Preparation and n-hexadecane hydroisomerization properties of SAPO-11-based composite molecular sieve

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Research on Chemical Intermediates Pub Date : 2024-09-27 DOI:10.1007/s11164-024-05393-4
Changmin Tuo, Qinghua Liu, Xianglian Wu, Abulikemu Abulizi, Tiezhen Ren, Aisha Nulahong
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Abstract

In this work, SAPO-11, SAPO-11-γ-Al2O3 and SAPO-11-ZSM-5-γ-Al2O3 molecular sieve supports were prepared by static hydrothermal synthesis, which SAPO-11-γ-Al2O3 and SAPO-11-ZSM-5-γ-Al2O3 supports were loaded with Co and Mo as active metal components. The hydroisomerization properties of n-hexadecane on SAPO-11, SAPO-11-γ-Al2O3 and SAPO-11-ZSM-5-γ-Al2O3 molecular sieves were investigated, as well as the effects of reaction temperature, reaction time, solid–liquid ratio and reaction pressure on the hydroisomerization properties. The results demonstrated that the SAPO-11 molecular sieves synthesized under the ratios of 1Al2O3:2P2O5:0.6TEOS:1.2DPA:55H2O, crystallization time of 48 h, and crystallization temperature of 180 °C had high crystallinity and uniform size distribution, and the pore structure was more obvious. After loading metals onto the SAPO-11-γ-Al2O3 molecular sieves, the charged metals partially block the pores or pore openings of the molecular sieves, leading to a reduction in specific surface area and pore volume. As a result, some acidic sites become occupied by the metals, weakening the acidity. The results of the hydroisomerization experiments showed that the SAPO-11 molecular sieves achieved maximum isoparaffin selectivity and isoparaffin yield, reaching values of 31.26% and 28.32%, respectively, at 340 °C over a reaction time of 60 min. The selectivity and yield reached maximum of 51.02% and 43.76% at liquid–solid ratio up to 25:1. The selectivity and yield reached maximum values of 55.82% and 51.2% at an initial reaction pressure of 5 MPA. For the SAPO-11-γ-Al2O3 supports, the selectivity and yield the maximum values of 79.50% and 71.49% at a metal Co: Mo loading ratio of 1:3 was achieved. For the SAPO-11-ZSM-5-γ-Al2O3 supports, the selectivity and yield the maximum values of 55.44% and 54.05% were achieved with ZSM-5 loading of 30 wt%. These catalysts have the potential for a wide range of applications.

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基于 SAPO-11 的复合分子筛的制备及其正十六烷加氢异构化性能
本研究采用静态水热合成法制备了SAPO-11、SAPO-11-γ-Al2O3和SAPO-11-ZSM-5-γ-Al2O3分子筛载体,并在SAPO-11-γ-Al2O3和SAPO-11-ZSM-5-γ-Al2O3载体上添加了Co和Mo作为活性金属组分。研究了正十六烷在 SAPO-11、SAPO-11-γ-Al2O3 和 SAPO-11-ZSM-5-γ-Al2O3 分子筛上的加氢异构化性能,以及反应温度、反应时间、固液比和反应压力对加氢异构化性能的影响。结果表明,在 1Al2O3:2P2O5:0.6TEOS:1.2DPA:55H2O 的配比、48 h 的结晶时间和 180 °C 的结晶温度下合成的 SAPO-11 分子筛具有较高的结晶度和均匀的粒度分布,孔隙结构较为明显。在 SAPO-11-γ-Al2O3 分子筛上负载金属后,带电金属部分堵塞了分子筛的孔隙或孔口,导致比表面积和孔体积减小。因此,一些酸性位点被金属占据,从而削弱了酸性。加氢异构化实验结果表明,SAPO-11 分子筛在 340 ℃、反应时间为 60 分钟时,异链烷烃选择性和异链烷烃产率达到最大值,分别为 31.26% 和 28.32%。当液固比达到 25:1 时,选择性和产率分别达到 51.02% 和 43.76% 的最大值。在初始反应压力为 5 MPA 时,选择性和产率分别达到最大值 55.82% 和 51.2%。对于 SAPO-11-γ-Al2O3 支持物,当金属 Co:Mo 负载比为 1:3。对于 SAPO-11-ZSM-5-γ-Al2O3 载体,当 ZSM-5 的负载量为 30 wt%时,选择性和产率的最大值分别为 55.44% 和 54.05%。这些催化剂具有广泛的应用潜力。
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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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