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| 硬模板法制备微孔-介孔复合SAPO-11分子筛及其长链烷烃异构化反应 |
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刘 振1,2, 马志鹏1,2, 孙常庚1,2, 李婷婷1,2, 宋 浩1,2, 阎子峰1,2
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(1.中国石油大学重质油国家重点实验室,山东青岛 266580;2.中国石油大学CNPC催化重点实验室,山东青岛 266580)
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| 摘要: |
| 以常规SAPO-11分子筛水热合成方法为基础,在分子筛晶化过程中加入一定量的炭黑颗粒作为硬模板构造介孔结构,得到具有微孔-介孔复合结构的SAPO-11分子筛。考察不同碳模板含量对所得分子筛中介孔容量和表面酸性质的影响,并利用N2吸脱附测试、X-射线衍射(XRD)和透射电镜(TEM)和吡啶吸附红外光谱(Py-FTIR)对所得分子筛的晶体结构、孔结构和酸类型进行分析。以正十二烷作为模型化合物,对负载0.5％ Pt 的SAPO-11分子筛的异构化反应催化性能进行评价。结果表明:随着碳模板加入量的增加,分子筛介孔容量先增加后降低,在10％时达到最大;适量碳模板的加入并没有影响分子筛的晶体结构;分子筛中有明显介孔结构产生;异构化反应结果显示催化剂活性与分子筛介孔容量以及表面酸类型相关:一方面,介孔孔容增大可以降低传质阻力,暴露更多孔口活性位,从而提高异构化催化活性;另一方面,提高分子筛孔道内B酸和L酸比值,有利于提高异构化反应的异构化选择性;随着反应温度升高转化率升高,但选择性明显下降。 |
| 关键词: SAPO-11分子筛 微-介复合结构 硬模板 碳材料 临氢异构 |
| DOI：10.3969/j.issn.1673-5005.2014.02.024 |
| 分类号:TQ 032.4 〖HTH〗 |
| 基金项目:国家自然科学基金项目(21206196);山东省优秀中青年科学家奖励基金项目(BS2012NJ013);中央高校基本科研业务费专项(27R1204003A) |
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| Synthesis of meso-microporous SAPO-11by hard template method and its catalytic application for long-chain alkanes hydroisomerization |
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LIU Zhen1,2, MA Zhi-peng1,2, SUN Chang-geng1,2, LI Ting-ting1,2, SONG Hao1,2, YAN Zi-feng1,2
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(1.State Key Laboratory of Heavy Oil Processing in China University of Petroleum, Qingdao 266580, China;2.CNPC Key Laboratory of Catalysis in China University of Petroleum, Qingdao 266580, China)
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| Abstract: |
| Hierarchically SAPO-11zeolite with meso-microporous structures (meso-SAPO-11) was synthesized by adding carbon black as a hard template in crystallization process of traditional hydrothermally prepared method. The effect of different amounts of carbon addition on the mesoporous volume and acid property was evaluated. N2adsorption/desorption isotherm, XRD, TEM and Py-FTIR characterization were employed to identify the crystalline structures, pore properties, and acid types. Catalytic hydroisomerization performances of Meso-SAPO-11catalysts with 0.5% Pt loading were evaluated by using n-C12 as a model compound. It is found that the mesoporous volume shows a parabolic tendency with the increasing amount of carbon addition, and the volume reaches the highest at the 10% addition of carbon. No significant change on crystalline structure is observed by XRD pattern, and obvious mesoporous structure is presented by TEM images. The results of hydroisomerization test demonstrate that the catalytic performance is related to the mesoporous volume and acid property of SAPO-11zeolite:on one hand, increasing the mesoporous volume in microporous SAPO-11can increase the speed of mass transfer, as well as expose more activated microporous pores to enhance the isomerization activity; on the other, raising the ratio of Brnsted acid to Lewis acid can also enhance the hydroisomerization activity. Reaction temperature investigation shows that isomer products selectivities remarkably decrease with the increase of the reaction temperature. |
| Key words: SAPO-11 meso-microporous structure hard template carbon material hydroisomerization |
