Simultaneously catalytic removal of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> and particulate matter on diesel particulate filter

Diesel engines combine a high fuel economy with high durability and low maintenance costs and are, there-fore, used on a large scale for transportation purposes.However, the environmental pollution by diesel-engine exhausts has become more and more serious in the lastdecade, and currently the regulation of diesel emissions becomes tightened especially with respect to nitrogen ox-ides (NOx) and particulate matters (PM). Since the reduc-tion of both NOx and PM to the admitted level cannot be …     

H2为还原剂的钙钛矿类催化剂存储还原NOx试验

以LaCoO3/K2CO3/CeZrO2为催化剂，分别采用程序升温脱附（TPD）、程序升温表面反应测试（TPSR）和以H2为还原剂的NOx存储-还原循环试验，研究了催化剂存储NOx的热稳定性以及NOx存储还原的性能，并分别对反应温度、还原时间和还原剂浓度这些影响因素进行了讨论.结果表明：LaCoO3/K2CO3/CeZrO2具有良好的储存和脱附再生性能，H2有较强的还原能力，在340～400 ℃下NOx转化率均为70%~80%，这些非常有利于降低发动机在实际工况下排放的NOx.
     

Pt/Ba/Ce/γ-Al_2O_3催化剂H_2-NSR性能影响因素的试验分析

将改进的溶胶-凝胶法与等体积浸渍法相结合制备了Pt/Ba/Ce/γ-Al2O3钙钛矿催化剂,研究了其表面性能;采用NOx存储还原循环试验的方法,以氢气为还原剂,研究了还原剂体积分数、还原时间和空速等反应条件,以及以CO2与HC为代表的发动机排气成分对催化剂存储还原特性的影响.结果表明:所制备的Pt/Ba/Ce/γ-Al2O3催化剂具有良好的催化活性及较大的比表面积;在所研究的范围内,不同还原剂体积分数下存在NOx转化率最高的最佳还原时间,而且随着还原剂体积分数增加,最佳还原时间逐渐缩短;还原剂体积分数的增加将会加速NOx的脱附,若还原剂体积分数过高,则会造成部分NOx溢出过快,还原时间不足而引起转化率降低;在7.0×104 h-1的大空速条件下,NOx转化率仍可以保持在86.9%,Pt/Ba/Ce/γ-Al2O3催化剂的空速特性良好;CO2在一定程度上抑制了NOx的存储,影响催化剂的活性,但催化剂容易再生;采用C3H6模拟排气中的HC,其体积分数较低时对H2还原NOx具有抑制作用,当C3H6的体积分数较高时可以促进NOx的还原转化.     

Heterobimetallic clusters of Na<Subscript>8</Subscript>Ln(O<Superscript>t</Superscript>Bu)<Subscript>10</Subscript>(OH) as homogeneous catalysts for amidation of aldehydes with amines

Heterobimetallic clusters of Na8Ln(O^tBu)₁₀(OH) (Ln = ytterbium, europium, samarium and neodymium) are found to be useful catalysts for amidation of aldehydes with amines under mild conditions. The catalytic activity depends on the central metal ion in the cluster, and the order activity is ytterbium < europium < samarium ≈ neodymium. The catalysts show a wide range of scope in their activity towards amines including aliphatic amines and secondary cyclic amines such as pyrrolidine and piperidine.     

高校实验室催化剂还原方法的分析与探索

催化剂的还原是催化剂具有催化活性的关键步骤。文章分析比较了在催化剂制备中不同还原剂对催化剂纳米粒度和稳定性的影响,并提出以金属整体型为还原剂进行催化剂还原的新概念。这些催化剂还原方法的分析,为实验室范围内催化剂提供了有力的指导。     

富氧条件下烃类选择性催化还原NOx研究进展--金属氧化物催化剂体系及NO还原反应机理

综述了负载或非负载的金属氧化物催化剂体系上,富氧条件下NO的非选择性催化还原反应性能及反应机理.着重讨论了还原剂种类、催化剂结构与化学性质对催化反应的影响及催化剂的耐水性和耐SO2性能.探讨并总结了金属氧化物催化剂体系上NO的还原机理.     

超细煤粉再燃技术降低NOx排放试验

通过试验研究确定了超细煤粉再燃技术中影响NOx排放的主要因素,研究结果表明,对于不同煤种的主燃料,超细煤粉再燃均能起到显著降低NOx排放的作用,脱氮率在50％～70％之间;高挥发分的褐煤、烟煤是较好的再燃燃料;煤粉越细,对NOx的还原性越强,同常规粒度煤粉再燃相比,使用超细煤粉,NOx脱除率增加了10％以上;随着再燃燃料比例的增加,各工况均呈现NOx排放量降低、脱氮率增加的趋势。     

前手性酮的不对称还原(Ⅰ)

综述了前手性酮的不对称还原方法及其近年来的新进展．包括手性恶唑硼烷类催化剂的应用，使用手性改型氢化铝锂的还原,手性修饰的硼氢化钠或硼氢化钾的应用，具有膦酰胺结构的手性催化剂的应用，手性金属络合物催化氢化不对称还原，不对称相转移催化还原，酶催化不对称还原．     

中国温室气体减排与选择性催化还原脱硝材料

综述了中国温室气体排放和Nox污染的现状及相互影响.论述了电厂锅炉和机动车发动机的稀燃化对CO2减排的意义和对Nox污染控制的影响,阐述了选择性催化还原脱硝技术对解决中国经济发展带来的能源危机和温室气体减排的重要性.基于温室气体减排和Nox排放的相互制约关系,指出了采用燃料的稀燃方式辅以SCR脱硝后处理技术是中国同时实现温室气体减排和Nox控制的显示可行途径.重点论述了中国燃煤电厂烟道气脱硝和柴油车尾气脱硝对选择性催化还原(SCR)脱销材料的要求,对国内外脱硝材料的研究领域、研发现状和发展趋势进行了探讨,并结合中国国情指出,具有自主知识产权的V-W-Ti基SCR脱硝材料、低温SCR脱硝材料和沸石基SCR脱硝材料是适应我国电厂烟道气脱硝和机动车尾气脱硝的SCR脱硝材料发展方向.     

基于3d过渡金属的氧电极材料研究进展

氧还原催化剂及缓慢的阴极氧还原动力学是制约低温燃料电池商业化的关键瓶颈因素之一.非贵金属氧还原催化剂是近年来低温燃料电池最受关注的研究热点之一.在简要介绍燃料电池及氧还原反应机理的基础上,详细地综述了近年来低温燃料电池用3d过渡金属基氧还原催化剂的主要研究进展,包括过渡金属大环化合物、过渡金属-氮/碳类化合物、过渡金属硫族化合物和过渡金属氧化物,总结了提高催化活性和稳定性、降低催化剂制备成本以及催化剂制备工艺等方面所取得的研究结果,并指出了各类催化剂目前尚待解决的问题和发展方向.     

Removal of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> by radical injection

Removal of NOx(DeNOx, NOx is the total of NO and NO2) from flue gas by radical injection has been investigated .the discharge characteristics were examined and the steady streamer corona was acquired hy adjusting the nozzle gases properly. It was Found that an increase in the voltage resulted in a decrease in the NO concentration and the concentration of the NO2 increased at tow voltages but decreased as the voltage rose to a certain level. The DeNOx efficiency increased as the applied voltage rose and reached a maximum of 70% when the voltage approached the breakdown voltage. The hypothetical mechanism of NOx removal suggested that the radicals formed in the discharge process converted the NO and NO2 into acidic species. The Monte Carlo method was used to calculate the rate coefficients and the productivity of the radicals, and then the concentrations of both NO and NO2 and the DeNOx effielencies were calculated with chemical kinetics. The calculated DeNOx efficiencies were coalparable with the experimental DeNOx efficiencies at low voltages, but were lower at high voltages.     

氮掺杂还原氧化石墨包覆金属钴复合材料的制备及其氧还原性能的研究

采用搅拌反应法制备了ZnCo（ZIF）与氧化石墨（graphite oxide,GO）的复合材料,热处理得到Co@N-doped rGO催化剂。通过X射线衍射（X-ray diffraction,XRD）和扫描电子显微镜（scanning electron microscopy,SEM）对催化剂进行结构表征,通过X射线光电子能谱（X-ray photoelectron spectroscopy,XPS）对催化剂进行表面元素分析,分别考察了金属（Zn和Co）加入量和热处理温度对催化剂氧气还原反应（oxygen reduction reaction,ORR）催化性能的影响,结果表明：所制备的催化剂整体呈层状分布,表面附着金属小颗粒团簇;随着金属加入量的增加,催化剂的ORR催化性能先增强后减弱;随着热处理温度的升高,催化剂的ORR催化性能先增强后减弱。所制备的S-2-850催化剂具有最好的ORR催化性能,在0.1 mol/L KOH电解液中,其起始电位和半波电位分别为0.871 V和0.804 V,在相同测试条件下活性稳定性优于20% Pt/C。     

铁基氧电极催化剂研究进展

燃料电池是一种通过化学反应将燃料所具有的化学能直接转化为电能的装置,因具有系统结构简单、启动快速、寿命长、功率密度和能量密度高等优点而备受关注。但是,燃料电池的氧还原反应动力学过程缓慢,需要高效的催化剂以提高整个体系的运行效率。目前,性能最好、使用最广泛的燃料电池催化剂是铂基催化剂。但铂价格极其昂贵,无法支持大规模商业化应用,此外,铂催化剂易中毒和稳定性差等问题也无法完全解决。近年来的研究表明,铁基催化剂具有良好的氧还原反应催化性能,最有希望替代铂基催化剂。基于此,对近年来各类非贵金属铁基催化剂进行了综述,并在此基础上阐述了各类催化剂目前尚待解决的问题和发展方向。     

天然气再燃烧还原NO_X的数值模拟

燃烧过程排放的氮氧化物（ＮＯＸ） 气体是危害很大、很难处理的大气污染物．降低燃烧过程中的ＮＯＸ排放有两类方法：一是降低ＮＯＸ的原始形成，第二类是还原已形成的ＮＯＸ；在还原已形成的ＮＯＸ 方法中，再燃烧（即部分燃烧后期喷入燃烧） 是当今世界前景看好的低ＮＯＸ 控制技术，它是利用燃料分级形成还原性气氛迫使ＮＯＸ分解来降低ＮＯＸ 形成的燃烧方法．其中，天然气做为再燃烧料已成功用于商业，并在其它措施的基础上再降低ＮＯＸ５０％ ～７０％ ．叙述了以天然气做为再燃烧料的再燃烧原理和途径，重点论述了采用无限快反应速率模型，并假定模拟烟气为层流或湍流粘性系数为常数的湍流情况下，运用有限差分及多重网格方法，计算出了这一还原反应过程的浓度场，得到了较为合理的结果．     

Selective formation of tetrahedral Pt nanocrystals from K2PtCl6／PVP

Tetrahedral platinum (Pt) nanocrystals (3-8 nm) are synthesized in high selectivity (ca. 80%) from hydrogen reduction of aqueous K2PtCI6 by using polyvinylpyr-rolidone (PVP: Mw≈360000) as a protector. Morphology (TEM) measurements of the metal colloids and UV-Vis absorption of the colloidal solution are employed to monitor the tetrahedron formation during the syntheses with varying K2PtCl6/PVP ratios. The results clearly show a two-stage process for the selective formation of tetrahedral nanocrystals. Rapid nucleation and crystal formation at the early stage result in round-like crystallites and the external facet evolution in thereafter slow crystal growth leads selectively to the formation of the tetrahedrons.     

Electro-deoxidation of V<Subscript>2</Subscript>O<Subscript>3</Subscript> in molten CaCl<Subscript>2</Subscript>-NaCl-CaO

The electro-deoxidation of V₂O₃ precursors was studied. Experiments were carried out with a two-terminal electrochemical cell, which was comprised of a molten electrolyte of CaCl₂ and NaCl with additions of CaO, a cathode of compact V₂O₃, and a graphite anode under the potential of 3.0 V at 1173 K. The phase constitution and composition as well as the morphology of the samples were studied by X-ray diffraction (XRD) and scanning electron microscopy (SEM). 3 g of V₂O₃ could be converted to vanadium metal powder within the processing time of 8 h. The kinetic pathway was investigated by analyzing the product phase in samples prepared at different reduction stages. CaO added in the reduction path of V₂O₃ formed the intermediate product CaV₂O₄.     

碳基材料在电催化还原CO2中的应用

电催化还原CO₂能够将CO₂转换成高附加值的化学品或燃料,该工艺是一种缓解能源危机和全球变暖的理想途径。但由于缺乏性能优异、价格低廉、环境友好的催化剂,该途径的实用化仍具挑战性。碳基催化剂因具有资源丰富、导电性好、比表面积大、环境友好等优点而被广泛应用于多种催化反应中。目前报道的系列碳基催化剂在CO₂还原反应中也展现出极好的催化性能和应用潜力。综述了N原子掺杂、构造缺陷、单原子负载和金属纳米颗粒负载等手段对碳基材料电催化还原CO₂性能的影响及其催化机制,并总结了电催化还原CO₂所面临的挑战。同时对未来碳基电催化剂的合成及发展进行了展望。     

Synthesis and characterization of Pt-MoO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>-TiO<Subscript>2</Subscript> electrodes for direct ethanol fuel cells

To enhance the CO-tolerance performance of anode catalysts for direct ethanol fuel cells, carbon nanotubes were modified by titanium dioxide (donated as CNTs@TiO₂) and subsequently served as the support for the preparation of Pt/CNTs@TiO₂ and Pt-Mo/CNTs@TiO₂ electrocatalysts via a UV-photoreduction method. The physicochemical characterizations of the catalysts were carried out by using X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and infrared spectroscopy of adsorbed probe ammonia molecules. The electrocatalytic properties of the catalysts for methanol oxidation were investigated by the cyclic voltammetry technique. The results show that Pt-Mo/CNTs@TiO₂ electrode exhibits the highest performance in all the electrodes. It is explained that, the structure, the oxidation states, and the acid-base properties of the catalysts are influenced due to the strong interaction between Ti and Mo species by adding TiO₂ and MoO _x to the Pt-based catalysts.     

介质阻挡放电协同铜氧化物催化剂脱除NOx反应研究

研究了以煤基活性炭为载体的铜氧化物催化剂在阻挡介质放电反应器中对NOx脱除效率的影响规律,以及催化剂在反应前后的变化和主要产物。研究结果表明,以煤基活性炭为载体的铜氧化物催化剂协同阻挡介质放电反应器,可使NO有效氧化为NO2,对NOx也有明显的脱除效果,使NO2进一步氧化为NO3-,阻止了等离子体状态下活性氧自由基自身结合生成氧气的循环反应;该催化剂对氮氧化物具有吸附和储存功能,提高了反应物浓度和反应速率。随着介质阻挡放电反应器输入能量的增加,氮氧化物脱除效率增大,该能量可有效产生等离子体,提高活性粒子和氧自由基浓度,同时提高催化剂的吸附和催化活性。     

CO2催化重整生物质焦油金属催化剂的研究进展

生物质焦油是生物质气化过程中产生的一种有害副产物,它的存在严重制约了生物质气化技术的发展。利用先进的金属催化剂,将生物质焦油与CO₂进行催化重整,获取小分子燃料气体,不仅可将生物质焦油进行转化利用,而且还实现了温室气体的减排,具有重大的现实意义。介绍了CO₂催化重整生物质焦油所用的金属催化剂,主要包括Ni基催化剂、碱金属催化剂以及非Ni的其他过渡金属催化剂。总结了各类催化剂的优缺点,并对未来生物质焦油催化重整技术作了展望。