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。     

新型重整催化剂的研究——Pt／L中沸石酸碱性的作用

Ｐｔ／ＫＬ、Ｐｔ／ＢａＫＬ及Ｐｔ／ＨＬ上的铂与沸石的酸碱位发生相互作用，导致催化剂上存在不同电子状态和粒度分布的铂位，从而产生有着完全不同催化作用、不同抗硫性能的两类催化剂，即以碱性沸石为载体的“单功能”催化剂和以酸性沸石为载体的“双功能”催化剂。在Ｐｔ／ＫＬ、Ｐｔ／ＢａＫＬ催化剂上，存在着对硫敏感的具有环化脱氢功能和对硫不敏感的仅具有脱氢功能的两类铂活性位。     

Synthesis and Characterization of Nanosized ZSM-5 Zeolite with Mesoporous Carbon Nanotube as Templates

Preparation of nanocrystalline ZSM-5 has been proven possible with carbon matrix by using confined space synthesis. In combination with the hydrothermal method, by the use of a mesoporous carbon nanotube as the inert support material, ZSM-5 with SiO₂/Al₂O₃ ratios of 100 was successfully synthesized with an average crystal size of 27 nm. Their structures were preliminarily characterized by x-ray power diffraction (XRPD) and infrared spectroscopy (IR), and scanning electron microscopy (SEM), respectively. At the same time, we put forward the mechanism about the confined space synthesis in terms of the results.     

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。