等离子体引入方式对强化制备二氧化碳重整甲烷反应的Ni/γ-Al2O3催化剂的影响

采用等离子体技术强化制备了Ni/γ-Al2O3催化剂, 以CO2重整CH4为模型反应考察了等离子体引入方式对催化剂性能的影响, 并采用H2-TPR, BET, CO2-TPD, XRD, CO2-TPSR, TGA及XPS技术对催化剂进行了表征. 研究结果表明, 与常规焙烧的催化剂相比, 在氢气还原过程前引入氮气等离子体处理能有效提高催化剂的低温反应活性. N2气等离子体处理使前驱体中的硝酸盐能在温和条件下分解, 并使催化剂具有较强的还原能力和较大的比表面积. 先进行N2气等离子体处理再进行H2气还原的催化剂, 其活性组分的分散度显著提高, 对CO2的吸附量也明显增加, 并且反应后催化剂上的积炭量比常规催化剂上的显著降低, 形成比较单一的碳物种.     

Recovery and Reduction of Spent Nickel Oxide Catalyst via Plasma Sintering Technique

A thermal plasma process for the recovery and reduction of nickel oxide in the spent nickel-based catalyst (NiO/SiO₂) was developed. The spent catalyst was sintered at >1,500 °C under plasma condition and the nickel oxide therein was reduced to nickel, which was proven by XRD and EDX. By application of SEM and GC technique, the organic tar on the surface of the spent catalyst was found to decomposed and converted to syngas (CO, CO₂, and H₂), which might be the reducing agents in the process. A gasification mechanism for the generation of syngas and the reduction of nickel oxide under plasma conditions was proposed.     

Effect of decomposition of catalyst precursor on Ni/CeO2 activity for CO methanation

CO methanation on Ni/CeO₂ has recently received increasing attention. However, the low-temperature activity and carbon resistance of Ni/CeO₂ still need to be improved. In this study, plasma decomposition of nickel nitrate was performed at ca. 150°C and atmospheric pressure. This was followed by hydrogen reduction at 500 °C in the absence of plasma, and a highly dispersed Ni/CeO₂ catalyst was obtained with improved CO adsorption and enhanced metal-support interaction. The plasma-decomposed catalyst showed significantly improved low-temperature activity with high methane selectivity (up to 100%) and enhanced carbon resistance for CO methanation. For example, at 250°C, the plasma-decomposed catalyst showed a CO conversion of 96.8% with high methane selectivity (almost 100%), whereas the CO conversion was only 14.7% for a thermally decomposed catalyst.     

A short review on recent progress of Bi/semiconductor photocatalysts: The role of Bi metal

Bi/semiconductor photocatalysts have extensively been applied in the production of hydrogen, CO₂ reduction and environmental remediation in recent years. This short review summarizes the role of Bi metal as a plasma photocatalyst and cocatalyst. As a cocatalyst, Bi metal can be electron/hole trappers, charge transfer mediators, or oxygen vacancy coordinators. In addition, the preparation methods of the Bi/semiconductor photocatalysts are also reviewed. Challenges and future research directions related to Bi/semiconductor photocatalysts are discussed and summarized, including the use of advanced characterization techniques to refine the reaction mechanism, the difficulties of preparing Bi single atom catalyst, and the improvement of the reduction ability of Bi-based photocatalysts. This review helps understand the reaction mechanisms of the composite photocatalytic systems containing Bi metal and proposes new perspectives for designing the photocatalysts which can control air pollution via a reductive process.     

低温等离子体制备与改性纳米催化材料的研究进展

低温等离子体属于非热平衡等离子体,它具有较高的电子温度和较低的气体温度,是一种纳米催化剂制备与改性的新方法。 低温等离子体因其高效、环境友好、材料易实现功能化等特点在制备和改性纳米催化材料方面引起了广泛关注,在纳米催化材料的非常规制备、掺杂、缺陷和空位制造中展现了突出的优势,因而被广泛用于各类催化剂的制备与改性中。 本文主要综述了低温等离子体在氧还原(ORR)、氧析出(OER)、析氢(HER)和燃料氧化反应(FOR)催化剂制备与改性方面的研究进展,从不同角度阐述了上述各类催化剂性能改善的原因,并对低温等离子体在纳米催化剂制备与改性方面存在的成本相对较高、反应器放大、材料可控制备等挑战进行了总结,最后对等离子体制备与改性纳米催化剂的发展趋势进行了预测。     

等离子体还原催化剂在CO2甲烷化反应中的活性

采用浸渍法和原位生长水滑石法制备了Ni-Ce/γ-Al₂O₃和Ni-Ce-LDHs/γ-Al₂O₃ 2种不同类型的催化剂前驱体, 考察了2种前驱体分别经氩-氢等离子体和常规氢热方法还原所得催化剂在CO₂甲烷化反应中的活性. 结果表明, 等离子体还原催化剂的低温活性明显高于常规氢热还原催化剂, 主要表现为前者反应启动的临界温度点比后者低20~30 ℃. 采用X射线衍射(XRD)分析、 透射电子显微镜(TEM)、 CO₂程序升温脱附(CO₂-TPD)以及X射线光电子能谱(XPS)对所得催化剂的形貌和结构进行了表征. 结果表明, 等离子体还原催化剂具有较小的活性组分粒径、 较高的活性组分分散度以及较高的表面碱性, 这些特性有利于催化剂活性位对CO₂的化学吸附, 使其在甲烷化反应中表现出较好的低温活性.     

冷等离子体强化制备TiO2光催化材料及其机理

等离子体技术在材料制备和改性方面的优势得到众多研究者的认可。Ti O2具有化学稳定性高、氧化活性强、生产成本低等优势,被广泛应用于太阳能电池和光催化领域。本文综述了近年来介质阻挡放电等离子体在强化制备Ti O2光催化材料方面的研究成果,包括等离子体辅助制备Ti O2光催化薄膜和Ti O2的等离子体法掺杂两个方面,并分析了其作用机理。从目前的研究成果来看,等离子体技术制得的Ti O2光催化材料具有更好的均匀性和催化活性,这主要得益于等离子体中的高能电子,一方面,Ti O2粒子吸附电子,彼此之间产生静电场的斥力作用,可以抑制颗粒的团聚,另一方面,电子的强还原能力,能够打断Ti-O键,形成氧空位,从而提高其催化性能。     

Low-temperature plasma technology for electrocatalysis

The latest applications of plasma in energy storage and conversion are summarized here, including using it as the preparation and modification technology of the various electrocatalysts and the usage of it as the synthesis technology directly. Also, the challenges and outlook of plasma technology in energy storage and conversion were summarized, and the solutions and prospected its development in the future were present.     

等离子体在同时去除NOx和碳烟催化反应中的作用

采用程序升温反应(TPR)技术,研究了等离子体辅助同时催化去除富氧柴油机尾气中NO_x和碳烟(soot)的反应特性.研究结果表明,等离子体提高了同时去除NO_x-soot的催化反应活性,降低了碳烟的燃烧温度,使碳烟起燃温度从300 ℃降到280 ℃,燃尽温度从425 ℃降到380 ℃;同时,等离子体辅助提高了NO_x转化为N₂的效率,使催化选择性从1.12％提高到1.53％.本文还分别研究了在NO和O₂的环境中,有或没有等离子体作用下,碳烟在催化作用下的去除特性.等离子体作用使得NO在和O₂共存、只有NO和只有O₂存在的各种条件下,碳烟的催化燃烧活性都有不同程度的提高,促进了N₂的生成.此外,本文也对等离子体辅助同时催化去除NO_x-soot的机理进行了探讨.     

超细Ir催化剂对氨氧化的电催化性能

报道了一种新型的、用NH4F作络合剂的络合还原法制备的Ir催化剂及其对氨氧化的电催化性能. 结果表明, 由于溶液中的Ir3+和NH4F形成络合物, 因此用这种络合法制得Ir催化剂中Ir粒子的平均粒径为2.8 nm, 要比不加络合剂时制得的Ir催化剂中Ir粒子的平均粒径(7.5 nm)小很多. 所以, 用络合还原法制得的Ir催化剂对氨氧化的电催化活性和稳定性都比不加络合剂时制得的Ir催化剂好很多. 且该制备方法简单、实用, 适用于催化剂的实际生产.     

低温等离子体技术在催化剂领域的应用

低温等离子体技术在化学生产中的用途越来越广泛，它在催化剂领域的应用主要表现在以下几个方面：超细颗粒催化剂合成，催化剂再生，催化剂表面处理，活性组分沉淀到基体以及低温等离子体系统中添加催化剂。经过低温等离子体制备或处理过的催化剂，其催化活性有显著提高。在等离子体反应系统中加入适当的催化剂，可以降低等离子体击穿电压，减少能量消耗，提高反应活性。     

Influence of Temperature on Gas-Phase Toluene Decomposition in Plasma-Catalytic System

The decomposition of toluene on γ-alumina, MnO₂-alumina and Ag₂O-alumina catalysts in a plasma-catalytic reactor is tested. A comparison between catalytic, catalyst-after-plasma and catalyst-in-plasma systems is made in 150–400 °C temperature range. An Arrhenius plot is made in order to deduce the mechanism of plasma activation. It was found that there is no difference between the measured activation energy for catalytic and catalyst-after-plasma systems. On the other hand it was found that plasma could activate catalyst placed inside of the discharge. Plasma treatment decreases the activation energy for the silver-alumina catalyst but does not increase the number of active centers on the surface of Ag₂O-alumina. In case of MnO₂-alumina, the activation mechanism is different: plasma does not change the activation energy and but does increase its efficiency due to formation of additional active centers. The mechanism of catalyst activation in plasma, which includes the structural change of manganese ions, is suggested.     

The chemical reduction of small inorganic gases in an electrothermal plasma reactor

Chemical reduction of small inorganic gases is accomplished using an electro-thermal plasma reactor. This benchscale reactor maintains a highly reactive plasma zone in a fluidized bed of carbon particles through which an electrical current is discharged. The carbon particles function as current-controlling media, heat sinks and reaction sites. Chemicals introduced into this medium are subjected to a variety of energy sources and chemically reactive species, which result in chemical reduction. It is shown that the inorganic gases, H₂O, CO₂, NO, NO₂ and SO₂, are chemically reduced in the plasma zone of the reactor. The end products consist of hydrogen, carbon monoxide and nitrogen gases. Additionally, elemental sulfur is deposited onto the carbon particles.     

Catalytic Reaction Assisted by Plasma or Electric Field

Direct conversion of methane, other hydrocarbons, and alcohol at lower temperatures can be achieved using plasma or an electric field and catalysts. Non‐equilibrium plasma enables activation of stable molecules including methane, carbon dioxide, and water, even at low temperatures, by virtue of high electron energy. Use of a hybrid system of plasma and catalyst provided high conversion and selectivity to products by virtue of adsorption on the catalyst. Imposing a DC electric field to the catalyst bed also promotes catalytic reactions, even at low temperatures. Two mechanisms for electro‐catalytic reactions are proposed for the DC electric field imposition: reactant activation by surface protonics and production of active surface oxygen species on the catalyst. This review presents summaries of these novel processes.     

介质阻挡放电等离子制备5Ni-5La/SiO2催化剂及其甲烷干重整反应催化性能

利用介质阻挡放电等离子体法制备了5Ni-5La/SiO₂催化剂,并用于甲烷干重整反应.在常压, 700℃,空速为4.8×104 mL·g^-1·h^-1时,等离子体法所制催化剂催化甲烷干重整反应的CH₄和CO₂的转化率分别为81.2%和88.4%,且在30 h内保持稳定;而传统催化剂的CH₄和CO₂初始转化率分别为81%和88.4%, 30 h后下降到58.8%和68.6%.研究结果表明,介质阻挡放电等离子体法制备的催化剂具有更高的分散性和更强的金属与La₂O₃的相互作用.等离子体处理增加了Ni周围的电子密度,增强了CO₂在催化剂表面的吸附能力和活化能力,促进了HCOO^-中间体的生成,有利于反应正向进行.     

PREPARATION OF CUO/γ-Al2O3 CATALYSTS FOR CATALYTIC COMBUSTION VOCS VIA PLASMA

CuO/γ-Al2O3 catalysts were prepared by plasma treatment and conventional impregnation methods. The catalytic combustion of two kinds of volatile organic compounds (VOCs), toluene and benzene, were carried out over these CuO/γ-Al2O3 catalysts. The surface properties of these catalysts were characterized by X-ray Diffraction (XRD) and Scanning Electron Microscopy (SEM). The experimental results showed that in catalytic combustion the activity of the CuO/γ-Al2O3 catalyst prepared via plasma was much higher than that of the CuO/γ-Al2O3 catalyst prepared by conventional impregnation method. XRD results showed that an enhanced dispersion had been achieved with the plasma treatment. SEM results indicated that the size became much smaller and the surface became more uniform with the plasma treatment.     

负载型纳米镍铈催化剂的表征及其选择性催化加氢活性(英文)

采用氢电弧等离子体法制备了具有储氢性能的镍铈纳米颗粒,通过扫描电镜、透射电镜、X光电子能谱、X射线粉末衍射、程序升温还原等手段对比表征了氧化铝负载的纳米镍铈催化剂和工业用负载镍催化剂,并以裂解汽油一段加氢反应为模型反应研究了它们的催化性能.研究结果表明,纳米镍铈催化剂的催化活性和储氢性能与催化剂表面的镍铈合金有关,负载性纳米镍铈催化剂的优良选择性与其特殊的制备方法有关.     

Developing asymmetric iron and ruthenium-based cyclone complexes; complex factors influence the asymmetric induction in the transfer hydrogenation of ketones

The preparation of a range of asymmetric iron and ruthenium-cyclone complexes, and their application to the asymmetric reduction of a ketone, are described. The enantioselectivity of ketone reduction is influenced by a single chiral centre in the catalyst, as well as by the planar chirality in the catalyst. This represents the first example of asymmetric ketone reduction using an iron cyclone catalyst.     

常压高频放电等离子体炬改进制备CO2/CH4重整用Ni/MgO催化剂

比较了常规法、等离子体炬法和等离子体炬辅助焙烧法制得的Ni/MgO催化剂上CO2/CH4重整反应性能差异,并利用X射线衍射、透射电镜、X射线光电子能谱和CO2程序升温表面反应等技术对反应前后催化剂进行了表征,结果表明,采用等离子体炬辅助焙烧法制备的催化剂上Ni晶粒粒径小,分散度较高,低温活性和抗积炭性能较高;在常压,7...