光谱和催化证据的结合镓在AEL框架

Francisco J. Machado, Carmen M. López, José Goldwasser, Bernardo Méndez, Yván Campos, Douglas Escalante, Miguel Tovar, María M. Ramírez-Agudelo
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引用次数: 11

摘要

在GaAPSO-11的合成过程中,Ga在AlPO4-11 (AEL)框架中被掺入。在+120 ppm左右,一个独特的清晰信号被提出与未修饰的GaAPSO-11的AEL框架中四面体Ga的存在有关。结构Ga原子迁移到AEL框架的硅畴似乎是温和水热处理的结果,在+156 ppm时产生额外的信号,以前与具有MFI拓扑结构的低硅硅酸盐中的四面体镓有关。在正丁烯的骨架异构化过程中,GaAPO-11和GaAPSO-11的行为方式与它们的对应物AlPO4-11和SAPO-11相似,这一事实加强了在AEL框架中Al(III)被Ga(III)同构取代的观点。正丁烷的转化被证明是检测Ga负载的SAPO-11 (Ga/SAPO-11)中存在少量氢化脱氢的框架外镓(EFGS)的有价值的测试。GaAPSO-11样品对这种转变完全不活跃,这一事实使我们相信镓在AEL框架四面体位置的结合几乎完成了。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Spectroscopic and catalytic evidence for the incorporation of gallium in the AEL framework

71Ga MAS n.m.r. analysis and the catalytic behavior during the transformation of 1-butene and n-butane strongly suggest the incorporation of Ga into the AlPO4-11 (AEL) framework during the synthesis of GaAPSO-11. A unique clear signal at around +120 ppm is proposed to be associated with the presence of tetrahedral Ga in the AEL framework of the unmodified GaAPSO-11. Migration of structural Ga atoms to the silicon domain of the AEL framework seems to occur as a result of a mild hydrothermal treatment, giving rise to an additional signal at +156 ppm, previously associated with tetrahedral gallium in gallosilicates with the MFI topology. The fact that GaAPO-11 and GaAPSO-11 behaved in a way similar to their counterparts AlPO4-11 and SAPO-11 during the skeletal isomerization of n-butenes reinforces the idea of an isomorphous substitution of Al(III) by Ga(III) in the AEL framework. The transformation of n-butane was shown to be a valuable test for detecting the presence of small amounts of hydro-dehydrogenating extraframework gallium species (EFGS) in Ga-supported SAPO-11 (Ga/SAPO-11). The fact that the sample of GaAPSO-11 was completely inactive for this transformation leads us to believe that the incorporation of gallium into the tetrahedral positions of the AEL framework was almost complete.

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