阴极扩展电催化还原法对五氯苯酚的脱氯特性

以负载Pd催化剂的活性碳纤维作为扩展阴极,对吸附在活性碳纤维上的五氯苯酚进行了电催化还原脱氯研究.考察了电解质浓度、催化剂含量、电流密度等主要因素对还原脱氯效率的影响.结果表明,电解质浓度0.25 mol·L-1,温度40℃,电流密度25 mA·cm-2,催化剂Pd的含量5%,反应4 h,五氯苯酚的降解率可达到94.3%.通过中间产物的分析对电催化还原脱氯反应机理进行了初步探讨.     

Cu-Ag/海泡石催化还原NO的研究

以天然海泡石为原料,对其进行酸改性并与活性氧化铝混合后作为催化剂载体,采用浸渍法制备了用于CO还原NO的Cu-Ag复合金属催化剂.对不同Ag负载量催化剂催化还原NO的活性进行了评价,考察了载体对催化剂催化活性的影响,用BET、XRD、SEM等对催化剂进行了表征.结果表明,当Ag负载量不超过5%时,复合金属催化剂性能好于单一金属催化剂;Ag负载量为2%时催化剂性能最好;采用海泡石-氧化铝混合物为载体的催化剂的孔径分布得到改善,对NO催化还原反应有更高的活性.     

等离子体耦合Ce改性的复合型催化剂去除氮氧化物研究

为开发一种在大气污染物条件下可以复合催化氮氧化物的自制锯板脉冲放电反应器,同时为进一步制备高性能催化剂研究提供试验依据,采用脉冲放电耦合复合型催化剂对NOx进行去除试验.通过分步浸渍法制备一系列催化剂,研究脉冲放电耦合不同活性组分催化剂的脱硝效果,其中重点研究Fe掺杂及其不同掺杂量下制备的Fe/5A催化剂对NO转化率的影响.此外,进一步对Fe/5A催化剂掺杂适量Ce进行改性,进而制备复合型Ce-Fe/5A催化剂.通过XRD、SEM对催化剂进行相关性能表征.结果表明,Fe/5A催化剂活性在Cu/5 A,Mn/5 A,Cr/5A催化剂中最优,且当Fe掺杂的质量分数为8％时,单组分Fe/5A分子筛活性最好.掺杂一定量Ce后的Ce-Fe/5A催化剂表面更光滑,微孔增多,比表面积增大,被覆盖的不饱和金属配位点更易暴露以增加反应所需的活性点位,进而促进催化反应的有效进行,加强对NOx的脱除.当Ce掺杂的质量分数为3％时,Ce-Fe/5A催化剂对NO转化率效果最佳.由于脉冲放电可以改变催化剂的晶形和结构,因此Ce-Fe/5A催化剂耦合脉冲放电可以显著提高脱硝效率,其中添加还原性气体C2H2后效果更佳,且随着电压的增加,Ce-Fe/5A催化剂脱硝效果整体呈上升趋势.     

La/γ-Al2O3催化剂的改性及其催化还原脱硫活性研究

设计了一套模拟烟气催化还原脱硫实验装置.采用分步浸渍法,用Ce、Fe和Ti 对La/γ-Al2O3催化剂进行改性,实验对比分析了在不同的反应温度下改性前后催化剂的脱硫活性,以获取具有较高脱硫活性及较低反应温度的还原脱硫催化剂.实验结果表明,催化剂9%La-3%Fe-5%Ce-0.8%Ti/γ-Al2O3在420℃的反应...     

V2O5/TiO2催化剂选择性催化还原脱除NOx的研究

通过浸渍法制备V2O5/TiO2催化剂,在固定床反应器中进行NH3选择性催化还原脱除NOx的研究.结果表明,对于100/140目催化剂,NOx转化率随反应时间线性增加,NH3选择性催化还原NOx反应为一级反应,反应活化能为98.23 kJ*mol-1.对于片状催化剂,气体流量和催化剂的厚度对脱氮反应有较大的影响,气体流量增加,NOx转化率提高,当流量增至120 L*h-1后,NOx转化率趋于稳定;催化剂厚度由0.1 cm增至0.2 cm, NOx转化率从83%降至40%, 催化剂有效因子从0.254降至0.127.对于0.1 cm厚的片状催化剂,在573 K和空速1.4 s-1条件下,NOx转化率可达92%.     

柱状V2O5/AC催化剂低温选择性催化还原NO的研究

为了研究柱状活性焦负载V2O5选择性催化还原NO的性能,采用等体积浸渍法制备一系列柱状V2O5/AC催化剂,采用工业分析、元素分析、SEM、BET对催化剂进行表征.结果表明,柱状活性焦表面具有大量的孔隙结构,硝酸改性提高活性焦的氧含量、比表面积和微孔率.同时研究了V2O5负载量、反应温度、Q浓度、空速等因素对NO脱除率的影响.结果表明,在V2O5负载量为3％、反应温度150℃,O2体积分数为5％,空速2500 L/(M·h)时NO的脱除率可达61.89％.     

低温NH3-SCR脱硝催化剂研究进展

低温NH3-SCR脱除NOx是一种有潜力的烟气脱硝技术.综述了低温NH3-SCR脱硝催化剂的研究现状,重点介绍了锰基催化剂、钒基催化剂,以及其他金属氧化物基催化剂的研究状况,阐述了制备方法、催化剂载体,以及以不同金属改性对催化剂脱硝活性的影响.其中具备高比表面积、良好非晶态结构的低温NH3-SCR催化剂都有良好的低温脱硝活性.以CeO2改性锰(MnOx)基催化剂为例,探讨了低温NH3-SCR脱硝催化剂的脱硝机理.反应气体(NH3、NO和O2)在催化剂表面的吸附在低温NH3-SCR脱除NOx中发挥了重要作用.CeO2改性锰基催化剂催化NH3-SCR反应过程中涉及ER机理和LH机理,并且NH2与气态NO发生反应生成亚硝胺(NH2NO),进一步分解为N2和H2O是关键步骤.就燃煤烟气中水蒸气(H2O)和SO2在低温条件下对低温NH3-SCR脱硝催化剂的失活机制进行了阐述.烟气中的水蒸气与反应气体的竞争性吸附能够导致催化剂脱硝活性的降低.水蒸气(H2O)和SO2共同存在对低温NH3-SCR催化剂脱硝活性的影响表现为两者共同作用.烟气中水和SO2存在时生成的硫酸盐沉积在催化剂表面,并导致催化剂失活.     

负载型膨胀石墨催化剂低温催化氧化NO研究

膨胀石墨(EG)具有四级孔结构,是一种优良的吸附剂和催化剂载体.采用超声浸渍法制备了Mn/EG催化剂,用于低温催化氧化NO,考察了金属负载量、进口NO质量浓度及O2体积分数对NO氧化效率的影响.结果表明,利用超声浸渍法制备得到的Mn/EG催化剂低温催化氧化活性较好,且催化剂表面的3价Mn对反应活性有重要影响.进口气体中O2体积分数对反应活性有明显的影响,低温时高体积分数的氧能促进NO的转化.150℃时,在NO体积分数为0.05％、O2体积分数为3％、空速为47 770 h-1的条件下,该催化剂的NO催化氧化效率可达42％.     

蜂窝状微量贵金属催化剂对几种典型VOCs的催化氧化性能

研制出了用于催化氧化废气中挥发性有机化合物(VOCs)的蜂窝状微量贵金属催化剂.用浸渍法制备催化剂Pt-Ce-La-Zr/Al2O3,并在自行设计的活性检测系统上,对用该催化剂净化含有苯、甲苯、乙醇、正己烷的模拟废气进行了研究,考察了空速、质量浓度等因素对催化剂活性的影响.实验结果表明,该催化剂对上述几种典型的VOCs气体都具有较低的起燃温度,其催化转化活性较好.     

基于烧结矿催化还原的烧结烟气脱硝试验研究

以烧结矿为催化剂对烧结烟气进行选择性催化还原(SCR)脱硝,研究了反应温度、NH3/NO物质的量比、空速和烧结矿粒径对烧结烟气SCR脱硝的影响.结果表明:烧结矿催化还原烧结烟气脱硝效果明显;烧结矿SCR脱硝的适宜窗口温度为350 ～ 450℃;随NH3/NO物质的量比增大、烧结矿粒径减小、空速(气体流速/催化剂体积)降低,脱硝效率提高;在反应温度为450℃、NH3/NO物质的量比为1.0、空速为3000h-1的条件下,用粒径为0.2～ 1.0 mm的烧结矿脱除烧结烟气中的NO,可以将NO质量浓度从400 mg/m3降到约260 mg/m3.     

反应条件对矿用充填发泡树脂活性的影响研究

采用二价金属A作为催化剂,合成矿用发泡树脂。通过测定树脂的固含量、黏度、凝胶时间、羟甲基指数等,研究反应温度、时间和催化剂用量对矿用发泡树脂活性的影响。试验结果表明:随着反应时间的延长、温度的升高、催化剂用量的增加,树脂的黏度和固含量逐渐增加,而树脂中残余B、残余C和凝胶时间逐渐减少。在较高温度下,羟甲基指数随着反应时间的延长先增加后减少;在较低温度下,羟甲基指数随着反应时间的延长先减少后增加;较大的催化剂用量有利于树脂缩合反应,较低的用量有利于促进B与C的羟基化反应。     

整装催化转化器中CO氧化的数值模拟

研究整装催化转化器中CO氧化的起燃过程.建立了起燃过程数学模型,通过数值计算,分析和讨论了起燃过程中温度的变化,气流性质和催化剂性质各种参数对转化器起燃性能的影响.结果表明,在起燃过程中,壁温峰值的位置逐渐向催化剂入口处移动;固相导热系数在反应点火前后对壁温峰值位置的影响不同;增大CO浓度、增大气体流速、降低气体温度会延迟催化剂的起燃;缩短催化剂长度、增大孔密度有利于起燃.参数分析有助于反应器的设计和建模.     

Thermal hazard assessment for synthesis of 3-methylpyridine-N-oxide

The exothermic oxidation of 3-methylpyridine with hydrogen peroxide was analyzed by Reaction Calorimeter (RC1e) in semi-batch operation. Heat releasing rate and heat conversion were studied at different operating conditions, such as reaction temperature, feeding rate, the amount of catalyst and so on. The thermal hazard assessment of the oxidation was derived from the calorimetric data, such as adiabatic temperature rise (ΔT_ad) and the maximum temperature of synthesis reaction (MTSR) in out of control conditions. Along with thermal decomposition of the product, the possibility of secondary decomposition under runaway conditions was analyzed by time to maximum rate (TMR_ad). Also, risk matrix was used to assess the risk of the reaction. Results indicated that with the increase of the reaction temperature, the reaction heat release rate increased, while reaction time and exotherm decreased. With the increase of feeding time, heat releasing rate decreased, but reaction time and exotherm increased. With the amount of the catalyst increased, heat releasing rate increased, reaction time decreased and exothermic heat increased. The risk matrix showed that when the reaction temperature was 70 °C, feeding time was 1 h, and the amount of catalyst was 10 g and 15 g, respectively, the reaction risk was high and must be reduced.     

Biodiesel production from waste oil feedstocks by solid acid catalysis

Biodiesel is a non-toxic and biodegradable substitute for petroleum-based diesel. However, it is impractical to use refined edible oils to produce biodiesel due to its high cost and priority for food products, especially in China, while waste oils with high free fatty acids (FFAs) can be considered as the raw materials. In the present work, a solid acid catalyst comprising SO₄²⁻/TiO₂–SiO₂ was prepared, characterized and studied for its activity for the production of biodiesel from several low cost feedstocks with high FFAs. The solid acid catalyst can be recycled, easily removed and can simultaneously catalyze esterification and transesterification. The influence of reaction parameters was studied, and the optimized reaction parameters are reaction temperature 200 °C, molar ratio of methanol to oil 9:1 and catalyst concentration 3 wt.%. The catalyst showed good stability. A continuous process for biodiesel production from cheap raw feedstocks was proposed, and a 10,000-tonnes/year biodiesel production demonstration plant has been built.     

陶瓷管表面NaHCO3粉体干法脱硫研究

探讨Na HCO3的加热分解特性并将其负载于陶瓷管表面进行了脱硫实验研究,发现Na HCO3在合理的灼烧温度下将在热分解为Na2CO3的过程中形成多孔结构,可在没有液相水存在的情况下成功实现SO2去除,灼烧温度过高则发生颗粒烧结从而降低脱硫效果;进口气流SO2浓度150 ppm的情况下,陶瓷管表面厚度仅仅50μm的Na HCO3粉体可以在20~40 min内将出口气流中的SO2限制在17.5 ppm(50 mg/m^3)的超净排放限值以下。Na HCO3作为干法脱硫剂可在不明显提高烟气湿度和降低其温度的条件下成功实现脱硫,结合陶瓷过滤管的除尘作用,有望实现烟气的深度除尘和脱硫操作的一体化。     

Optimization of biodiesel production from the waste cooking oil using response surface methodology

In this research, transesterification of the waste cooking oil has been studied. Response surface methodology (RSM) based on Box–Behnken design was used to investigate the effects of the main operating parameters, including the methanol to oil molar ratio, catalyst concentration, and reaction temperature, on the biodiesel yield. The results revealed that the catalyst concentration is the most important parameter. The maximum biodiesel yield under the optimized conditions was 99.38 wt.%. Thermogravimetric analysis (TGA) was used for the determination of biodiesel conversion and the results were compared with that of gas chromatography (GC) analysis, showing a very small difference. Furthermore, an empirical quadratic equation has been presented to show the relation between biodiesel conversion and product viscosity.     

车用催化转化器起燃温度的数值模拟

车用催化转化器是降低汽车排气污染物浓度的主要装置.起燃温度是催化转化器的重要特性之一,它表明催化器在多高的温度下有较高转化率.数值模拟研究催化转化器的性能可以减少实验量,指导和优化催化器的设计.建立了催化转化器一维稳态转化率的数学模型,对起燃温度特性曲线进行模拟.数值模拟结果与实验测量值较吻合.这说明,建立的数学模型可以用来模拟起燃温度特性曲线.用该模型考察了空速、载体长度、催化剂比表面积、载体导热系数以及壁厚等因素对起燃温度特性曲线的影响.结果表明,空速越大,催化转化器的起燃温度越高;增大载体长度和催化剂比表面积有利于降低起燃温度;载体导热系数和壁厚的大小对起燃温度几乎没有影响.     

神经网络预测催化超临界水氧化废水效果的研究

在间歇式反应器中进行催化超临界水氧化DDNP废水试验,考察催化剂浓度、反应温度、压力、停留时间对氧化效果的影响。在实验基础上采用BP神经网络算法,建立以催化剂浓度、反应温度、压力、停留时间作为网络模型的输入层,COD去除率作为输出层的双隐层BP神经网络预测模型,预测催化超临界水氧化废水的效果,仿真结果表明模型预测效果较好。     

The influence of temperature on the deactivation of commercial Pd/Rh automotive catalysts

Automotive catalyst deactivation can be promoted by thermal and poisoning mechanisms. Catalyst efficiency is reduced by thermal degradation resulting in the agglomeration of precious metals and the reduction of the washcoat surface area. In this paper, the temperature influence on the commercial Pd/Rh-based automotive catalyst performance was studied. Textural and physicochemical characterisation techniques were employed, such as X-ray fluorescence (XRF), atomic absorption spectrometry (AAS), N₂ physisorption, X-ray diffraction (XRD), temperature programmed reduction (TPR) and scanning electron microscopy coupled with energy-dispersive X-ray analysis (SEM–EDX). The catalysts were evaluated for CO and propane oxidation with a stoichiometric gas mixture similar to engine exhaust gas. The results indicated the transformation of alumina into high temperature phases and the formation of new mixed oxide phases. Evidence of sintered particles and several spots of palladium agglomerates was seen by SEM–EDX analysis. The activity results showed the effects of thermal deactivation on the conversion of the pollutants. In spite of exposure to extreme temperature conditions (72 h at 1200 °C), significant activity was still observed for carbon monoxide and propane oxidation reactions.     

Optimization of biodiesel production by alkali-catalyzed transesterification of used frying oil

Biodiesel as an alternative fuel for fossil diesel has many benefits such as reducing regulated air pollutants emissions, reducing greenhouse gases emissions, being renewable, biodegradable and non-toxic. In this study, used frying oil was applied as a low cost feedstock for biodiesel production by alkali-catalyzed transesterification. The design of experiments was performed using a double 5-level-4-factor central composite design coupled with response surface methodology in order to study the effect of factors on the yield of biodiesel and optimizing the reaction conditions. The factors studied were: reaction temperature, molar ratio of methanol to oil, catalyst concentration, reaction time and catalyst type (NaOH and KOH). A quadratic model was suggested for the prediction of the ester yield. The p-value for the model fell below 0.01 (F-value of 27.55). Also, the R² value of the model was 0.8831 which indicates the acceptable accuracy of the model. The optimum conditions were obtained as follows: reaction temperature of 65 °C, methanol to oil molar ratio of 9, NaOH concentration of 0.72% w/w, reaction time of 45 min and NaOH as the more effective catalyst. In these conditions the predicted and observed ester yields were 93.56% and 92.05%, respectively, which experimentally verified the accuracy of the model. The fuel properties of the biodiesel produced under optimum conditions, including density, kinetic viscosity, flash point, cloud and pour points were measured according to ASTM standard methods and found to be within specifications of EN 14214 and ASTM 6751 biodiesel standards.