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机构地区:[1]中国石油化工股份有限公司上海石油化工研究院,上海201208
出 处:《化学反应工程与工艺》2011年第6期481-487,共7页Chemical Reaction Engineering and Technology
基 金:国家自然科学基金石油化工联合基金资助项目(20736011)
摘 要:采用X射线粉末衍射(XRD)和扫描电镜(SEM)手段研究了合成条件对高岭土微球上原位晶化ZSM-5沸石的影响,并以含C5~C12烃的石脑油为原料,在固定流化床上评价了不同催化剂的催化裂解性能。结果发现,采用转动晶化方式,控制合适的原料组成与晶化时间,能得到结构完整的含纯相ZSM-5沸石的高岭土微球。对比催化剂水热老化前后的XRD,氨气程序升温脱附(NH3-TPD)和N2吸附-脱附以及石脑油催化裂解结果,发现磷元素改性能有效提高催化剂的水热稳定性,而且原位法制备的催化剂比半合成法制备的催化剂具有更高的水热稳定性。在650℃,常压,进料水油质量比1:1,质量空速1 h-1的条件下,在老化后的原位型催化剂作用下,石脑油的转化率达41.0%,乙烯和丙烯总收率达21.0%,均高于相同条件下半合成型催化剂的反应结果。The effects of synthesis conditions on in-situ crystallization of ZSM-5 zeolite on Kaolin microspheres were investigated by means of X-ray diffraction(XRD) and scanning electron microscope(SEM).The catalytic cracking properties of the catalysts for naphtha with C5-C12 hydrocarbon were also investigated in a fixed fluidized bed.The results showed that integrated Kaolin microspheres with pure ZSM-5 zeolite could be prepared by rotary crystallization mode through adjusting material composition and crystallization time.The comparison of XRD,temperature-programmed desorption(NH3-TPD),N2 adsorption-desorption and naphtha cracking results of catalysts before and after steam aged indicated that the phosphorus modification effectively improved the hydrothermal stability of catalysts and the in-situ catalyst exhibited superior hydrothermal stability to semi-synthesized catalyst.Under the conditions of 650 ℃,mass hourly space velocity(WHSV) 1.0 h-1 and mass ratio of water to oil 1.0,high conversion of naphtha(41.0%) and high yield of ethylene-plus-propylene(21.0%) were achieved over the steam aged in-situ catalyst.
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