Plasmon Coupling-Induced Hot Electrons for Photocatalytic Hydrogen Generation

We present the fabrication of core-shell-satellite Au@SiO₂-Pt nanostructures and demonstrate that LSPR excitation of the core Au nanoparticle can induce plasmon coupling effect to initiate photocatalytic hydrogen generation from decomposition of formic acid. Further studies suggest that the plasmon coupling effect induces a strong local electric field between the Au core and Pt nanoparticles on the SiO₂ shell, which enables creation of hot electrons on the non-plasmonic-active Pt nanoparticles to participate hydrogen evolution reaction on the Pt surface. In addition, small SiO₂ shell thickness is required in order to obtain a strong plamon coupling effect and achieve efficient photocatalytic activities for hydrogen generation.     

g-C3N4催化石墨化碳质材料的制备及光催化性能研究

通常采用以氢氧化物作为造孔剂,过渡金属硝酸盐或氯化物作为石墨化催化剂的传统两步法策略制备多孔石墨化碳材料。然而制备过程中多涉及有毒和腐蚀性试剂,且多步骤的过程耗时较长。本文以双氰胺为原料通过热缩聚反应得到g-C₃N₄,采用高铁酸钾为催化剂一步法实现g-C₃N₄的同步碳化-石墨化,并研究其光催化性能。与传统的两步法相比,该方法耗时少、效率高、无污染。与初始的g-C₃N₄材料相比,石墨化g-C₃N₄衍生碳质材料不仅显著改善了可见光的吸收,而且大大增强了光催化活性。研究了不同石墨化温度对g-C₃N₄衍生碳质材料在可见光下降解甲基橙溶液的影响。700 ℃下制备的衍生碳质材料的降解率为12.4 mg/g。光电化学测试结果表明,多孔g-C₃N₄衍生碳质材料的光生载流子密度、电荷分离和光电流(提高了5.4倍)均得到显著提高。因此,该简便、灵活方法为提高g-C₃N₄衍生碳质材料的吸附和光催化性能提供了一种有前景的、高效的途径。     

从废水到新能源:光催化燃料电池的优化与应用

随着经济的飞速发展,社会对能源的需求日益扩大,对工业废水的无害化处理也提出了更高的要求。光催化燃料电池 (photocatalytic fuel cell, PFC) 在燃料电池中引入半导体光催化材料作为电极,实现了有机污染物高效降解和同步对外产电的双重功能,在废水无害化与资源化利用方面具有潜在的应用价值。半导体光催化电极是PFC系统高效运行的核心组件,增强其可见光响应和光生载流子分离是提高PFC性能的关键策略。反应器结构设计和运行参数优化也有利于改善PFC性能。本文从PFC基本原理和应用入手,综述了PFC在环境污染物资源化处理中的研究进展,并详细阐述了提高PFC的污染控制性能和产电效率的优化手段,为进一步设计高效稳定的PFC系统并实现其在水污染控制和清洁能源生产中的应用提供理论指导。     

催化剂薄层内甲烷水蒸气重整反应强化管内对流换热的数值模拟

本文以竖直圆管内壁催化剂薄层内发生甲烷水蒸气重整反应强化对流换热作为研究对象,对其进行了数值模拟．结果发现,催化剂薄层内的吸热化学反应可以有效地强化对流换热,降低流体和壁面温度,从而对壁面起到保护作用;极限热流密度的大小与流体的入口温度有关,存在最佳入口温度使极限热流密度最大．     

CO_2 Reforming of CH_4 over Ni/CeO_2-ZrO_2-Al_2O_3 Prepared by Hydrothermal Synthesis Method

The Ni/CeO2-ZrO2-Al2O3 catalyst with different Al2O3 and NiO contents were prepared by hydrothermal synthesis method. The catalytic performance for CO2 reforming of CH4 reaction, the interaction among components and the relation between Ni content and catalyst surface basicity were investigated. Results show that the interaction between NiO and Al2O3 is stronger than that between NiO and CeO2-ZrO2.The addition of Al2O3 can prevent the formation of large metallic Ni ensembles, increase the dispersion of Ni, and improve catalytic activity, but excess Al2O3 causes the catalyst to deactivate easily. The interaction between NiO and CeO2 results in more facile reduction of surface CeO2. The existence of a small amount of metallic Ni can increase the number of basic sites. As metallic Ni may preferentially reside on the strong basic sites, increasing Ni content can weaken the catalyst basicity.     

稀土添加剂对烃类水蒸汽重整镍催化剂性能的影响——水蒸汽吸附的TPD研究

用程序升温脱附技术,研究了添加稀土的烃类水蒸汽重整催化剂(Ni/α-Al_2O_3)对水蒸汽的吸附性能,同未加稀土的镍催化剂作了对比。结果表明,加有稀土的镍催化剂对水蒸汽的吸附能力主要是稀土的贡献。还原态催化剂对水蒸汽的吸附量比相应的氧化态多1.4倍。发现催化剂对水蒸汽的吸附能力不仅取决于浸渍方式,而且同稀土含量有关。当稀土含量较多时,催化剂表面上呈现出三个能量不同的吸附位。稀土含量少于1.3%时。对提高催化剂吸附水蒸汽的能力已作用不大。含稀土的镍催化剂吸附水蒸汽的能力大,正是其抗结炭性能耐硫性能好的原因。     

后处理对TiO_2纳米薄膜的表面结构和光催化活性的影响

半导体TiO2光催化材料对环境中各种污染物的明显去除效果已引起人们的广泛关注犤1～6犦。在普通钠钙玻璃表面涂制高光催化活性的TiO2纳米薄膜,制成环保建筑材料,不仅可以自洁玻璃表面,而且可以用于净化空气、处理废水等。但由于在热处理过程中玻璃基体内的Na+离子扩散到薄膜表面,形成光生电子和空穴的复合中心,使TiO2纳米薄膜的光催化活性大大降低犤7～10犦。为了减少玻璃中Na+离子对TiO2薄膜光催化活性的有害影响,Paz等犤8犦研究了将钠钙玻璃浸入酸溶液中,使玻璃表面的钠离子被酸中的氢离子置换出来;在玻璃表面形成SiO2凝胶层,以便阻…     

低温水热法制备硅胶负载型二氧化钛催化剂

TiO2作为一种优良的光催化材料,能够降解有机物,起到抗菌防污的作用,其在工业上的潜在应用已吸引众多研究者的普遍关注和深入研究[1-3]。为了进一步提高它的光催化活性,研究者试图运用各种方法和技术对纯TiO2进行改进。负载[3]是其中常用方法之一。对于无负载的二氧化钛,由于本     

Preparation and catalytic performance of superfine Ni/BaTiO3 catalyst

Superfine Ni/BaTiO₃ catalysts were prepared by impregnation method and used successfully for CO₂ reforming CH₄ to syngas. The effects of preparation method and the temperatures of calcination, reduction and reaction on the catalytic activity of the Ni/BaTiO₃ system were investigated. This revised version was published online in June 2006 with corrections to the Cover Date.     

Preparation and characterization of nitrogen-doped TiO2 photocatalyst in different acid environments

Nitrogen-doped TiO₂ powders were successfully prepared by a wet method, i.e., a micro-emulsion-hydrothermal method, in different acid environments. Several characterization techniques, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and UV-visible diffuse reflectance spectra, were combined to determine the crystal phase, concentration and chemical states of the nitrogen doped in TiO₂. The high photocatalytic activity of the nitrogen-doped TiO₂ was evaluated through the decomposition of rhodanmine B under visible light irradiation. It was suggested that the doped nitrogen formed oxynitride (NO) and produced impurity states at higher above the valence band of TiO₂. Therefore, the nitrogen doping could enhance the response of photocatalyst to the visible light and improve the photocatalytic activity because of the narrowing of band gap of TiO₂.