由于杂原子的引入,增强了磷酸铝分子筛的酸性,从而影响其催化性能。研究通过改变合成液中过渡金属钴的含量制备杂原子磷酸铝分子筛CoAPO-5,采用XRD、SEM、Py-IR、NH_3-TPD等手段考察杂原子改性对分子筛的结晶效果、晶形、酸位以及酸性位分布等的影响,并以氧化脱除模拟油中苯并噻吩为探针反应,评价其催化脱硫性能。实验结果表明,合成液中n(CoO):n(Al_2O_3)为0.10时制备的CoAPO-5分子筛呈包裹的六棱柱状,粒径为8μm,晶粒均匀,且催化活性较高。在反应温度为40℃、反应时间45 min、V(oil):V(extract):V(oxidant)为1:1:0.1、m(catalyst):m(oil)为1.5%的条件下,苯并噻吩的脱除率达到74.32%。动力学分析表明,苯并噻吩的氧化反应为一级反应,表观活化能Ea为16.96 kJ×mol^(-1)。
Introduction of hetero-atoms into aluminum phosphate molecular sieves can result in the increase of acidity and change of catalytic performance. Effects of cobalt dosage on crystallization, crystal morphology,acid position and acidity distribution of the heteroatom aluminum phosphate molecular sieve CoAPO-5 were investigated by XRD, SEM, Py-IR and NH_3-TPD. Desulfurization performance of CoAPO-5 was evaluated by catalyzing benzothiophene in simulated petroleum. The results show that CoAPO-5 has uniform particle size（8μm） with the highest catalytic activity when prepared under n（CoO）：n（Al_2O_3） = 0.10. Benzothiophene removal rate is 74.32% when studied under conditions of reaction temperature = 40 ℃, reaction time = 45 min,V（oil）：V（extract）：V（oxidant） = 1：1：0.1 and m（catalyst）：m（oil） = 1.5%. Kinetic analysis show that oxidation of benzothiophene is a first order reaction and the apparent activation energy Ea = 16.96 kJ×mol^（-1）.
作者
郑静静
王俊
孙雪妮
韶晖
黄春香
ZHENG Jing-jing;WANG Jun;SUN Xue-ni;SHAO Hui;HUANG Chun-xiang(School of Petrochemical Engineering,Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Changzhou University,Changzhou 213164,China)
出处
《高校化学工程学报》
EI
CAS
CSCD
北大核心
2018年第3期690-695,共6页
Journal of Chemical Engineering of Chinese Universities
基金
江苏省青年科学自然基金(BK20150262)
