V-W/TiO_2/γ-Al_2O_3催化剂催化还原NO的研究

掺杂15%TiO2对γ-Al2O3改性制备了TiO2/γ-Al2O3复合氧化物载体,以此复合氧化物及TiO2、γ-Al2O3为载体用浸渍法负载钒钨制备了一系列催化剂,采用比表面积和孔结构分析、X射线衍射(XRD)、高分辨电镜(HRTEM)、原位红外(in situ FT-IR)等技术对载体和催化剂进行宏观-微观表征,同时在模拟氨气选择性催化还原NO(NH3-SCR)的反应条件下对催化剂的脱硝反应活性进行考察,比较研究TiO2掺杂对V2O5-WO3/TiO2和V2O5-WO3/γ-Al2O3催化剂的改性作用。结果发现,少量TiO2掺杂制得的TiO2/γ-Al2O3复合载体中,TiO2和γ-Al2O3之间的协同作用使得V2O5-WO3/TiO2/γ-Al2O3催化剂的选择性催化还原脱硝效率及活性窗口明显优于单一载体制备的催化剂,并表现出了良好的热稳定性;各种表征结果表明,TiO2/γ-Al2O3复合载体中TiO2高度分散在γ-Al2O3上,复合载体具有较大的比表面积,载体表面存在大量的Br?nsted酸位和较多的活性中间产物,这些可能是TiO2/γ-Al2O3复合载体催化剂具有较好SCR活性的原因。     

纳米TiO_2-Al_2O_3负载CuMnO_x对甲苯的催化燃烧

研究采用改进的溶胶-凝胶法制备了TiO2-Al2O3复合载体,并用浸渍法制备CuMnOX/TiO2-Al2O3催化剂,通过对甲苯废气催化燃烧的实验,分别考察了Cu-Mn负载量、Cu/Mn摩尔比、焙烧温度及载体对催化剂制备过程及催化剂活性的影响。实验结果表明:活性组分负载量25%,铜锰活性组分的配比Cu:Mn=1:2,焙烧温度500℃是浸渍法制备CuMnOX/TiO2-Al2O3催化剂较佳的工艺条件;XRD衍射图谱表明,500℃下铜锰尖晶石的存在是催化剂催化活性优良的主要原因;由复合载体制备的CuMnOX/TiO2-Al2O3催化剂比单一载体制备的CuMnOX/Al2O3催化剂具有更高的甲苯转化率,其T99比单一载体要低20℃以上。     

Photocatalytic performance of TiO2 catalysts modified by H3PW12O40, ZrO2 and CeO2

The binary composite photo-catalysts CeO2/TiO2, ZrO2/TiO2 and the ternary composite photo-catalysts H3PW12O40-CeO2/TiO2,H2PW12O40-ZrO2/TiO2 were prepared by sol-gel method. The catalysts were characterized by thermogravimetric-differential thermal analysis (TG-DTA), scanning electron microscopy (SEM) and X-ray diffraction (XRD). The photocatalyfic elimination of methanol was used as model reaction to evaluate the photocatalytic activity of the composite catalysts under ultraviolet light irradiation. The effects of doped content, activation temperature, time, initial concentration of methanol and gas flow rate on the catalytic activity were investigated. The results showed that after doping a certain amount of CeO2 and ZrO2, crystaniTation process of TiO2 was restrained, particles of catalysts are smaller and more uniform. Doping ZrO2 not only significantly improved the catalytic activity, but also increased thermal stability. Doping H3PW12O40 also enhanced the catalytic activity. The catalytic activities of binary and ternary composite photocatalysts were significantly higher than tin-doped TiO2. The dynamics law of photocatalytic reaction over the binary CeO2/TiO2 and ZrO2/TiO2 catalysts has been studied. The activation energy 15.627 and 15.631 kJ/mol and pre-exponential factors 0.5176 and 0.9899 s-1 over each corresponding catalyst were obtained. This reaction accords to the first order dynamics law.     

Treatment of phenol wastewater by microwave-induced ClO2-CuOx/Al2O3 catalytic oxidation process

The catalyst of CuOx/Al2O3 was prepared by the dipping-sedimentation method using γ-Al2O3 as a carrier. CuO and Cu2O were loaded on the surface of γ-Al2O3, characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). In the presence of CuOx/Al2O3, the microwave-induced chlorine dioxide (ClO2) catalytic oxidation process was conducted for the treatment of synthetic wastewater containing 100 mg/L phenol. The relationships between removal percentage and initial ClO2 concentration, catalyst dosage, microwave power, contact time, initial phenol concentration and pH were investigated and the results showed that microwave-induced ClO2-CuOx/Al2O3 process could effectively degrade contaminants in a short reaction time with a low oxidant dosage, extensive pH range. Under a given condition (ClO2 concentration 80 mg/L, microwave power 50 W, contact time 5 min, catalyst dosage 50 g/L, pH 9), phenol removal percentage approached 92.24%, corresponding to 79.13% of CODCr removal. The removal of phenol by microwave-induced ClO2-CuOx/Al2O3 catalytic oxidation process was a complicated non-homogeneous solid/water reaction, which fitted pseudo-first-order by kinetics. Compared with traditional ClO2 oxidation, ClO2 catalytic oxidation and microwave-induced ClO2 oxidation, microwave-induced ClO2 catalytic oxidation system could significantly enhance the degradation efficiency. It provides an effective technology for the removal of phenol wastewater.     

Fe-MnOx-CeO2/ZrO2低温催化还原NO性能研究

以纳米ZrO2为载体,用浸渍法制备出Fe-MnOx-CeO2/ZrO2催化剂,考察了活性组分配比和助剂负载量对催化剂低温NH3选择性催化还原NO活性的影响,并对催化剂进行了XRD、SEM、EDS和BET表征;探讨了温度、H2O和SO2对Fe-MnOx-CeO2/ZrO2催化剂低温下NH3选择性催化还原NO的影响,结果表明,无SO2和H2O条件下,8%Fe-10%MnOx-CeO2/ZrO2催化剂具有良好的催化活性和稳定性.120℃时,催化剂的脱硝效率为85.23%,当温度升至180℃时,脱硝效率可达到92.0%.SO2和H2O共存条件下,催化剂易失活,采用傅立叶变换红外光谱对各反应阶段的催化剂进行了表征,对其失活机制进行深入研究,结果表明,催化剂失活的主要原因是催化剂表面硫酸铵盐的沉积和催化剂本身活性成分的硫酸盐化.     

Cu/ZrO2/S2O2-8/γ-Al2O3固体酸催化剂制备与催化选择还原NO性能

以拟薄水铝石焙烧得到的γ-Al2O3为载体,分步浸渍负载（NH4）2S2O8、ZrOCl2和Cu（NO3）2,制成Cu/ZrO2/S2O28-/γ-Al2O3固体酸催化剂.考察了Cu/ZrO2/S2O8^2-/γ-Al2O3在富氧条件下对C3H6选择还原NO的催化性能,并借助SEM、XRD、Py-IR和TPR等表征方法研究了它的结构和性能的关系.性能的实验结果表明,Cu/ZrO2/S2O28-/γ-Al2O3在无水条件下能使NO的最大转化率达到82.9%,在有10%水蒸气存在条件下仍能使NO的最大转化率达到80.2%.表征测试的结果表明,S2O8^2-和ZrO2能够抑制γ-Al2O3颗粒之间的烧结及CuAl2O4尖晶石相的生成,同时促使催化剂表面新酸性中心（B酸）的形成及总酸量的增加,另外ZrO2还能提高Cu物种的还原性,从而有效地改善了催化剂的催化活性和水热稳定性.     

催化湿式氧化处理造纸废水的研究

以过渡金属氧化物CuO为活性组分,采用催化湿式氧化法处理造纸废水,考察Cu负载量、催化剂用量、反应温度对废水COD去除率的影响。结果表明:固定氧气分压在2.5MPa和反应时间3h,催化剂用量为3g,Cu负载量为4%,反应温度为220℃,500mL浓度为3250mg/L造纸废水的COD去除率为90%,色度去除率为89%,pH值由9.6变为7.8。另外,对催化剂进行再生处理和稳定性测试。结果表明:450℃下活化3h,在上述相同反应条件下,对原废水的COD去除率降低为88%,重复使用9次后对废水的COD去除率仍能保持在85%左右。     

Preparation and characterization of Fe2O3-CeO2-TiO2/γ-Al2O3 catalyst for degradation dye wastewater

In order to develop a catalyst with high activity for catalytic wet oxidation (CWO) process at room temperature and atmospheric pressure, Fe2O3-CeO2-TiO2/γ-Al2O3 catalyst was prepared by consecutive impregnation method and the prepared parameters were optimized. The structure of the catalyst was characterized by BET, XRF, SEM and XPS technologies, and the actual wastewater was used to investigate the catalytic activity of Fe2O3-CeO2-TiO2/γ-Al2O3 in CWO process. The experimental results showed that the prepared catalyst exhibited good catalytic activity when the doping amount of Ti was 1.0 wt% (the weight ratio of Ti to carriers), and the middle product, CeO2-TiO2/γ-Al2O3, was calcined in 450℃ for 2 h. The CWO experiment for treating actual dye wastewater indicated that the COD, color and TOC of actual wastewater were decreased by 62.23%, 50.12% and 41.26% in 3 h,respectively, and the ratio of BOD5/COD was increased from 0.19 to 0.30.     

CuxCe1-xO2/γ-Al2O3催化剂催化燃烧甲苯性能的研究

以γ-Al₂O₃ 为载体,以复合氧化物Cu_xCe_1-xO₂为活性组分,其中,x=0.1,0.2,0.4,0.6,0.8,通过浸渍法制备了一系列Cu_xCe_1-xO₂/γ-Al₂O₃催化剂.在固定床反应器中评价了催化剂对甲苯的催化活性,通过XRD、SEM对催化剂进行表征,并运用ICP-MS分析并计算Cu、Ce的摩尔比以及活性组分的负载量.结果表明,在Cu_xCe_1-xO₂/γ-Al₂O₃催化剂中Cu、Ce摩尔比的实际值与理论值相近,活性组分的负载量在19%以上,而且对甲苯都有较好的低温催化活性,其中当x=0.2时,即Cu_0.2Ce_0.8O₂/γ-Al₂O₃催化剂对甲苯的催化活性最高,其中T₁₀=160 ℃,T₉₀=265 ℃;当甲苯的进口浓度在700~3000 mg·m^-3时,进口浓度对Cu_0.2Ce_0.8O₂/γ-Al₂O₃催化剂的催化活性影响较小,且经过连续80 h的稳定性操作后转化率仍然保持在90%以上.     

负载型金属氧化物催化剂分解臭氧的研究

用浸渍法制备了活性炭、γ-氧化铝和分子筛负载的MnO2,CuO,Fe2O3催化剂,并考察了它们对臭氧分解的催化性能。结果表明,MnO2催化剂优于CuO,Fe2O3,催化剂,活性炭为载体的催化剂优于γ-氧化铝和分子筛为载体的催化剂。温度对臭氧催化分解影响很大,在90℃时,MnO2／AC催化剂对臭氧的去除率可达80％以上。当存在一定浓度的水蒸气时,湿度越大,催化性能越差。当臭氧初始质量浓度低于50mg／L时,随着臭氧初始浓度的增加,催化性能有一定的下降。     

Influence of NOx on the activity of Pd/θ-Al2O3 catalyst for methane oxidation: Alleviation of transient deactivation

Alumina supported Pd catalyst（Pd/Al₂O₃） is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900 °C and isothermal experiments at 650 °C were conducted to investigate the influence of NO_x on transient deactivation of Pd/θ-Al₂O₃ catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient d...     

O_3催化氧化深度处理兰炭废水的试验研究

采用O3催化氧化法深度处理兰炭废水,提出了兰炭废水达标排放的新处理方法。以铜为活性组分,氧化铝为载体采用浸渍法制备CuO/γ-Al2O3催化剂,并采用XRD对其进行表征,利用催化剂结合O3催化氧化法去除兰炭废水中经生化处理后残留的污染物。设计了催化氧化试验装置,考察了催化剂投加量、反应时间、O3用量以及pH等因素对处理效果的影响。实验结果表明,pH在酸性条件下有利于COD去除率的提高,O3用量提高有助于COD去除率的提高,将催化剂用量和反应时间控制在一定范围内有利于污染物的去除;最佳条件下催化剂投加量300 g,反应时间1 h,O3用量0.08 m3/h,pH为7左右时COD去除率可达到95%左右。另外,催化剂在20次反应过程中表现出较高的催化活性及较强的稳定性。     

CuO-CeO2/γ-Al2O3粒子电极对垃圾渗滤液降解特性

研制了负载型CuO-CeO2/γ-Al2O3粒子电极,并与活性炭颗粒混合填充于主阴阳极之间,实现三维电催化氧化反应,采用XRD、SEM对粒子电极进行表征.结果表明, CuO-CeO2/γ-Al2O3粒子电极对垃圾渗滤液显示了良好的电催化活性和稳定性,在pH为7.0、槽电压10V、空气流速0.04m3·h-1反应条件下,150min后, COD、氨氮去除率达到87.8%、45.4%,去除效果较传统二维平板、三维复极性电解槽更高,经20次反复使用后仍具有一定催化活性.研究了电-多相催化氧化体系对垃圾渗滤液降解的动力学规律,表明渗滤液降解符合准一级反应动力学规律;并在此条件下,体系以直接氧化占优.     

纳米铜复合材料催化还原染料废水的研究

以铜的有机金属框架为铜源前驱物,酚醛树脂为碳源,合成了多孔碳层支撑的Cu/Cu2O/C非贵金属复合材料.负载的Cu/Cu2O颗粒粒径在40nm左右,多孔碳层的高孔隙结构有利于Cu/Cu2O颗粒与目标物充分接触.将Cu/Cu2O/C作为催化剂用于水中多种染料类污染物(邻硝基苯、亚甲基蓝和罗丹明B)的催化还原反应中,材料重复利用5次后,目标物的降解率仍在99%以上,催化剂表现出了良好的催化活性和稳定性.     

Remove cooking fume using catalytic combustion over Pt/La-Al2O3

Five monolithic catalysts with low noble metal content were prepared by irnmerge method （Pt/γ=Al2O3, Pt/La-Al2O3, Pt/YSZ-AI203, Pt＋Pd/La-Al2O3 and Pd/La-Al2O3） and their activity measurements were carried out in a conventional fixed-bed flow reactor. The results show that La-Al2O3 can promote activity of the prepared catalysts and can decrease the complete conversion temperature of cooking fume. The Pt/La-Al2O3 catalyst has the highest activity and can be applied in wide range of gas hourly space velocity （GHSV）. Some characterizations （XRD, TPR） were carried out with the objective to explain differences in catalytic behaviors. The prepared catalyst showed a great potential for application.     

催化湿式氧化法处理桉木CTMP模拟废水

通过浸渍法制备固载金属非均相型催化剂,用于催化湿式氧化处理桉木CTMP模拟废水。结果表明:在焙烧温度400℃,焙烧时间4h,浸渍液浓度为6%,浸渍时间为5h下制得的CuO/γ-Al2O3催化剂的催化活性最好;在反应时间为8h,鞣酸溶液pH为4.5,H2O2加入量为0.2mL,催化剂用量为4g的条件下处理鞣酸溶液的效果最好,鞣酸去除率>90%。     

金属氧化物负载γ-Al_2O_3粒子电极对酸性橙Ⅱ的电催化氧化研究

以γ-Al_2O_3作为载体,采用浸渍热分解法制备了Sn、Mn、Cu、Pb单组分氧化物和Sn-Ce-Sb复合氧化物粒子电极。通过对酸性橙II(AOII)的降解实验,以及采用重复试验和扫描电镜(SEM)、紫外光谱扫描等方法,探讨了粒子电极材料的性能。研究结果表明:Sn/γ-Al_2O_3相比于Mn/γ-Al_2O_3、Cu/γ-Al_2O_3、Pb/γ-Al_2O_3等单组分氧化物粒子电极表现出了更好的电催化活性和稳定性。掺杂Ce、Sb后电极表面晶体粒径细小且分布均匀,有利于提高Sn/γ-Al_2O_3粒子电极的性能。电流密度为20 m A/cm2,曝气量0.5 L/min反应条件下,反应3 h后Sn-Ce-Sb/γ-Al_2O_3粒子电极对AOII的去除率为100%,TOC的去除率达84.2%,重复使用5次后TOC去除率仍保持在80%以上。表明Sn-Ce-Sb/γ-Al_2O_3粒子电极具有较好的应用前景。     

负载型燃烧催化剂La_(0.8)Ce_(0.2)CoO_3/Ce_(0.8)Zr_(0.2)O_2制备及性能研究

以复合氧化物La0.8Ce0.2CoO3为活性组分,Ce0.8Zr0.2O2固溶体为载体,采用柠檬酸络合法制备出负载型燃烧催化剂La0.8Ce0.2CoO3/Ce0.8Zr0.2O2。用XRD、BET和SEM对其进行表征,考察了焙烧温度、反应时间、反应温度及H2S存在对催化剂活性的影响。结果表明,载体表面形成了均一的钙钛矿相;该负载型催化剂对二甲苯完全氧化反应具有较高的催化活性,有良好的热稳定性、操作稳定性和强的抗H2S毒化能力。这可能是载体与负载组分之间密切的协同作用所导致。     

ZnO包覆Al_2O_3的制备表征及光催化性能研究

采用化学沉积法制备了ZnO包覆Al2O3光催化剂,并通过X射线衍射(XRD)、扫描电镜(SEM)进行了表征。在自制的光化学反应器中,以中压汞灯作光源,一定浓度的甲基橙为光催化反应模型化合物,研究了光催化剂的活性。考察了甲基橙初始浓度、催化剂加投量、pH值、温度、光照强度、反应液体积等因素对脱色率的影响。实验结果表明,ZnO包覆Al2O3复合光催化剂具有较高的光催化活性。在250W中压汞灯下光照3h,0.10g复合光催化剂能使200mL,10mg/L甲基橙溶液的脱色率达到92.21%。     

催化湿式氧化法降解活性艳蓝的研究

以Fe2O3/γ-Al2O3为催化剂的非均相催化氧化体系处理活性艳蓝KN-R。考察了反应时间、反应温度、pH和Fe2O3/γ-Al2O3投加量等因素对降解效果的影响。结果表明,染料初始浓度为200mg/L时,在温度150℃、压力0.5MPa、H2O233mg/L、pH=6,反应时间1h,Fe2O3/γ-Al2O3投加量为8g/L的最佳条件下,活性艳蓝KN-R色度几乎完全去除,TOC和COD去除率分别为95.6%和82.5%。