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  4. H-MCM-22沸石分子筛中Brφnsted/Lewis酸协同效应的1H和27Al双量子魔角旋转固体核磁共振研究

催化学报 , 2012, 33(1): 129-139. doi: 10.1016/S1872-2067(10)60287-2

H-MCM-22沸石分子筛中Brφnsted/Lewis酸协同效应的1H和27Al双量子魔角旋转固体核磁共振研究

喻志武 1, , 王强 2, , 陈雷 3, , 邓风 4,

1.中国科学院武汉物理与数学研究所,波谱与原子分子物理国家重点实验室,武汉磁共振中心,湖北武汉430071;中国科学院强磁场科学中心,安徽合肥230031

2.中国科学院武汉物理与数学研究所,波谱与原子分子物理国家重点实验室,武汉磁共振中心,湖北武汉430071

3.中国科学院武汉物理与数学研究所,波谱与原子分子物理国家重点实验室,武汉磁共振中心,湖北武汉430071

4.中国科学院武汉物理与数学研究所,波谱与原子分子物理国家重点实验室,武汉磁共振中心,湖北武汉430071

基金项目:   国家自然科学基金(20773159;20933009)  

关键词： H-MCM-22分子筛 , 脱铝 , 酸性 , Brφnsted/Lewis酸协同效应 , 双量子魔角旋转核磁共振

Brφnsted/Lewis Acid Sites Synergy in H-MCM-22 Zeolite Studied by 1H and 27Al DQ-MAS NMR Spectroscopy

采用各种固体核磁共振(NMR)技术详细研究了H-MCM-22分子筛中Brφnsted/Lewis酸的协同效应.二维1H双量子魔角旋转(DQ-MAS) NMR结果表明,在脱铝H-MCM-22分子筛中Brφnsted酸位(骨架桥式羟基)和Lewis酸位(非骨架铝羟基)之间是空间邻近的,暗示着可能存在B/L酸协同效应.二维27A1 DQ-MAS NMR结果揭示了各种铝物种之间的空间邻近性,表明B/L酸协同效应优先发生在H-MCM-22分子筛超笼中的骨架T6位铝和非骨架铝物种之间.2-13C-丙酮探针分子实验发现,因B/L酸协同效应而导致脱铝H-MCM-22分子筛酸性明显增强,氘代吡啶探针分子实验也证实在H-MCM-22分子筛的超笼中发生了B/L酸协同效应.上述结果将有助于我们理解在脱铝H-MCM-22分子筛上发生的多相催化机理.

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