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高稳定性纳米Y分子筛的合成和表征OA

Synthesis and Characterization of Highly Stable Nano-Sized Y Zeolite

中文摘要英文摘要

纳米Y分子筛因其优异的扩散性能和丰富的外表面酸性位,在炼油领域得到了越来越多的关注,目前合成稳定性较高的纳米Y分子筛仍然存在着较大挑战.开发了一种新型水热晶化合成方法,以廉价阴离子表面活性剂脂肪醇聚氧乙烯醚硫酸铵(AESA)为模板剂,采用多次成胶、多步晶化和后加硅源的水热晶化策略合成了纳米Y分子筛.考察了合成方法、模铝比和钠铝比对分子筛形貌和物化性质的影响,采用粉末X射线衍射(XRD)、X射线荧光光谱(XRF)、N2物理吸附、傅里叶变换红外光谱(FT-IR)、吡啶红外光谱(Py-FTIR)、硅铝固体核磁(29Si MAS NMR、27Al MAS NMR)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和能谱面扫(EDS-mapping)对分子筛进行了表征,并对比了纳米Y和商业Y分子筛的高温水热稳定性.结果表明,在优化的合成条件下,纳米Y分子筛的平均粒径尺寸为83 nm,硅铝摩尔比(SAR)和晶胞参数分别为5.8和24.62 Å,比表面积为887 m2/g,600 ℃水热处理后相对结晶度降低率为16.0%,酸处理后相对结晶度降低率恢复至7.1%.相较商业Y分子筛,纳米Y分子筛脱铝后二次孔结构更为发达(孔径主要分布于10~80 nm),酸性位得到了有效保留,展现出了更好的稳定性,这归因于其较好的骨架完整性和较高的硅铝比.

Nano-sized Y zeolite has attracted increasing attention in the petroleum refining industry due to its excellent diffusion properties and abundant external surface acid sites.However,synthesizing highly stable nanosized Y zeolite still remains challenging.A novel hydrothermal crystallization method was developed using inexpensive anionic surfactant ammonium fatty alcohol ether sulfate(AESA)as a template agent.The synthesis involved a strategy of multiple gel formation steps,multi-stage crystallization,and post-addition of silicon source.The effects of synthesis conditions,AESA/Al2O3 ratio,and Na2O/Al2O3 ratio on the morphology and physicochemical properties of the zeolite were investigated.The synthesized materials were characterized by powder X-ray diffraction(XRD),X-ray fluorescence spectroscopy(XRF),N2 physisorption fourier transform infrared spectroscopy(FT-IR),pyridine-adsorbed FT-IR(Py-FTIR),solid-state NMR(29Si MAS NMR and 27Al MAS NMR),scanning electron microscopy(SEM),transmission electron microscopy(TEM),and EDS-mapping.The hydrothermal stability at high temperatures was compared between the nano-sized Y and commercial Y zeolites.The results demonstrate that under optimized synthesis conditions,the nano-sized zeolite exhibits an average particle size of 83 nm,a silica-alumina ratio(SAR)of 5.8,a unit cell parameter of 24.62 Å,and a specific surface area of 887 m2/g.After hydrothermal treatment at 600℃,the reduction rate of relative crystallinity was 16.0%,which recovered to 7.1%after acid treatment.Compared to commercial Y zeolite,the nano-sized Y zeolite possesses highly developed secondary pore structure(pore size distribution mainly in the 10~80 nm range),retains more acid sites,and exhibits superior stability,which were attributed to its improved framework integrity and higher SAR.

薛景航;秦波;柳伟;张通;谢文杰

中石化(大连)石油化工研究院有限公司,大连 116045中石化(大连)石油化工研究院有限公司,大连 116045中石化(大连)石油化工研究院有限公司,大连 116045中石化(大连)石油化工研究院有限公司,大连 116045中石化(大连)石油化工研究院有限公司,大连 116045

化学化工

Y分子筛纳米高稳定性

Y zeoliteNano-sizedHigh stability

《应用化学》 2026 (3)

373-386,14

国家自然科学基金联合基金项目(No.U24A202895)资助 Supported by the Joint Funds of the National Natural Science Foundation of China(No.U24A202895)

10.19894/j.issn.1000-0518.250291

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