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作 者:张进飞[1] 林碧洲[1] 许百环[1] 孙东亚[1] 耿凤[1]
机构地区:[1]华侨大学材料物理化学研究所,福建泉州362021
出 处:《催化学报》2006年第1期29-35,共7页
基 金:国家自然科学基金资助项目(50172016).
摘 要:采用单分子层技术将羟基铝聚合物Al7+13阳离子嵌入到二硫化钼板层间,得到层间距为1.488~1.599nm的柱撑复合材料.X射线粉末衍射等研究表明,羟基铝聚合物Al7+13经60℃恒温陈化2d即可作为稳定的柱撑液使用;在柱撑反应体系中,较小的Al/Mo摩尔比有利于获得客体物种较均一和结晶度较好的柱撑复合材料.与原料2HMoS2相比,柱撑二硫化钼的层间距增大,晶粒变小,比表面积增加.差示扫描量热分析结果表明,柱撑材料具有较好的热稳定性.选择苯饱和加氢反应为探针,测定了柱撑材料的催化活性.气相色谱测定结果表明,柱撑二硫化钼的催化性能显著优于未柱撑的2HMoS2和RaneyNi催化剂.这与柱撑材料比表面积的增大、可能存在的缺陷增多而导致活性位增多以及对氢气的有效吸附增加有关.The molybdenum disulfide composite material pillared by hydroxy-aluminum oligocations, [Al13O4- (OH)24 (H2O)12 ]^7+ (denoted as Al13^7+ ), with the basal interlayer space from 1. 488 to 1. 599 nm was prepared by intercalating Al13^7+ into the interlayers of molybdenum disulfide through the single-molecular-layer technology. The pillared composite was characterized by X-ray diffraction and differential scanning calorimetry (DSC). The results showed that Al13^7+; can be used as a stable pillaring agent after aging at 60℃ for two days, and a pillared composite with uniform pillared species and high crystallinity can be obtained at a smaller molar ratio of Al/Mo in the reaction system. Compared with the pristine 2H-MoS2, the pillared composite exhibited larger interlayer space, smaller crystallite size, and larger specific surface area. The DSC test showed that the pillared composite had better thermal stability. The liquid phase benzene hydrogenation was used as the probe reaction to examine the catalytic activity of the pillared composite. The gas chromatography test showed that the catalytic activity of the pillared composite was evidently superior to that of the pristine 2H-MoS2 and the Raney Ni catalysts widely used in industry. This was attributed to the more catalytically active sites derived from the larger surface area and more defects of the materials, and the effective adsorption of hydrogen.
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