【作者】 裴小科；

【导师】 林碧洲；

【作者基本信息】 华侨大学 ， 材料物理与化学， 2005， 硕士

【摘要】 柱撑二硫化钼复合材料是用人工合成方法,使无机或有机分子（离子）插入MoS₂层间组装复合而成的一种新功能材料。它具有各向异性、电学、磁学、催化等性能,在电极材料、石油化工、环境保护等方面有着广阔的应用前景。本文采用了单分子层剥离-重堆积技术,以无机聚合羟基铝离子为客体,制备铝柱撑二硫化钼复合材料,并采用XRD、DSC、SEM、IR、UV-Vis DRS、BET、EDS等分析手段对材料进行结构和性能表征。研究表明,铝柱撑二硫化钼的层间距从1.481到1.521 nm,客体Keggin离子以三重轴垂直于主体板层的取向位于主体二硫化钼层间域中:采用稀浓度的柱撑液和较低Al/MoS₂物质的量比的柱撑反应体系对制备层间距较大的铝柱撑二硫化钼有利:与原料2H-MoS₂相比,柱撑材料的层间距增大,晶粒变小,比表面积增加。通过取代反应,将铁、镍引入Keggin离子而制备的铁铝、镍铝柱撑二硫化钼的层间距分别为1.394至1.513 nm和1.211至1.472 nm,而且柱撑材料的层间距随着Fe/（Al+Fe）、Nil（Al+Ni）物质的量之比的增加而逐渐降低。 在此基础上,本文开展了所得的柱撑材料对二价硫离子的催化、光催化氧化性能研究。研究表明,柱撑材料可将S^2-催化氧化为S₂O₃^2-,其催化、光催化氧化活性是原料2H-MoS₂的3～8倍,且光催化活性大于催化活性。柱撑材料催化氧化活性的提高与其晶粒尺寸变小、比表面积增大以及可能存在的缺陷和晶格畸变有关。而在光照条件下催化氧化活性较高则与材料所含的2H-MoS2板层的半导体性质有关。此外,加入Fe、Ni后,材料的催化、光催化氧化活性得到较大的改善。更多还原

【Abstract】 Molybdenum disulfide composite materials pillared by inorganic or organic molecules（or ions） are provided with the properties of anisotropy, electricity, magnetism, catalysis and so on, which are expected to make them apply in the several areas such as electrode materials, petrochemical industry and environment protection. Due to the insufficient researches in molybdenum disulfide composites pillared by inorganic guests, the pillared nanocomposites were prepared by intercalating the hydroxy-Al oligocations into the interlayers of the molybdenum disulfide host sheets through the single-molecular-layer exfoliated-restacked technology. The structures and properties of the pillared composites were investigated by means of XRD, DSC, SEM, IR, UV-Vis, DRS, BET, EDS etc. The results showed that the basal interlayer spacings of the pillared composites are from 1.481 to 1.521 run, where the intercalated Keggin species are arranged in a mono-layer fashion between the molybdenum disulfide sheets with their C₃ symmetry axes perpendicular to the host sheets. It was revealed that a lower concentration of pillaring agents and a lower ratio of Al/MoS₂ in reaction system will result in a larger interlayer spacing. Compared with the pristine 2H-M0S2, the pillared nanocomposites exhibit larger interlayer spacings, smaller crystallite sizes and larger specific surface areas. Hydroxy-Fe-Al and -Ni-Al oligocations with a Keggin structure, prepared by a substitution reaction, were intercalated into the molybdenum disulfide host interlayers, and the pillared composites possess the basal interlayer spacings from 1.394 to 1.513nm and 1.211 to 1.472 nm, respectively. It was shown that the interlayer spacings of the pillared composites decrease with the increasing of Fe/Al and Ni/Al molar ratio.The catalytic and photocatalytic activities of the as-prepared pillared composites were studied in the oxidization of sulfide ions. The experimental results indicated that the pillared composites exhibit good catalytic activities in the oxidization of sulfide ions into thiosulfate ions, being three to eight times higher than that of the pristine 2H-MoS₂. The catalytic activities are enhanced upon irradiation with visible light owing to the semiconducting 2H-MoS₂ matrix. The results are related to their smaller crystallite sizes, larger specific surface areas, the existence of the defects and the lattice distortion. It was illustrated that the catalytic activities are improved by introducing the iron and nickel into the pillared composites.更多还原