Confined-space synthesis of hierarchical MgAPO-11 molecular sieves with good hydroisomerization performance

Confined-space synthesis of hierarchical MgAPO-11 molecular sieves with good hydroisomerization performance
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密闭空间合成具有良好加氢异构性能的多级孔MgAPO-11分子筛

DOI:
10.1016/j.micromeso.2017.11.041
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发表时间:
2018-05
影响因子:
5.2
通讯作者:
Tian Zhijian
Tian Zhijian
中科院分区:
材料科学2区
文献类型:
--
作者:
Tao Shuo;Li Xiaolei;Gong Huimin;Jiang Qike;Yu Wenguang;Ma Huaijun;Xu Renshun;Tian Zhijian

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以磷酸镁铝-碳(MAP-C)复合材料为原料,通过凝胶转化法合成了具有大比表面积和高孔容的多级结构MgAPO-11分子筛。碳膜包覆在非晶磷酸镁铝(MAP)的介孔上,提供了一个限制晶体生长的受限空间。采用XRD、SEM、TEM、N2吸附-脱附、吡啶吸附红外光谱(Py-IR)和固体核磁共振等技术对产物进行了表征。结果表明,在合适的碳负载量下,可以得到结晶度好的高介孔MgAPO-11。随时间变化的研究表明,分级结构MgAPO-11的形成过程遵循一个反向的晶体生长路线:晶化从非晶前驱体的外表面开始,然后向内扩展,最终得到由尺寸约为50 nm的纳米晶体组装而成的分级结构分子筛。与传统的Pt/MgAPO-11催化剂相比,MgAPO-11具有更高的酸性和更好的扩散性能,因此在正十二烷加氢异构化反应中表现出更高的活性和选择性。
Hierarchical MgAPO-11 molecular sieves with large BET surface areas and high pore volumes have been synthesizedviadry-gel conversion of the magnesioaluminophosphate-carbon (MAP-C) composites. The carbon film coated on the mesopores of amorphous magnesioaluminophosphate (MAP) provides a confined-space to restrict the overgrowth of the crystals. The products were well characterized using XRD, SEM, TEM, N2adsorption-desorption, infrared spectroscopy of pyridine adsorption (Py-IR) and solid-state NMR techniques. The results show that highly mesoporous MgAPO-11 with good crystallinity can be obtained at an appropriate carbon loading amount. The time-dependent study indicates that the formation process of hierarchical MgAPO-11 obeys a reversed crystal growth route: crystallization started on the outer surface of the amorphous precursor, then extended to inward, and finally hierarchical molecular sieves assembled by nanosized crystals with a size of about 50 nm were obtained. The catalyst based on hierarchical MgAPO-11 exhibits a significant higher activity and selectivity than the conventional Pt/MgAPO-11 catalyst in the hydroisomerization ofn-dodecane, attributing to its higher acidity and excellent diffusion properties resulting from the hierarchical pore architecture.
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