煅烧温度对γ-Fe_2O_3催化剂结构及其脱硝活性的影响

采用沉淀-微波热解法,以Fe SO4·7H2O为铁源制备环境友好的γ-Fe2O3催化剂,结合XRD(X射线衍射)、N2等温吸附-脱附、SEM(扫描电子显微镜)、EDS(能谱仪)等手段对催化剂样品的晶相、孔结构、表面形貌、表面元素组成等进行表征,并考察其NH3-SCR(选择性催化还原)脱硝性能,研究煅烧温度对γ-Fe2O3催化剂物性及NH3-SCR脱硝性能的影响规律.结果表明:300、350和450℃下煅烧制备的催化剂中生成的杂质α-Fe2O3对SCR反应不利,而400℃煅烧制备的γ-Fe2O3催化剂脱硝性能最优,NOx转化率最高可达95%以上,XRD结果表明其纯度高,并且在60~100 nm孔径区间具有发达的孔隙结构,有利于SCR反应进行;随着煅烧温度升高,γ-Fe2O3催化剂表面晶格氧逐渐增加,颗粒形貌经历了片状颗粒(300、350℃)→球状颗粒(400℃)→针状颗粒(450℃)的变化过程,均匀的球状颗粒形貌及其表面丰富的晶格氧是400℃煅烧制得催化剂具备最优脱硝性能的重要因素.     

钙钛矿型四效催化剂净化柴油烟气的热力学分析

根据热力学原理,计算吉布斯自由能的变化量,讨论柴油烟气净化反应的可行性。钙钛矿型四效催化技术是提高CxHy、PM、CO、NOx转化率和降低反应温度的有效方法,也是改变吉布斯自由能变化量ΔG的间接条件。     

Removal of formaldehyde over MnxCe1-xO2 catalysts: Thermal catalytic oxidation versus ozone catalytic oxidation

MnxCe1- xO2（x： 0.3–0.9） prepared by Pechini method was used as a catalyst for the thermal catalytic oxidation of formaldehyde（HCHO）. At x = 0.3 and 0.5, most of the manganese was incorporated in the fluorite structure of Ce O2 to form a solid solution. The catalytic activity was best at x = 0.5, at which the temperature of 100% removal rate is the lowest（270°C）. The temperature for 100% removal of HCHO oxidation is reduced by approximately 40°C by loading 5 wt.% Cu Oxinto Mn0.5Ce0.5O2. With ozone catalytic oxidation, HCHO（61 ppm） in gas stream was completely oxidized by adding 506 ppm O3 over Mn0.5Ce0.5O2 catalyst with a GHSV（gas hourly space velocity） of 10,000 hr-1at 25°C. The effect of the molar ratio of O3 to HCHO was also investigated. As O3/HCHO ratio was increased from 3 to 8, the removal efficiency of HCHO was increased from 83.3% to 100%. With O3/HCHO ratio of 8, the mineralization efficiency of HCHO to CO2 was 86.1%. At 25°C, the p-type oxide semiconductor（Mn0.5Ce0.5O2） exhibited an excellent ozone decomposition efficiency of 99.2%,which significantly exceeded that of n-type oxide semiconductors such as Ti O2, which had a low ozone decomposition efficiency（9.81%）. At a GHSV of 10,000 hr-1, [O3]/[HCHO] = 3 and temperature of 25°C, a high HCHO removal efficiency（≥ 81.2%） was maintained throughout the durability test of 80 hr, indicating the long-term stability of the catalyst for HCHO removal.     

OMS-2负载Ag催化剂的制备及催化氧化性能研究

以KMnO4和MnSO4为基底采用回流法合成了氧化锰八面体分子筛(OMS-2)。以OMS-2为载体采用前掺杂法和浸渍法制备了不同Ag含量的负载型OMS-2催化剂,对所制催化剂进行了结构和织构表征。并研究了不同制备方法和Ag负载量对Ag/OMS-2催化氧化CO性能的影响。结果表明,OMS-2为典型的cryptomelane一维隧道结构,适量掺杂Ag使OMS-2载体分子筛的有序性得到改善。负载型Ag/OMS-2的催化活性均明显优于OMS-2载体,且前掺杂法催化活性优于浸渍法。这与Ag/OMS-2-PI催化剂中Ag颗粒大小及OMS-2载体与Ag之间存在强相互作用有关。Ag负载量明显影响Ag/OMS-2-PI催化剂的催化活性,3Ag/OMS-2-PI催化剂(Ag=3.0 wt%)催化活性最高,这是由于适当Ag负载量,Ag颗粒较小,与载体OMS-2的相互作用较强,能较好地活化OMS-2晶格氧,同时Ag的引入使OMS-2对CO的吸附性能及晶格氧的扩散能力得到显著增强,提高了催化剂对CO的氧化催化能力。     

燃煤电站 SCR 催化剂管理及其优化

选择性催化还原(SCR)方法是目前国际上电站烟气脱除氮氧化物(NOx)的主要技术手段之一,其脱硝率的高低对于催化剂有着较高的要求。研究采用文献分析的方法,就燃煤电站SCR催化剂的管理及优化进行研究,旨在探索实现SCR效益最大化的途径。研究表明,只有根据当地的实际情况,计算出成本与脱硝率之间的合理比例,才能有效地实现对SCR催化剂管理的优化。     

铈插层黏土负载铁催化剂在H2S选择性催化氧化过程中催化性能的研究

合成了铈插层的Laponite黏土材料(Ce-Lap),并以此材料为载体,分别负载质量分数为3%、5%、8%、10%的Fe制备Fe/Ce-Lap催化剂,通过XRD、氮气吸脱附曲线、XRF、TG、FT-IR、O2-TPD、H2-TPR、XPS等手段,对催化剂的物理化学性质进行了表征测试,并考察了催化剂在H2S选择性催化氧化反应过程中的活性.结果表明,5%的Fe/Ce-Lap在180℃时表现出最好的催化活性,能达到96%的硫产率,这归因于Fe与Ce之间的相互作用,改善了Fe3+的氧化还原能力.此外,较高的氧吸附能力及铁物种的高分散度促进了氧化反应的进行.     

Catalytic combustion of soot over ceria-zinc mixed oxides catalysts supported onto cordierite

Modified substrates as outer heterogeneous catalysts was employed to reduce the soot generated from incomplete combustion of diesel or diesel/biodiesel blends, a process that harms the environment and public health. The unique storage properties of ceria(CeO2) makes it one of the most efficient catalysts available to date. Here, we proposed that ceria-based catalysts can lower the temperature at which soot combustion occurs; more specifically, from 610℃ to values included in the diesel exhausts operation range(300–450℃). The sol-gel method was used to synthesize mixed oxide-based catalysts(CeO2:ZnO); the resulting catalysts were deposited onto cordierite substrates. In addition, the morphological and structural properties of the material were evaluated by XRD, BET, TPR-H2, and SEM. Thermogravimetric(TG/DTA) analysis revealed that the presence of the catalyst decreased the soot combustion temperature by 200℃ on average, indicating that the oxygen species arise at low temperatures in this situation, promoting highly reactive oxidation reactions. Comparative analysis of soot emission by diffuse reflectance spectroscopy(DRS) showed that catalyst-impregnated cordierite samples efficiently oxidized soot in a diesel/biodiesel stationary motor: soot emission decreased by more than 70%.     

钛板SCR脱硝催化剂的制备及性能研究

选用钛板作为催化剂的骨架,预先在钛板表面制备二氧化钛涂层,再浸渍活性组分以制备催化剂。用SEM结合能谱分析的方式表征催化剂表面性能,通过固定床实验来测试不同NO负荷、不同温度、不同O2含量、二氧化硫、水蒸气等烟气条件对脱硝效率的影响,并对该催化剂的抗冷热性能和稳定性进行了测试。     

Heterogeneous Fenton-like degradation of 4-chlorophenol using iron/ordered mesoporous carbon catalyst

Ordered mesoporous carbon supported iron catalysts(Fe/OMC) were prepared by the incipient wetness impregnation method and investigated in Fenton-like degradation of 4-chlorophenol(4CP) in this work. XRD and TEM characterization showed that the iron oxides were well dispersed on the OMC support and grew bigger with the increasing calcination temperature. The catalyst prepared with a lower calcination temperature showed higher decomposition efficiency towards 4CP and H2O2, but more metals were leached. The effect of different operational parameters such as initial pH, H2O2 dosage, and reaction temperature on the catalytic activity was evaluated. The results showed that 96.1% of 4CP and 47.4% of TOC was removed after 270 min at 30°C, initial pH of 3 and 6.6 mmol/L H2O2. 88% of 4CP removal efficiency was retained after three successive runs, indicating Fe/OMC a stable catalyst for Fenton reaction. 4CP was degraded predominately by the attack of hydroxyl radical formed on the catalyst surface and in the bulk solution due to iron leaching. Based on the degradation intermediates detected by high performance liquid chromatography, possible oxidation pathways were proposed during the 4CP degradation.     

Photocatalytic removal of NO and NO2 using titania nanotubes synthesized by hydrothermal method

In this study, the photocatalysts of titania nanotubes(TNTs) were synthesized at different calcination temperatures using commercial Degussa TiO2(P25) as a precursor. The materials were then characterized by BET, SEM, TEM, and XRD analyses. The photocatalytic reactions with NO and NO2 under UV-A irradiation were both performed. The results showed that the photocatalytic reaction rate of NO was much faster than that of NO2, and the conversion of NO2 to nitrate was the rate-limiting step for photocatalytic removal of NOx if the nitrate produced cannot be removed continuously from the photocatalyst surface. For TNTs calcined at different temperatures, a significant enhancement was observed on the total NOx removal efficiency by TNT calcined at 500°C for both NO and NO2 photocatalytic reaction, which could be attributed to its high anatase crystallinity as well as high surface area. These two factors affect primarily on the NO2conversion step in which the high anatase crystallinity could be responsible for the high efficiency at the beginning, while the high surface area could be accounted for retaining this high efficiency from nitric acid poisoning during the test period.