Ir/H-ZSM-5 Catalysts in the Selective Reduction of NOx with Hydrocarbons

Three different Ir catalysts supported on H-ZSM-5 were prepared and tested for the selective catalytic reduction of NO under net oxidizing conditions using propene as reducing agent. The preparation of highly active Ir catalysts and the elaboration of a procedure for enhancing activity by on stream conditioning was targeted. Structural changes of the catalyst during conditioning were investigated by means of XRD, TEM and activity measurements. Under reaction conditions Ir was present as Ir⁰ and IrO₂. The presence of Ir⁰ was essential for high DeNOx activity. The ratio of Ir⁰/Ir⁴⁺ was found to depend on the size of Ir-containing crystallites. Larger crystallites contained predominantly Ir⁰. Crystallite size and oxidation state of Ir have been identified to be crucial for the NO reduction behaviour of Ir/H-ZSM-5.     

Pd/C催化水合肼还原法制备4-氨基苄醇

在优化实验条件下,即0.60 gw(Pd)=10%的Pd/C催化下,2.94 g质量分数为85%的水合肼还原3.83 g4-硝基苄醇,在80~85℃下反应3.5 h后,反应产物用乙醇-水重结晶得4-氨基苄醇2.788 g,收率为90.67%。3次扩大10倍实验的平均收率为88.56%。     

Influence of Na doping on the magnetic properties of LaFeO3 powders and dielectric properties of LaFeO3 ceramics prepared by citric sol-gel method

The emergence of ferromagnetism in perovskite oxide LaFeO₃ nanoparticles and colossal dielectric response in ceramics has inspired researchers to study the effect of various dopants on the magnetic and dielectric properties of LaFeO₃ powders and ceramics. However, the influence of alkali element Na doping has not been studied yet, and the origin of such ferromagnetic behavior is still ambiguous. The primary objective of the present work is to elucidate the effect of Na doping on the magnetic properties of La_1−xNa_xFeO₃ (x=0, 0.1 and 0.2) powders and dielectric properties of corresponding ceramics prepared by citric sol-gel method. FE-SEM results showed that the introduction of Na dopant actually resulted in the formation of nonstoichiometric La_1−xFeO₃ and x/2 Na₂O. Compared to the canted AFM behavior for the pure powder, ferromagnetic behavior with enhanced magnetization of 2.11 emu/g at 10 kOe could be obviously observed at room temperature for the powder with x=0.2. XPS measurement suggested nonstoichiometric Fe/La ratio which leads to the distortion of lattice structure and enlarged canting angle between the two AFM coupled Fe sublattice should be responsible for the enhancement of magnetization in the Na-doped samples. Meanwhile, the introduction of Na dopant lowered the growth temperature of grains of the parent LFO and resulted in larger average grain size, which in turn leaded to great enhancement of ε′ into the order of 10⁵ at 100 Hz at the cost of high tanδ for the Na-doped ceramics.     

生物还原法制备Pd/TiO2光催化剂

用芳樟叶煮液将PdCl2还原成Pd单质纳米颗粒,将其沉积于TiO2上制得Pd/TiO2催化剂,采用X射线衍射(XRD),扫描电镜(SEM)和能量色散谱仪(EDS)对催化剂进行表征,并以甲基橙为目标降解物评价Pd/TiO2催化剂的光催化降解活性.结果表明,Pd/TiO2催化剂中的Pd纳米颗粒的平均粒径小于10 nm,能够很好地分散在TiO2表面,且不改变TiO2锐钛矿的晶型结构.与未负载Pd的TiO2催化剂相比,Pd/TiO2光催化剂对甲基橙有更高的光催化降解活性,能够提高甲基橙的降解速率.在实验范围内.Pd与TiO2质量比为5%的催化剂活性最高,反应30 min甲基橙就能完全降解,而空白TiO2催化剂在反应1 h时降解率只达到95%.Pd与TiO2质量比为5%的Pd/TiO2光催化剂矿化率可达到96.2%,且重复使用仍能保持良好的催化活性.     

Influence of oxygen and promoting effect of barium on the reduction of NOx by ethanol on Pd/ZrO2 catalyst

The NO reduction by ethanol over barium promoted Pd/ZrO₂ catalyst and the effect of the oxygen on the selectivity were studied. The catalysts were prepared by incipient wetness impregnation with 14.3% of Ba over zirconia and 1% of palladium. The specific surface areas were 58 and 47 m²/g and the dispersions of Pd were 37% and 30% for the Pd/ZrO₂ and Pd–Ba/ZrO₂ catalysts, respectively. The X-ray diffraction patterns indicate the presence of monoclinic zirconia phase on the support and BaCO₃, which is decomposed at 715 and 815 °C. Temperature programmed desorption profiles of NO on Pd/ZrO₂ and Pd–Ba/ZrO₂ catalyst showed a huge amount N₂ formation for the promoted Ba catalyst. Catalytic results showed high NO conversion even at low temperature, in accordance with the TPD results and an increasing selectivity to N₂ when compared with Pd/ZrO₂. The effect of O₂ in the NO_x reduction with ethanol provoked less NO dissociation and lower selectivity to methane.     

微波辅助法制备Pd／C和Pd-Co／C催化剂及其氧还原催化活性研究

为了减少有机溶剂的使用量,使制备方法更加环境友好,文章研究了有机溶剂量对微波反应制备Pd／C系列催化剂的影响,并采用XRD、TEM和电化学测试等方法对催化剂结构和电化学性能进行了表征和评价。研究表明：当有机溶剂使用量降到5mL时,该催化剂依然能保持较高的催化活性。在此基础上,文章还对一系列不同组成的Pd-Co／C合金催化剂进行了研究．发现活性组分粒径约为3．5nm时,Pd2Co／C催化剂具有最佳的氧还原电催化活性。     

制备条件对Pd/C催化剂活性相PdH_x的影响

PdHx相是Pd/C催化剂中一种重要的活性物种。研究以浸渍-水合肼还原法制备出PdHx含量较高的Pd/C催化剂,通过XRD、XPS和TEM等表征方法研究了还原方式和条件及载体活性炭的预处理条件对催化剂中PdHx含量的影响,以无氢条件下的2,6-二甲基苯酚胺化法合成2,6-二甲基苯胺作为探针反应,验证了PdHx含量与催化活性的相关性。结果表明:以2.5%(wt)硝酸预处理的活性炭为载体,水合肼为还原剂,在40℃还原制得的催化剂具有较高的PdHx含量,以其为催化剂时原料的转化率和产品的选择性分别高达59.8%和87.3%。说明PdHx是该反应的活性相,其含量与载体预处理时的硝酸浓度密切相关。     

Residual Stress Relaxation Induced by Mass Transport Through Interface of the Pd/SrTiO3

Metal interconnections having a small cross-section and short length can be subjected to very large mass transport due to the passing of high current densities. As a result, nonlinear diffusion and electromigration effects which may result in device failure and electrical instabilities may be manifested. Various thicknesses of Pd were deposited over SrTiO₃ substrate. Residual stress of the deposited film was evaluated by measuring the variation of d-spacing versus sin²ψ through conventional X-ray diffraction method. It has been found that the lattice misfit within film and substrate might be relaxed because of mass transport. Besides, the relation between residual intrinsic stress and oxygen diffusion through deposited film has been expressed. Consequently, appearance of oxide intermediate layer may adjust interfacial characteristics and suppress electrical conductivity by increasing electron scattering through metallic films.     

Pd/C催化水合肼还原法制备5-氨基-8-羟基喹啉

在1.25gw(Pd)=10%的Pd/C催化下,5 29g质量分数为85%的水合肼还原9 70g5 硝基 8 羟基喹啉,在80～85℃下反应4h后,反应产物用苯重结晶得5 氨基 8 羟基喹啉7 31g,收率91 38%。     

碳热还原法合成硼化锆粉体影响因素探究

以氧化锆(ZrO2)、硼酸(H3 BO3)和碳(C)粉为原料,研究了不同碳粉(活性炭、石墨)与前驱体粒度、温度及保温时间对碳热还原法制备硼化锆(ZrB2)粉体的影响.通过X射线衍射(XRD)分析合成粉体物相,扫描电镜(SEM)观察合成粉体形貌,并通过化学方法分析了合成粉体中的C、O含量.结果表明:以活性炭为碳源合成的粉体形貌呈条棒状,以石墨为碳源合成的粉体形貌呈规则的块状;合成粉体的粒度随前驱体粒度减小而减小,形貌由规则的块状逐渐转变为圆滑的不规则形貌,合成ZrB2粉体最小平均粒度约为1.69μm,产物中C含量随前驱体粒度减小而减少,O含量随前驱体粒度减小而增加,氧含量最低为0.54wt％;碳热还原法合成ZrB2粉体在1500℃下是可行的,但直到1900℃碳热还原反应合成ZrB2才进行完全;碳热还原反应合成ZrB2粉体最佳的反应条件为1900℃保温30 min.     

Cu,Co, Ag-Containing Pillared Clays as Catalysts for the Selective Reduction of NOx by Hydrocarbons in an Excess of Oxygen

Thermally stable Al- and Zr-PILC loaded with copper and cobalt cations and silver nanoparticles were synthesized. The structural and surface features of these nanosystems were studied and compared with those of bulk analogs – partially stabilized ZrO₂ loaded with the same active components. Specificity of the catalytic properties of nanocomposites in SCR of NO _x by propane, propylene and decane in the excess of oxygen appears to be determined both by distribution of active components on the catalytic surface and degree of their interaction with supports. Formation of ads.-NO _x , nitroxyl-hydrocarbon C _x H _y NO₂ and isocyanate NCO intermediates was observed by ESR and IR spectroscopy in situ.     

制备条件对钯/陶瓷膜催化剂性能的影响

将钯纳米颗粒负载于陶瓷膜表面制备钯/陶瓷膜催化剂,并用于对硝基苯酚催化加氢反应中,考察了陶瓷膜孔径,硅烷偶联剂KH550溶剂及其浓度和改性时间,钯盐浸渍浓度、温度及时间以及还原温度对膜催化剂催化性能的影响.结果表明,采用孔径为200 nm 的氧化铝陶瓷膜,在6g/L的硅烷偶联剂KH550溶液中浸渍48 h,然后在40℃的浓度为0.030 mol/L乙酸钯溶液中浸渍20 h,最后采用水合肼在0℃还原30 min,得到的钯/陶瓷膜催化剂在对硝基苯酚催化加氢反应中显示了较好的催化性能,其加氢速率达15.5 mol/(h·m2).     

镁热还原法制备多孔硅碳复合负极材料

分别以介孔二氧化硅(SBA-15和 MCM-48)和硅藻土为硅源,通过镁热还原制备多孔硅,然后向多孔硅中注入有机碳前躯体,经过高温碳化处理得到多孔Si/C复合负极材料。采用X射线衍射仪、Raman光谱仪、场发射扫描电子显微镜和N2吸附脱附测试仪对合成的材料分别进行了表征,研究了多孔 Si/C 复合材料的电化学性能。结果表明：镁热还原介孔二氧化硅可以得到多孔硅材料,碳加入到多孔硅材料中可以有效提高材料的电子电导率,可明显改善材料的循环稳定性。同时多孔结构可以有效缓解硅基材料充放电过程中的体积应力,提高材料的循环稳定性。以SBA-15、MCM-48和硅藻土为硅源制备得到的3种多孔Si/C复合材料在200 mA/g电流密度下循环30次之后的可逆容量分别为712、664、463 mA·h/g。     

Preparation of Pd/Al2O3/Al catalysts for CO removal

Aluminum was carefully anodized, then palladium salts were supported on its A1₂O₃ surface layer by ion-exchange. CO 3.76 vol% contained in the air can be eliminated at around 200 °C. Both anodization conditions and the nature of the precursor solutions affect catalyst nature, particularly the pH value of the precursor solutions. The pH value of the solution suitable for supporting active components is 5–6. Palladium, which is present as Pd²⁺ and Pd⁴⁺ after calcination,distributes uniformly on the support surface which had a honeycomb structure.     

制备方法对TiO2/HZSM-5光催化氧化NOx活性的影响

分别采用同相扩散法、浸渍法和溶胶.凝胶法制备了三种TiO<,2>/HZSM-5分子筛复合TiO<,2>光催化剂,在紫外光下考察其对NO<,2>的光催化氧化活性.利用XRD、UV-Vis表征催化剂结构,结果表明,制备方法是影响复合催化剂中TiO<,2>结晶度的重要因素,而对TiO<,2>的光吸收无显著影响.对NO<,x>光催化活性评价结果显示,固相扩散法和浸渍法制备的复合光催化剂的活性明显高于P25 TiO<,2>,其中国相扩散法制备的催化剂光催化活性最高,归因于其具有较高的TiO<,2>结晶度和混晶效应;相比P25,复合催化剂对中间产物NO<,2>的生成有明显的抑制作用.     

三丁基锡氢化物在Pd/C催化下还原酰氯的反应研究

制备了活性炭负载钯催化剂,发现它对三丁基锡氢化物还原酰氯合成芳香醛的反应具有较高的催化活性和化学选择性,催化剂可重复使用,减少了贵金属Pd的流失。采用XPS分析方法对催化反应机理进行了研究和探讨,结果表明金属态Pd(0)为催化活性中心。     

ACS/Sb2O3复合材料制备方法对性能的影响

对采用原位悬浮聚合制备的苯乙烯一氯化聚乙烯一丙烯腈（ACS）共聚物／Sb2O3复合树脂、原位聚合苯乙烯一丙烯腈（SAN）共聚物／Sb2O3复合树脂与ACS树脂的共混物和ACS树脂／Sb2O3的直接共混物的力学性能和阻燃性能进行了研究比较。结果发现：原位聚合法制备的ACS／Sb2O3复合材料的性能优于其它两种方法制备的复合物;三种复合材料的冲击性能都劣于纯ACS材料;采用原位聚合方法,Sb2O3质量分数小于7％时,Sb2O3对复合材料有增强作用;当Sb2O3质量分数大于10％时,直接共混ACS／Sb2O3复合物的阻燃性能劣于其它两种方法制备的ACS／Sb203复合材料。     

钯/氧化铝催化剂对四氢糠醇合成吡啶的研究

研究了以四氢糠醇(THFA)为原料,Pd/Al2O3为催化剂经气固相接触催化合成吡啶的反应.采用XPS、BET对催化剂进行了表征,气相色谱-质谱联用仪对反应产物进行了分析,确定了主要产物吡啶.考察了四氢糠醇流量、反应温度,氢气、氨气流量,Pd负载量对反应的影响.结果表明,负载量为5%的Pd/～2O3经固定床反应器,反应温度为320℃,n(THFA):n(NH3):n(H2)=1:5:10时,可使吡啶的反应收率达到81.73%.     

制备方法对Al/Fe_2O_3纳米铝热剂性能的影响

分别采用超声共混法、机械球磨法和溶胶-凝胶法制备出Al/Fe2O3纳米铝热剂。研究了3种制备方法对纳米铝热剂晶型、平均粒径、形貌、比表面积和热反应性能的影响。结果表明,超声共混法只能使两组分简单地混合在一起;机械球磨法通过机械作用力使两组分混合均匀,但部分Al颗粒破裂,平均粒径减小;溶胶-凝胶法制备的Fe2O3凝胶均匀包裹着Al颗粒,形成核壳结构的Al/Fe2O3纳米铝热剂,有效地保护了Al颗粒,同时纳米铝热剂具有高的比表面积,固—固反应放热量为896J/g。