ZrO2-Al2O3复合载体的制备方法对Pd基催化剂加氢脱硫性能的影响

采用连续流动微反装置考察了ZrO2-Al2O3复合载体制备方法对Pd基催化荆加氢脱硫性能的影响,并采用XRD,TPR,H2-TPD.NH3-TPD和H2吸附等技术对催化剂进行了表征.结果表明,复合载体的制备方法对Pd基催化剂加氢脱硫性能有较大的影响,与浸渍法相比,溶胶一凝胶法制备的复合载体增强了活性组分与载体的相互作用,有利于Pd分散度的增大和催化剂酸量的增加,从而有利于Pd基催化剂活性的提高.     

MnOx-MoO3/TiO2-Al2O3催化剂的制备及其SCR脱硝性能

采用共浸渍负载成型法制备了MnOx-MoO3/TiO2-Al2O3(MMTA)催化剂,研究了该系列催化剂在NH3选择性催化还原反应(NH3-SCR反应)中的脱硝性能.通过固定床连续反应器考察了温度及不同载体对SCR反应的影响.采用X射线衍射(XRD)、BET、扫描电镜(SEM)等表征手段对该催化剂进行了表征,研究了催化剂的晶相、微观形貌.试验结果表明,与TiO2(T)载体相比,TiO2-Al2O3(TA)载体有较大的比表面积和孔体积.在空速为10000 h-1,150～450℃范围内,MMTA催化剂还原NOx的转化率高达75％～95％.活性组分MnOx在TiO2-Al2O3(TA)载体上分散较好,TiO2-Al2O3(TA)载体催化剂表现出良好的催化活性和高温稳定性,可有效控制氮氧化物的排放.     

AgO/Al_2O_3催化剂选择还原氮氧化物的研究

对浸渍法和水热共沉淀法制备的AgO/Al2O3催化剂进行了选择还原氮氧化物的研究。结果表明:催化剂制备方法对催化剂的催化效果起重要作用,水热共沉淀法制备的AgO/Al2O3催化剂要比浸渍法制备的更有活性;引入不同的还原剂表现出不同的还原性能,水热共沉淀法制备的AgO/Al2O3催化剂具有更强的抗水抗硫性能。AgO与高比表面积Al2O3之间的强相互作用是水热共沉淀法制备的AgO/Al2O3催化剂具有高选择还原活性的原因所在。催化剂表面吸附的氧气很大程度上促进了氮氧化物的选择性氧化过程。     

Au-Pd/ZnO-CeO_2催化剂甲醇部分氧化制氢性能的研究

采用聚合物保护乙醇还原法制备了Au-Pd/ZnO-CeO_2催化剂,考察了CeO_2对Au-Pd/ZnO催化剂甲醇部分氧化制氢反应性能的影响,并运用BET、XRD、TPR、H_2-TPD和CH_3OH-TPD等手段对催化剂进行了表征.结果表明,CeO_2对Au-Pd/ZnO催化剂具有较好的改性效果,CeO_2的引入能提高Au-Pd/ZnO催化剂的活性和氢气的选择性,归结于CeO_2的加入增加了催化剂的比表面积、分散度和对反应物甲醇的吸附,同时减少了对生成物H_2脱附,这些均有利于甲醇部分氧化制氢反应.     

镧或钕掺杂TiO2可见光催化剂及其对甲基橙的降解活性

用溶胶-凝胶法制备的La2O3/TiO2和Nd2O3/TiO2等催化剂,在可见光下降解甲基橙活性顺序为Nd2O3/TiO2>La2O3/TiO2>Fe2O3/TiO2>TiO2.焙烧温度为500℃的掺Nd为0.7%(摩尔分数)的催化剂活性最高.用XRD、DTG分析了催化剂的晶型结构,探讨了稀土对晶格畸变和催化活性的影响.     

TiO2／活性炭的制备与光催化性能

以活性炭(AC)为载体，采用Sol-Gel法制备纳米TiO2／AC复合催化剂，利用SEM，TG-DTA，XRD等对其组成、结构、尺寸等进行分析和表征；并用紫外灯为光源，通过可溶性罗丹明B的光催化降解反映对其光催化活性进行研究。结果表明，TiO2纳米粒子的尺寸范围在30nm～60nm之间，其中TiO2的晶型主要为锐钛矿；活性炭载体与TiO2结合牢固，TiO2纳米颗粒不发生二维粘结；TiO2／AC复合体的比表面积比活性炭载体的大，对罗丹明B在200min内达到完全降解，而P25需要5h，TiO2／AC复合体具有很强的光催化活性，并且制备的TiO2／AC复合体催化剂容易从溶液中分离。     

水热法合成Sb2O3／TiO2复合光催化剂

采用温和的水热法合成Sb2O3／TiO2纳米颗粒,并利用XRD、TEM对样品的晶型和形貌进行表征;以光催化降解甲基橙反应,研究了Sb2O3／TiO2的光催化性能。结果表明,用Sb2O3复合提高了TiO2的光催化活性,在140℃、水热反应12h的条件下,合成的0．5％Sb2O3／TiO2的光催化活性最佳。     

纳米TiO2负载钯催化剂的性能研究

采用浸渍法制备了纳米TiO2负载钯催化剂,以乙炔选择催化加氢制备乙烯为反应模型考察了稀土元素La、空速对纳米Pd／TiO2催化剂性能的影响,并与纳米SiO2为载体的Pd—La／SiO2催化剂的性能做了比较。实验结果表明,纳米Pd／TiO2催化剂具有良好的催化活性和性能稳定性,La的加入显著提高了乙烯的选择性、增幅达加％左右。与Pd—La／SiO2催化剂相比,Pd—La／TiO2催化剂具有更高的选择性。     

Ce、Sm改性Cu2O/MgO催化环己醇脱氢制环己酮的研究

采用浸渍还原法以水合肼为还原剂制备Cu2O/MgO催化剂,以环己醇脱氢制环己酮为探针反应,考察了Ce、Sm的添加对Cu2O/MgO催化性能的影响;采用程序升温还原(TPR)、二氧化碳程序升温脱附(CO2-TPD)和X射线衍射(XRD)等手段对催化剂进行了表征.研究结果表明,Ce-Cu2O/MgO、 Sm-Cu2O/MgO的催化性能优于Cu2O/MgO.其原因是Ce、Sm的添加使Cu2O分散度变大,导致催化剂中活性组分与载体的相互作用力增强,Cu2O更稳定;同时增加了催化剂的弱、中碱中心强度并削弱了其强碱中心强度,从而有利于反应的进行.     

In含量对In-Ag-Ce-O/γ-Al_2O_3催化剂三效催化性能的影响

采用等体积浸渍法制备了以稀散金属In、过渡金属Ag和稀土金属Ce为活性组分,以γ-Al2O3为载体的三效催化剂。通过XRD、BET、SEM、N2吸附技术对In-Ag-Ce-O/γ-Al2O3催化剂的微观结构进行了表征,并考察了In含量(质量分数)对催化剂性能的影响。结果表明,加入In之后,在XRD谱图中出现了AgInO2物相,使催化剂活性得以提高,但随着In含量的增加,催化剂的活性逐渐下降;由BET、SEM分析可知,In含量的增加,造成活性组分聚集,使其分散度降低,催化剂比表面积降低,催化活性随之下降。活性组分In含量为2%时,In-Ag-Ce-O/γ-Al2O3催化剂的三效催化活性最佳。     

钛硅铁合金生产中金属元素与渣氧化物的反应和平衡

描述了在钛硅铁合金生产中Ｓｉ－Ｔｉ－Ｆｅ合金系和ＴｉＯ２－ＣａＯ－ＳｉＯ２－Ａｌ２Ｏ３渣系间的反应以及金属元素和渣系氧化物的化学平衡。攀钢高炉渣，硅铁和石灰按一定比例混合均匀，加入直流电炉中，在熔态条件下发生反应，得到钛硅铁合金和还原低钛渣。试验表明，在反应开始后４０ｍｉｎ反应可达到平衡；加入石磁可以提高渣的碱度；合金中高硅含量有利于钛回收率的提高。     

复合催化剂TiO2/Fe2O3的制备及其光催化性能

以Fe2O3和TiCl4为原料,通过水解法制备Fe2O3/TiO2包覆型复合光催化剂,并用XRD、SEM进行表征。以甲基橙为模型污染物,比较了Fe2O3、TiO2和TiO2/Fe2O3的光催化活性,确定了Fe2O3和TiO2的最佳配比,同时探讨了反应机理。     

Rare earths (Ce,Y, Pr) modified Pd/La_2O_3-ZrO_2-Al_2O_3 catalysts used in lean-burn natural gas fueled vehicles

14%REO_x-2.5%La_2 O_3-33.5%ZrO_2-50%Al_2 O_3(RE = Ce, Y, Pr) composites were prepared by a coprecipitation method. The Pd catalysts were obtained by an aqueous solution of Pd(NO_3)_2 loaded on the rare earths modified composites with an initial wet impregnated method. The experiment results show that catalytic activity of the rare earths modified Pd/La_2 O_3-ZrO_2-Al_2 O_3 catalysts is better than bare sample for methane oxidation. The structural characterization results reveal that the rare earths modified Pd catalysts increase amounts of surface active oxygen species by X-ray photoelectron spectroscopy(XPS) analysis and improve the dispersion of active component from H2-temperature programmed reduction(H2-TPR) measurement compared with bare sample. Especially,Pd/14%Y_2 O_3-2.5%La_2 O_3-33.5%ZrO_2-50%Al_2 O_3 sample exhibits highly active stability, it is related to the Pd particles highly dispersion,which was observed by transmission electron microscope(TEM) images.     

Enhanced photocatalytic activity of Gd~(3+) doped TiO_2 and Gd_2O_3 modified TiO_2 prepared via ball milling method

Gd~(3+)/TiO_2 and Gd_2O_3/TiO_2 nanoparticles were prepared by ball milling method.The effects of Gd~(3+)ion and Gd_2O_3 on the structure and optical property of TiO_2 were studied by XRD and UV-vis DRS.Specific surface area was determined by Brunauer-Emmett-Teller(BET)method.The morphology and elemental composition were characterized by SEM-EDS.XPS was used to determine the surface compositions and chemical character of elements.The sample sizes and microstructures were observed by TEM.The photocatalytic activities of TiO_2 nanoparticles modified with rare earth metal gadolinium(Gd~(3+)ion or Gd_2O_3)were evaluated by degradation of methylene blue(MB)under UV light.Experimental results indicate that 2,5 mol%Gd~(3+)/TiO_2 shows the best photocatalytic activity compared with Gd_2O_3/TiO_2 and pure TiO_2.The existence of gadolinium can exhibit the aggregation and induce lattice distortion of TiO_2 obtained from XRD,SEM and TEM results.The band gap energy of 2.5 mol%Gd~(3+)/TiO_2 decreases to3.07 eV and it leads to visible light absorption response which can be seen from UV-vis absorption spectra.The surface area of 2.5 mol%Gd~(3+)/TiO_2 equals to 85.8 m~2/g and average crystal size is 21.1 nm.EDS and XPS analyses reveal that gadolinium can be introduced either into TiO_2 lattice or adsorbed on the surface of TiO_2.The content of surface OH groups in 2.5 mol%Gd~(3+)/TiO_2 is 50,88%(1.55 times higher than that of pure TiO_2)and the content of lattice oxygen decreases to 11.26%.The MB(25 mg/L)degradation reaction rate constants of 2,5 mol%Gd~(3+)/TiO_2,0.5 mol%Gd_2O_3/TiO_2 and pure TiO_2 were0.0713,0.0588 and 0.0263 min~(-1),respectively.The degradation rates of rhodamine B(30 mg/L)in 60 min are 97,9%,90.1%and 84.6%for 2,5 mol%Gd~(3+)/TiO_2,0.5 mol%Gd_2O_3/TiO_2 and pure TiO_2,respectively.     

Experimental and DFT study on cerium inclusions in clean steels

To provide insights into deforming Ce-O-S-Al inclusions in steels and improving the mechanical properties,the evolution process of such harmful inclusions in clean steels was investigated by thermodynamic calculation,metallographic examination and first-principles calculation in this paper.For the tested IF steel,the thermodynamic analysis results are consistent with the calculated formation enthalpy.After Ce addition,the inclusions are transformed from Al₂O₃and TiN-Al₂TiO₅-Al₂O₃to Ce2O₃,Ce₂O₂S,CeAlO₃,TiN-Al₂TiO₅-Ce₂O₃and TiN-Al₂TiO₅-Ce₂O₂S composite inclusions,which can be confirmed by metallographic examination.The elastic constants were calculated,and the bulk modulus,Young's modulus,shear modulus and Poisson's ratio were evaluated by the Voigt-Reuss-Hill(VRH)approximation.All inclusions except Ce₂O₃show apparent brittleness.TiN,Al₂O₃,Al₂TiO₅and CeAlO₃present much higher hardness than iron matrix,while the hardness of Ce2O₃or Ce₂O₂S is close to that of iron matrix.The thermal expansion coefficients of Ce₂O₃and CeAlO₃are close to that of iron matrix,whereas,Ce₂O₂S inclusion has largely different thermal expansion coefficient from iron matrix and may deteriorate the steel performance at higher temperatures.The relatively small differences between Ce inclusions and iron matrix in terms of hardness,toughness,brittleness,and thermal expansion coefficient can explain the improvement of the mechanical properties of the tested steel.     

Effects of support property on the catalytic performance of CeO2-ZrO2-CrOx for 1,2-dichloroethane oxidation

HZSM-5, Al₂O₃, TiO₂ and SiO₂ supported CeO₂-ZrO₂-CrO_x catalysts were prepared by deposition-precipitation method and tested for deep catalytic oxidation of 1,2-dichloroethane（DCE）, as one of the common chlorinated organic pollutants. All the catalysts were characterized by means of N₂ adsorption-desorption, X-ray photoelectron spectroscopy（XPS）, ammonia-temperatureprogrammed desorption（NH₃-TPD） and hydrogen temperature-programmed reduction（H2-TPR）. The characterization results revealed that there was strongly synergistic effect between the oxidizability of CZCr species and the acidity of supports, which obviously promoted the catalytic activity for DCE degradation. 20% CZCr/HZSM-5 showed the highest activity and good durability during the long-term continuous test. The catalytic activity decreased in the order: 20%CZCr/HZSM-5>CZCr>20%CZCr/TiO₂>20%CZCr/Al₂O₃>20%CZCr/SiO₂.     

High activity of CeO_2-TiO_2 composites for deep oxidation of 1,2-dichloroethane

CeO_2-TiO_2 catalysts prepared by different methods were investigated for deep oxidation of 1,2-dichloroethane(DCE),as a typical representative of the chlorinated volatile organic compounds(CVOCs).Characterization analysis reveals that CeO_2-TiO_2 catalysts prepared by sol-gel and coprecipitation methods exhibit higher specific area,CeO_2 and TiO_2 particles are highly dispersed into each other and the reducibility and mobility of active oxygen species are obviously promoted due to the strong interaction between the two catalysts CeO_2 and TiO_2,resulting in higher catalytic activity for DCE oxidation to and less chlorinated byproduct.The high calcination temperature would lead to the formation of a new monoclinic phase Ce_(0.3)Ti_(0.7)O_2 and sintering,which is the main reason for the catalytic activity for DCE oxidation markedly decreases.     

Effect of Ce doping into V_2O_5-WO_3/TiO_2 catalysts on the selective catalytic reduction of NO_x by NH_3

In this work, the effectiveness of V_2O_5-WO_3/TiO_2 catalysts modified with different CeO_2 contents by impregnation and co-precipitation methods on the selective catalytic reduction of NOxby NH3 have been studied comparatively by various experimental techniques. The results showed that the NO conversion of V_2O_5-WO_3/CeO_2-TiO_2 catalysts modified by co-precipitation method obviously increased with the Ce doping contents in the studied range below 20%(All Ce contents are in mass fractions), but the NO conversion of V_2O_5-WO_3/CeO_2/TiO_2 catalysts modified by impregnation methods was lower than V_2O_5-WO_3/CeO_2-TiO_2 catalysts especially beyond 2.5% Ce doping contents. The V_2O_5-WO_3/CeO_2-TiO_2 catalysts showed better SCR activity, wider reaction window, and higher sulfur and water resistance. The characterization results elucidated that the modified catalysts by co-precipitation method exhibited higher specific surface area, much better dispersity of Ce component, more Ce~(3+)species and more Br?nsted acid sites than that by impregnation. The vacancies caused by more Ce~(3+)species were favorable for more NO oxidation to NO_2, and the interaction between Ce species and WOxspecies generated more Br?nsted acid sites. It could be supposed that dispersed Ce Oxspecies and WOxspecies offered more second active centers respectively to adsorb oxygen and activate ammonia as co-catalysis to the primary active center of V ions, thus facilitated the better SCR activity of modified V_2O_5-WO_3/CeO_2-TiO_2 catalysts by coprecipitation methods. The co-precipitation methods with Ce component were more suitable for production of modified commercial V_2O_5-WO_3/TiO_2 catalysts.     

Influence of CeO_2 loading on structure and catalytic activity for NH_3-SCR over TiO_2-supported CeO_2

A series of supported CeO_2/TiO_2 catalysts were prepared to explore the influence of CeO_2 loading on these catalysts for the selective catalytic reduction of NO_3 by NH_3(NH_3-SCR).The catalysts were investigated in detail by means of XRD,Raman,H_2-TPR,NH_3-TPD,XPS,in situ DRIFTS,and NH3-SCR reaction.The activity of the catalyst is closely related to the content of CeO_2.When the loading of CeO_2 is near the dispersion capacity(1.16 mmol Ce~(4+)/100 m~2 TiO_2),the catalytic activity is better.This may be because that the dispersed CeO_2 is the active species and the catalyst has appropriate redox property,along with the larger amounts of surface Ce content and surface adsorbed oxygen species.Finally,a possible reaction mechanism via the Langmuir-Hinshelwood(L-H) mechanism is tentatively proposed to further understand the NH_3-SCR reaction.