Electrocatalytic Reduction of CO2 to Ethylene by Molecular Cu‐Complex Immobilized on Graphitized Mesoporous Carbon

The electrochemical reduction of carbon dioxide (CO₂) to hydrocarbons is a challenging task because of the issues in controlling the efficiency and selectivity of the products. Among the various transition metals, copper has attracted attention as it yields more reduced and C2 products even while using mononuclear copper center as catalysts. In addition, it is found that reversible formation of copper nanoparticle acts as the real catalytically active site for the conversion of CO₂ to reduced products. Here, it is demonstrated that the dinuclear molecular copper complex immobilized over graphitized mesoporous carbon can act as catalysts for the conversion of CO₂ to hydrocarbons (methane and ethylene) up to 60%. Interestingly, high selectivity toward C2 product (40% faradaic efficiency) is achieved by a molecular complex based hybrid material from CO₂ in 0.1 m KCl. In addition, the role of local pH, porous structure, and carbon support in limiting the mass transport to achieve the highly reduced products is demonstrated. Although the spectroscopic analysis of the catalysts exhibits molecular nature of the complex after 2 h bulk electrolysis, morphological study reveals that the newly generated copper cluster is the real active site during the catalytic reactions.     

介孔-大孔结构无定形硅-铝催化剂的核磁共振研究

合成了具有介孔-大孔双模型分级结构的无定形硅-铝催化剂,利用硅和铝核的固体魔角核磁共振谱,考察了合成样品中硅和铝结构上的原子特征.     

介孔氧化铁对正辛醇乙氧基化反应的催化性能

以十二烷基磺酸钠为模板剂、乙二胺为碱性介质,将水热法合成的氧化铁/十二烷基磺酸钠复合中孔材料在550℃、空气气氛中煅烧10h,除去模板剂,得到介孔氧化铁。通过X射线衍射、氮气吸附-脱附方法对介孔氧化铁的晶体结构和表面物性进行表征。表征结果显示,煅烧后的介孔氧化铁具有典型的六方介孔的结构特征,平均孔径为5.4nm。将介孔氧化铁用于催化正辛醇乙氧基化反应,研究结果表明,升高反应温度和初始压力、增加催化剂用量,可加快环氧乙烷的反应速率,同时产物的相对分子质量分布较窄。当平均聚合度为6.5时,正辛醇聚氧乙烯醚相对分子质量分布的选择性系数达到21.1。     

催化裂化原位降硫助剂的制备及其性能研究

采用溶胶-凝胶法制备具有介孔结构的降硫基质材料，选择具有降硫选择性的活性元素对合成的基质材料进行改性处理，考察不同的改性方法对制得的催化裂化原位降硫助剂性能的影响，并对基质材料和降硫助剂的结构进行表征。采用美国进口的ACE-R小型催化裂化评价装置将降硫助剂与催化裂化催化剂匹配进行性能评价，在不改变原催化裂化产品分布和产品性质的同时，降低原料的总硫含量，总硫降低可达40％以上。     

A Silicon–Silica Nanocomposite Material

The synthesis and characterization of a novel silicon–silica nanocomposite material are reported. A self‐assembly method allows the encapsulation of silicon nanoclusters within the channels of a periodic mesoporous silica thin film. The result is the formation of a silicon–silica nanocomposite film with bright, room‐temperature photoluminescence in the visible range, and a nanosecond luminescence lifetime. The properties of the nanocomposite material have been studied by several analytical techniques, which collectively show the existence within the channels of non‐diamondoid‐structure‐type silicon nanoclusters with various hydrogenated silicon sites. It is estimated that the silicon nanoclusters in the silica mesoporous films occupy up to 39 % of the accessible pore volume. The nanocomposite film shows improved resistance to air oxidation compared to crystalline silicon. The high loading and chemical stability to oxidation under ambient conditions are important advantages in terms of the development of silicon‐based light‐emitting diodes from this class of materials.     

用介孔材料制备定向碳纳米管的研究进展

综述了近年来采用介孔材料制备定向碳纳米管的研究进展,包括介孔材料的合成及介孔材料在制备定向碳纳米管方面的应用。重点介绍了采用合成介孔材料的模板剂石墨化及介孔材料作为载体制备定向碳纳米管的方法,探讨了模板剂种类、催化剂的制备方法及反应温度和时间对定向碳纳米管生长的影响和定向碳纳米管生长的介孔限制机理,并提出了这一领域的研究方向。     

锐钛型介孔纳米二氧化钛粉体的制备与表征

采用沉淀法,以水溶液为反应体系,无机物（硫酸氧钛和氢氧化钠）为主要原料,加入少量模板剂,制备出锐钛型介孔纳米二氧化钛粉体。通过正交实验分析优选出最佳工艺。采用比表面仪、原子力显微镜（AFM）、高分辨场发射透射电镜等仪器对产品的结构进行了表征,得到了具有较高热稳定性,比表面积为121 m2·g-1,晶粒尺寸为12 nm,介孔平均孔径为10 nm,粉体粒径＜100 nm等特征的锐钛型介孔纳米二氧化钛粉体。