催化臭氧化降解含微囊藻毒素污水

应用金属氧化物构建催化臭氧化工艺处理含微囊藻毒素污水,比较了不同催化剂的性能差异,分析了催化剂投加量、温度、pH、原水浓度对该工艺的影响.结果表明,选用CuO作催化剂能较好地处理含微囊藻毒素污水.温度与原水浓度对该工艺影响较小;催化剂投加量与pH是该工艺的主要影响因素.实验温度40℃、混合气体流量1.8 L.L-.1min-1、pH=9、催化剂投加量5 g.L-1、处理时间60 min,原水MC-LR去除率达到90%以上、COD去除率达到64%以上.处理20 min,该工艺催化作用去除MC-LR贡献率达到28%、去除COD贡献率达到52%.     

异质结型光催化剂CuO/SnO2的制备及产氢性能

光催化降解有机废水可以实现在降解污染物同时回收清洁能源.本研究采用简单沉淀法制备了CuO/SnO2系列复合光催化剂,并用XRD、TEM对其结构进行表征.分别考察了氧化铜含量和乙醇浓度对复合材料光催化产氢性能的影响.实验结果表明,通过氧化铜与二氧化锡适当比例复合能显著提高复合材料的光催化产氢性能.复合材料48.51%CuO/SnO2的产氢性能比纯二氧化锡提高了近5倍.乙醇的浓度也对复合材料的产氢性能有较大影响,最佳的乙醇浓度为2.00 mol.L-1左右.长时间光催化产氢结果表明,每降解废水中1 kg的COD可产生氢气3724 mL.另外,对复合材料光催化分解乙醇的产氢机理也进行了分析.     

水热法制备PbMoO4微晶体及其光催化降解灭幼脲

以水热法合成的PbMoO4微晶体为催化剂,考察了反应溶液pH、污染物初始浓度和催化剂用量对光催化降解灭幼脲的影响,研究了光催化降解过程的反应动力学和作用机理.结果表明,最佳反应溶液pH 6.0、污染物初始浓度20 mg.L-1、催化剂用量0.4 g.L-1.反应4 h灭幼脲降解率达99.96%,矿化率达66.4%,降解反应符合一级动力学.通过加入自由基清除剂对比实验发现,PbMoO4微晶体主要通过空穴和.OH的氧化作用使灭幼脲降解,其中空穴起主要作用.     

Experimental study on oxidative decomposition of nitrobenzene in aqueous solution by honeycomb ceramic-catalyzed ozonation

The ozonation of nitrobenzene in aqueous solution was carried out in a semi-batch reactor to investigate the degradation efficiency, the effect factors, and the reaction mechanism, where honeycomb ceramic was used as a catalyst. The presence of honeycomb ceramic could improve the degradation rate of nitrobenzene by 15.46% compared to the results of ozonation alone. Under the conditions of this experiment, the degradation rate of honeycomb ceramic-catalyzed ozonation increased by 12.94% with the increase of the amount of catalyst from 1 to 5 blocks. The degradation rates all increased greatly with the increase of temperature and pH of the solution in the processes of honeycomb ceramiccatalyzed ozonation and ozonation alone. But, when the pH of the solution increased to 9.50, the advantage of the honeycomb ceramic-catalyzed ozonation process would be lost. The experimental findings indicated that in the processes of ozonation alone and honeycomb ceramic-catalyzed ozonation, nitrobenzene was primarily oxidized by ·OH free radical in aqueous solution. The adsorption of nitrobenzene was too limited to have an important influence on the degradation rate of nitrobenzene. With the same total dosage of applied ozone, the multiple step addition of ozone showed much higher removal efficiency than that obtained by one step in the two processes.     

易挥发有机化合物在Pt/Al_2O_3-Si纤维催化剂上的低温氧化

本文合成了一种新型的Pt负载在Al_2O_3涂膜强力富硅纤维载体的催化剂,研究低温下催化易挥发有机化合物的行为.用四种有机化合物检验实验参数对催化剂分解有机化合物分解率的影响.讨论了流速、浓度、有机物的本性、预热温度、反应热等参数的影响,并给出了催化剂对苯、甲苯在特定实验条件下的活化能、反应级数和指前因子的数值.     

树脂负载α-FeOOH异相光Fenton降解水中己烷雌酚

以Amberlite200树脂为载体,在Fe(NO3)3-HNO3体系中恒温水解制备了负载型催化剂α-FeOOH/Resin,以己烷雌酚(HEX)为目标化合物,研究了α-FeOOH/Resin的异相Fenton催化性能.结果表明,α-FeOOH/Resin异相Fenton反应能够有效降解水中的HEX,紫外光和H2O2的协同作用很大程度地提高了降解效率;pH值的降低或初始H2O2浓度的提高,均能增加HEX的降解速率;在中性条件下,HEX的光Fenton降解过程中,溶出的铁元素对降解贡献不大,异相Fenton反应起主导作用;催化剂重复使用后仍具有较好的催化活性和机械强度,说明铁在其表面负载牢固,催化剂具有一定的实用性.     

含氮有机物在Pt／HM,Pd／HM和CuO／HM催化剂上的氧化降解

本文考虑了乙腈、硝基甲烷和乙二胺在Ｐｔ／ＨＭ，Ｐｄ／ＨＭ和ＣｕＯ／ＨＭ催化剂上氧化降解产物随反应温度的变化。在实验温度范围内，含氮产物在Ｎ２，Ｎ２Ｏ和ＮＯ２。随着反应温度的升高，硝基甲烷氧化降解的Ｎ２选择性呈单调下降；而乙腈和乙二胺的Ｎ２选择性出现极小值；高温时Ｎ２选择性升高可能是氧化生成的ＮＯ在高温时更在利于和ＣＮ基或ＮＨ２基相互反应生成Ｎ２的缘故。对于乙腈和乙二胺的催化氧化降解活性为：Ｐｔ／Ｈ     

以ZrO2为载体的金属氧化物催化剂对NO还原性能的研究

研究了负载于氧化锆载体上的多种金属氧化物在富氧条件下,以丙烯为还原剂,选择性还原NO的活性,考察了CuO和Ag的负载量与活性关系,CuO和Ag单独负载与共同负载时的催化性能,以及氧气浓度对催化剂活性影响.结果表明:在CuO,MgO,La2O3 ,CoO,Fe2O3 ,MoO3和WO3等七种金属氧化物中,CuO活性最好,NO转化率为47.5%,加入活性组分银可明显提高催化剂的NO还原能力,转化率提高到61%.单独负载银时,催化剂活性较差,NO转化率仅为22.1%.在对氧气浓度的考察中,确定在0.4%NO,0.4?H6的反应气中,氧气的最佳含量为2%.     

Effect of Cu-ZSM-5 catalysts with different CuO particle size on selective catalytic oxidation of N,N-Dimethylformamide

● A series of Cu-ZSM-5 catalysts were tested for DMF selective catalytic oxidation. ● Cu-6 nm samples showed the best catalytic activity and N₂ selectivity. ● Redox properties and chemisorbed oxygen impact on DMF catalytic oxidation. ● Isolated Cu²⁺ species and weak acidity have effects on the generation of N₂. N, N-Dimethylformamide (DMF), a nitrogen-containing volatile organic compound (NVOC) with high emissions from the spray industry, has attracted increasing attention. In this study, Cu-ZSM-5 catalysts with different CuO particle sizes of 3, 6, 9 and 12 nm were synthesized and tested for DMF selective catalytic oxidation. The crystal structure and physicochemical properties of the catalyst were studied by various characterization methods. The catalytic activity increases with increasing CuO particle size, and complete conversion can be achieved at 300–350 °C. The Cu-12 nm catalyst has the highest catalytic activity and can achieve complete conversion at 300 °C. The Cu-6 nm sample has the highest N₂ selectivity at lower temperatures, reaching 95% at 300 °C. The activity of the catalysts is determined by the surface CuO cluster species, the bulk CuO species and the chemisorbed surface oxygen species. The high N₂ selectivity of the catalyst is attributed to the ratio of isolated Cu²⁺ and bulk CuO species, and weak acidity is beneficial to the formation of N₂. The results in this work will provide a new design of NVOC catalytic oxidation catalysts.     

Photocatalytic water splitting of ternary graphene-like photocatalyst for the photocatalytic hydrogen production

•The MoS₂/SiC/GO composite has a strong photocatalytic activity than SiC. •The optimal catalyst yielded the highest quantum of 21.69%. •GO acts as a bridge for electron passage in photocatalytic reaction. In recent times, therehas been an increasing demand for energy which has resulted in an increased consumption of fossil fuels thereby posing a number of challenges to the environment. In the course finding possible solutions to this environmental canker, solar photocatalytic water splitting to produce hydrogengas has been identified as one of the most promising methods for generating renewable energy. To retard the recombination of photogenerated carriers and improve the efficiencyof photocatalysis, the present paper reports a facile method called the hydrothermal method, which was used to prepare ternary graphene-like photocatalyst. A “Design Expert” was used to investigate the influence of the loading weight of Mo and GO as well as the temperature of hydrothermal reaction and their interactions on the evolution of hydrogen (H₂) in 4 h. The experimental results showed that the ternary graphene-like photocatalyst has a strong photocatalytic hydrogen production activity compared to that of pure SiC. In particular, the catalyst added 2.5 wt% of GO weight yielded the highest quantum of 21.69 % at 400–700 nm of wavelength. The optimal evolution H₂ in 4 h conditions wasobtained as follows: The loading weight of Mo was 8.19 wt%, the loading weight of GO was 2.02 wt%, the temperature of the hydrothermal reaction was 200.93°C. Under the optimum conditions, the evolution of H₂ in 4 h could reach 4.2030 mL.     

Microwave enhanced stabilization of copper in artificially contaminated soil

Microwave processing was used to stabilize copper ions in soil samples. Its effects on the stabilization efficiency were studied as a function of additive, microwave power, process time, and reaction atmosphere. The stabilization efficiency of the microwave process was evaluated based on the results of the toxicity characteristic leaching procedure (TCLP) test. The results showed that the optimal experimental condition contained a 700W microwave power, 20 min process time and 3 iron wires as the additive, and that the highest stabilization efficiency level was more than 70%. In addition, the different reaction atmospheres showed no apparent effect on the stabilization efficiency of copper in the artificially contaminated soil. According to the result of the Tessier sequential extraction, the partial species of copper in the contaminated soil was deduced to transform from unstable species to stable states after the microwave process.     

生物膜法降解甲苯废气过程的探讨

采用陶粒为填料的生物滤池降解甲苯废气，并对清水试验和生物膜试验的结果进行分析，发现生物膜法降解甲苯这样的挥发性有机物（VOCs)具有良好的效果，已不再是清水试验中单纯的物理吸收过程，而是伴有生化反应的吸收过程，是以气膜控制为主的传质过程。     

六铝酸盐负载CuO催化还原NO性能

采用共沉淀法制备了LaAl12O19六铝酸盐载体,采用等体积浸渍法制备了不同负载量的CuO/LaAl12O19催化剂,并对其进行了XRD、H2-TPR和BET表征,考察了催化剂对CH4选择催化还原NO的性能.结果表明,CuO的负载并未改变六铝酸盐载体的结构,Cu在载体上以Cu2+的形式存在,活性组分CuO与载体LaAl12O19之间存在协同作用;CuO/LaAl12O19催化剂对CH4选择催化还原NO表现出良好活性,所制备的催化剂均能使NO的转化率达到99%;其中负载量为1.0 wt%的CuO/LaAl12O19催化剂的活性最好,完全反应温度T99%为560℃,且在80 h稳定性试验中表现出了良好的高温活性和热稳定性.     

Fe—C微电解法＋H2O2组合工艺处理对氯硝基苯废水

利用废铁屑对对氯硝基苯废水进行预处理 ,可以使废水中的对氯硝基苯转化为氨基氯苯 ,然后在废水中加入H2 O2 ,使H2 O2 与废水中的Fe2 + 构成Fenton试剂 ,反应生产OH·自由基 ,OH·自由基具有强烈的氧化性 ,将氨基氯苯和对氯硝基苯中的苯环打开 ,形成断链 ,再进一步将其矿化分解     

Removal of methylene blue by coupling black carbon adsorption with TiO2 photodegradation

In this study, the removal of methylene blue (MB) by the coupling of black carbon (BC) and TiO₂ was investigated. The effects of different parameters such as catalyst dose, sorbent, initial concentrations of dye, pH of the solutions, recycles on discoloration, and chemical oxidation demand (COD) reduction of MB were monitored to optimize the reaction conditions. The discoloration and COD conversation rate of MB obtained by the coupling process were 100% after 90?min irradiation. The synergistic effect of MB-adsorption on BC followed by degradation through TiO₂ photocatalysis was proved by FT–IR spectrophotometer. The BC as by-product of natural materials is a promising adsorbent for waste water treatment.     

Self-sustained catalytic combustion of CO enhanced by micro fluidized bed: stability operation,fluidization state and CFD simulation

● Catalytic combustion in fluidized bed realizes efficient heat and mass transfer. ● Catalytic combustion in fluidized bed reduces the lean combustion limits. ● Catalytic combustion and flame combustion can be coupled. ● The diffusion/kinetics limited reaction model is suitable for catalytic combustion. A micro fluidized bed reactor was used to study the self-sustaining catalytic combustion of carbon monoxide (CO). The Cu_1−xCe_xO_y catalyst, as well as the pure CuO and CeO₂, are used to investigate the contributing mechanism of different active sites including dispersed CuO and Cu–Ce solid solutions. The ignition temperature (T_i) of CO over these catalysts at a flow rate of 2000 mL/min followed the order: 74 °C (Cu_0.5Ce_0.5O_y) < 75 °C (Cu_0.25Ce_0.75O_y) < 84 °C (Cu_0.75Ce_0.25O_y) < 105 °C (CuO) < 500 °C (CeO₂). Furthermore, the lean combustion limits (equivalence ratio ϕ) over these catalysts under the flow rates of 750–3000 mL/min (through fixed, bubbling, and fluidized bed) were also measured, which are Cu_0.5Ce_0.5O_y < Cu_0.25Ce_0.75O_y < Cu_0.75Ce_0.25O_y < CuO < CeO₂. The fluidized bed was simulated using the Eulerian two-fluid model (TFM) coupled with a diffusion/kinetic-limited reaction model to evaluate the influence of operation conditions on the self-sustained combustion of CO. The predicted maximum temperature agreed with the experimental measurements, demonstrating the validity of the kinetic model and simulation parameters. The results of catalytic combustion with increasing CO concentrations suggest that the catalytic combustion reaction could co-exist with the flamed combustion. When a high concentration of CO is used, a blue-purple flame caused by CO combustion appears in the upper part of the fluidized bed, indicating that the range of CO-containing exhaust gas purification could be expanded to a larger range using the fluidized-bed catalytic combustion technique.     

酞菁锌改性介孔分子筛催化降解孔雀石绿

以介孔分子筛MCM-41为载体,采用浸渍法将1,4,8,11,15,18,22,25-八环戊氧基酞菁锌(α-CyOPcZn)负载到分子筛上得到了一种新型的催化剂CyOPcZn/MCM-41.并通过氮气吸附、红外光谱扫描及电镜扫描对催化剂的结构进行表征.考察了该催化剂的用量、H2O2浓度对孔雀石绿降解作用的影响.实验结果表明,在模拟可见光照射下,当催化剂用量0.6 g.L-1、H2O2浓度为0.1 mmol.L-1时,60 min后使0.1 mmol.L-1的孔雀石绿水溶液的脱色率达到98.6%,并呈现出一级反应的动力学特征,速率常数k为0.0891 min-1.催化剂重复使用3次后,脱色率可达96%以上.     

Combined ultrasound with Fenton treatment for the degradation of carcinogenic polycyclic aromatic hydrocarbons in textile dying sludge

To develop an effective method to remove the toxic and carcinogenic polycyclic aromatic hydrocarbons (CPAHs) from textile dyeing sludge, five CPAHs were selected to investigate the degradation efficiencies using ultrasound combined with Fenton process (US/Fenton). The results showed that the synergistic effect of the US/Fenton process on the degradation of CPAHs in textile dyeing sludge was significant with the synergy degree of 30.4. During the US/Fenton process, low ultrasonic density showed significant advantage in degrading the CPAHs in textile dyeing sludge. Key reaction parameters on CPAHs degradation were optimized by the central composite design as followed: H₂O₂ concentration of 152 mmol/L, ultrasonic density of 408 W/L, pH value of 3.7, the molar ratio of H₂O₂ to Fe²⁺ of 1.3 and reaction time of 43 min. Under the optimal conditions of the US/Fenton process, the degradation efficiencies of five CPAHs were obtained as 81.23% (benzo[a]pyrene) to 84.98% (benz[a]anthracene), and the benzo[a]pyrene equivalent (BaP_eq) concentrations of five CPAHs declined by 81.22–85.19%, which indicated the high potency of US/Fenton process for removing toxic CPAHs from textile dyeing sludge.     

三维电极电化学反应器组合Fenton试剂深度处理焦化废水

采用三维电极电化学反应器组合Fenton试剂法对经过二级生化处理后的焦化废水进行深度处理。在三维电极参数一定的条件下,考察了影nfi]TOC去除率的影响因素,探讨了该反应体系的降解动力学及降解机理。正交试验结果表明,反应体系中各参数的最佳值分别为p（H202投加量）=300mg·L-1,pH3．4,反应时间为90min,c（FeS04-7H20投加量）为3．5mmol·L-1,TOC去除率可达到61．7％。焦化废水的降解反应表现为一级动力学。紫外吸收光谱分析结果,废水中有机物彻底发生了降解矿化,这为三维电极组合Fenton试剂工艺在焦化废水深度处理中的工程应用提供了一定的理论指导。     

Kinetics of microwave-enhanced oxidation of phenol by hydrogen peroxide

Aqueous solutions of phenol were oxidized by hydrogen peroxide assisted by microwave (MW) irradiation. A simple kinetic model for the overall degradation of phenol in the presence of excess H₂O₂ is proposed in which the degradation rate of phenol is expressed as a linear function of the concentrations of phenol and H₂O₂. A detailed parametric study showed that the degradation rate of phenol increased with increasing [H₂O₂] until saturation was observed. Phenol degradation followed apparent zero-order kinetics under MW radiation or H₂O₂ oxidation. However, after 90 min of irradiation, the observed kinetics shifted to pseudo first order. The overall reaction rates were significantly enhanced in the combined MW/H₂O₂ system, mainly because microwave could accelerate H₂O₂ to generate hydroxyl radical (^·OH) and other reactive oxygen intermediates. The observed synergetic effects of the MW/H₂O₂ process resulted in an increased in the net reaction rate by a factor of 5.75. When hydrogen peroxide is present in a large stoichiometric excess, the time required to achieve complete mineralization is reduced significantly.