Francisco J. Machado, Carmen M. López, José Goldwasser, Bernardo Méndez, Yván Campos, Douglas Escalante, Miguel Tovar, María M. Ramírez-Agudelo
{"title":"光谱和催化证据的结合镓在AEL框架","authors":"Francisco J. Machado, Carmen M. López, José Goldwasser, Bernardo Méndez, Yván Campos, Douglas Escalante, Miguel Tovar, María M. Ramírez-Agudelo","doi":"10.1016/S0144-2449(97)00113-9","DOIUrl":null,"url":null,"abstract":"<div><p><sup>71</sup>Ga <em>MAS</em> n.m.r. analysis and the catalytic behavior during the transformation of 1-butene and <em>n</em>-butane strongly suggest the incorporation of Ga into the AlPO<sub>4</sub>-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 AlPO<sub>4</sub>-11 and SAPO-11 during the skeletal isomerization of <em>n</em>-butenes reinforces the idea of an isomorphous substitution of Al(III) by Ga(III) in the AEL framework. The transformation of <em>n</em>-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.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 387-394"},"PeriodicalIF":0.0000,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00113-9","citationCount":"11","resultStr":"{\"title\":\"Spectroscopic and catalytic evidence for the incorporation of gallium in the AEL framework\",\"authors\":\"Francisco J. Machado, Carmen M. López, José Goldwasser, Bernardo Méndez, Yván Campos, Douglas Escalante, Miguel Tovar, María M. Ramírez-Agudelo\",\"doi\":\"10.1016/S0144-2449(97)00113-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p><sup>71</sup>Ga <em>MAS</em> n.m.r. analysis and the catalytic behavior during the transformation of 1-butene and <em>n</em>-butane strongly suggest the incorporation of Ga into the AlPO<sub>4</sub>-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 AlPO<sub>4</sub>-11 and SAPO-11 during the skeletal isomerization of <em>n</em>-butenes reinforces the idea of an isomorphous substitution of Al(III) by Ga(III) in the AEL framework. The transformation of <em>n</em>-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.</p></div>\",\"PeriodicalId\":23983,\"journal\":{\"name\":\"Zeolites\",\"volume\":\"19 5\",\"pages\":\"Pages 387-394\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"1997-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00113-9\",\"citationCount\":\"11\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Zeolites\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0144244997001139\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Zeolites","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0144244997001139","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
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.