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通过老化处理调节分级 SAPO-11 沸石的酸度、孔隙率和形态。

Regulating acidity, porosity, and morphology of hierarchical SAPO-11 zeolite by aging treatment.

机构信息

State Key Laboratory for Heavy Oil Processing, Key Laboratory of Catalysis, CNPC, China University of Petroleum, Qingdao 266580, China.

State Key Laboratory for Heavy Oil Processing, Key Laboratory of Catalysis, CNPC, China University of Petroleum, Qingdao 266580, China.

出版信息

J Colloid Interface Sci. 2016 Oct 1;479:55-63. doi: 10.1016/j.jcis.2016.06.045. Epub 2016 Jun 21.

Abstract

A facile method to modify pore structure, acidic character, and morphology of SAPO-11 molecular sieve was proposed. Aging treatment (e.g., microwave irradiation or lyophilization) is introduced in the preparation of dry gel. It regulates the kinetics of zeolitic nucleation and growth. X-ray diffraction, scanning electron microscopy, N2-adsorption, temperature programmed desorption, laser particle analyzer, and (29)Si MAS NMR were employed to investigate the effects of aging treatments on SAPO-11 products. The experimental results indicate that depolymerization reaction of silicon species is enhanced aged by microwave irradiation with a higher temperature (90°C). Ratio of SM 3 to SM 2 substituting mode increases producing more strong Brønsted acid sites. Lyophilization technology, as another aging method, was employed to control the morphology of SAPO-11. Nano-sized hierarchical SAPO-11 molecular sieve (200nm in length) is obtained with an oriented growth. Activity of hydroisomerization catalysts is regulated by aging treatment. Cracking reaction attributes to a high conversion nearly 87wt% for M90. The hydroisomerization reaction is enhanced for M40 due to a large proportion of moderate acid sites.

摘要

提出了一种简便的方法来修饰 SAPO-11 分子筛的孔结构、酸性和形貌。在干凝胶的制备中引入老化处理(如微波辐射或冻干),以调节沸石成核和生长的动力学。采用 X 射线衍射、扫描电子显微镜、N2 吸附、程序升温脱附、激光粒度分析仪和(29)Si MAS NMR 研究了老化处理对 SAPO-11 产物的影响。实验结果表明,微波辐射可以提高硅物种的解聚反应温度(90°C),从而增强其老化作用。SM3 取代 SM2 的比例增加,产生更多的强 Brønsted 酸位。冻干技术作为另一种老化方法,用于控制 SAPO-11 的形貌。得到了具有定向生长的纳米级分级 SAPO-11 分子筛(长 200nm)。老化处理调节了加氢异构化催化剂的活性。M90 的高转化率(近 87wt%)归因于裂化反应。M40 的加氢异构化反应增强,因为中等酸位的比例较大。

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