MnO2/Al2O3催化剂-微气泡臭氧体系催化降解喹啉及其机理

制备了纳米MnO₂,并以Al₂O₃为载体制备了掺杂型MnO₂/Al₂O₃颗粒催化剂.催化剂焙烧温度和时间分别为500℃和4 h、MnO₂质量分数为8%时,催化剂具有最高的臭氧催化氧化活性.SEM分析表明,纳米MnO₂均匀分布于Al₂O₃载体表面.MnO₂/Al₂O₃催化剂的比表面积（BET）为183.22 m²·g^-1,平均孔容为0.27 cm³·g^-1,平均孔径为4.87 nm.建立了MnO₂/Al₂O₃催化剂-微气泡臭氧催化反应体系,研究了该体系对喹啉的降解去除效果及其机理.臭氧微气泡的平均粒径为61.7 μm.微气泡臭氧投量为30 mg·L^-1时,反应60 min后喹啉去除率能达到95%以上;反应20 min后,MnO₂/Al₂O₃催化剂-微气泡臭氧体系对实际煤化工废水二级出水的TOC去除率可达到55%以上.以叔丁醇作为分子探针,证明了羟基自由基（·OH）氧化作用在臭氧微气泡催化氧化体系中对喹啉的降解起到主导作用.     

2-丁烯醛生产废水的臭氧脱毒预处理

CMW（crotonaldehyde manufacturing wastewater,2-丁烯醛生产废水）污染物浓度高、毒性强、直接采用生物法处理难度大.为了降低CMW的生物处理毒性,采用臭氧氧化法对CMW进行脱毒预处理,并通过考察不同臭氧氧化条件对废水COD_Cr、TOC（总有机碳）、UV_{254 nm}去除率及SMA（specific methanogenic activity,比产甲烷活性）抑制率的影响,获得了优化的臭氧氧化条件,进一步分析了废水脱毒机理.结果表明:①优化的臭氧氧化条件为接触反应时间180 min、初始pH 3.0、反应温度35℃、气相臭氧浓度30.3 mg/L,进气流量500 mL/min;并且在该条件下,CMW中COD_Cr、TOC和UV_{254 nm}的去除率分别为19.9%、9.9%和70.6%,主要特征有机污染物[包括2-丁烯醛、（E,E）-2,4-己二烯醛、3-（2-甲基-2-丙烯）-5-戊内酯、1,5-二甲基-1-烯-4-羰基-环氧己烷、山梨酸乙酯等]的去除率在74.4%以上.②厌氧产甲烷毒性试验结果显示,CMW的SMA抑制率由臭氧氧化前的82.0%降至臭氧氧化后的47.2%.③反应动力学研究显示,CMW中COD_Cr、TOC及UV_{254 nm}的去除过程均符合一级反应动力学方程,R2分别为0.82、0.97、0.94.研究显示,臭氧氧化预处理可以较好地去除CMW中的特征有机污染物,降低废水的厌氧生物处理毒性,是一种可行的脱毒预处理方法.      

MgO低温催化臭氧降解氨氮的机制研究

研究了低温条件下单独臭氧及MgO催化臭氧化降解水中氨氮的效率和特征,并对其反应机制分别进行了探讨.结果表明,pH是影响臭氧和催化臭氧化除氨的重要因素,不仅影响溶液中NH_3与NH~+_4的比例和臭氧氧化氨氮的速率,还影响氧化产物种类,从而影响脱氮效果.10℃时,单独臭氧对水中氨氮的氧化降解效率随pH的升高而增大,pH≤9时整体降解效率不高,pH=9时仅为16.39%,而pH=10时达到41.77%.臭氧和·OH共同参与降解氨氮的过程.单独臭氧氧化氨氮生成氮气的选择性具有pH依赖性,并与Cl~-密切相关.pH低(≤9)时,氨氮多以NH~+_4形态存在,O_3与Cl~-反应生成ClO~-_x(x=1、3),再氧化NH~+_4,从而生成气态产物N_2或N_2O.MgO在低温条件下具有很强的催化臭氧化降解氨氮的能力且温度升高有利于反应的进行,0、10、20℃时,MgO催化臭氧化氨氮的效率分别为77.53%、80.17%、91.26%.此过程中,·OH参与反应的程度低,一部分氨氮降解依靠ClO~-_x氧化NH~+_4,而氨氮降解的主要途径为O_3对NH_3的直接氧化.     

Synergistic effect of F and triggered oxygen vacancies over F-TiO2 on enhancing NO ozonation

Oxidation-absorption technology is a key step for NO_x removal from low-temperature gas. Under the condition of low O₃ concentration (O₃/NO molar ratio = 0.6), F-TiO₂ (F-TiO₂), which is cheap and environmentally friendly, has been prepared as ozonation catalysts for NO oxidation. Catalytic activity tests performed at 120°C showed that the NO oxidation efficiency of F-TiO₂ samples was higher than that of TiO₂ (about 43.7%), and the NO oxidation efficiency of F-TiO₂-0.15 was the highest, which was 65.3%. Combined with physicochemical characteristics of catalysts and the analysis of active species, it was found that there was a synergistic effect between F sites and oxygen vacancies on F-TiO₂, which could accelerate the transformation of monomolecular O₃ into multi-molecule singlet oxygen (¹O₂), thus promoting the selective oxidation of NO to NO₂. The oxidation reaction of NO on F-TiO₂-0.15 follows the Eley-Rideal mechanism, that is, gaseous NO reacts with adsorbed O₃ and finally form NO₂.     

不同pH条件下Fe~(2+)/Fe~(3+)/Ni~(2+)/O_3体系对活性艳蓝X-BR的催化氧化

臭氧和催化臭氧氧化法是对印染废水有效的处理手段之一。选取用途较广的活性艳蓝X-BR为研究对象,探讨了氧化过程中染料的降解和结构变化情况。并选取了Fe2+、Fe3+和Ni2+为均相催化剂,讨论了pH对催化效果的影响。实验表明,均相催化体系中,酸性条件下更有利。     

Degradation of nitrobenzene in aqueous solution by ozone-ceramic honeycomb

IntroductionAs a promising advanced oxidation technology for watertreatment ,catalytic ozonation has received great attentionforthe efficient degradation of organic compoundsinrecent years(Legube , 1999) . Some studies showed that homogeneousand heterogen…     

人工神经元网络对水处理系统建模适应性的研究

针对水处理系统的特点和研究中的难点，引入人工神经元网络的理论和思想，提出了水处理系统的神经网络分析方法．通过建立基于ＢＰ人工神经元网络的臭氧生物活性炭系统的模型，具体地考察了人工神经元网络对水处理系统建模的适应性，使水处理系统的研究迈向智能化和控制化．     

微气泡臭氧催化氧化-生化耦合工艺深度处理煤化工废水

采用微气泡臭氧催化氧化-生化耦合工艺对煤化工废水生化出水进行深度处理,考察耦合系统处理性能及不同臭氧投加量和进水COD量比值的影响.结果表明,微气泡臭氧催化氧化处理能够有效降解废水中难降解含氮芳香族污染物,去除部分COD并释放氨氮,显著提高废水可生化性,臭氧利用率接近100%,无需进行臭氧尾气处理;同时为生化处理提供充足溶解氧(DO),实现生化处理对COD和氨氮的进一步有效去除,生化处理无需曝气.在系统出水回流比为30%、臭氧投加量和进水COD量之比为0.44 mg·mg~(-1)的运行条件下,耦合系统处理性能较好.微气泡臭氧催化氧化处理对COD去除率为42.5%,臭氧消耗量与COD去除量比值为1.38 mg·mg~(-1),臭氧利用率为98.0%;生化处理对COD去除率为42.3%;耦合系统整体COD去除率为66.7%,最终平均出水COD浓度为91.5 mg·L~(-1),估算整体臭氧消耗量与COD去除量比值为0.68 mg·mg~(-1),具有较优的技术经济性能.     

响应面法优化赤泥负载Co催化剂制备及活性评价

以催化臭氧氧化去除水中苯扎贝特(bezafibrate,BZF)的处理效果为评价指标,采用Plackett-Burman和响应面(Response Surface Methodology,RSM)法对Co/RM催化剂的制备条件进行优化.结果表明,浸渍质量分数和焙烧温度为催化剂制备的主要影响因素,当浸渍质量分数为4.14%、煅烧温度为389℃时BZF去除率预测值最高(71.29%).采用上述最佳制备条件制备的Co/RM催化臭氧氧化去除苯扎贝特的去除率为70.74%,与模型预测值十分接近,偏差为1%(<5%),说明响应面法实验设计和数学模型具有较好可靠性.通过比较RM和Co/RM两种催化剂对BZF的催化臭氧氧化去除效果,发现Co/RM催化臭氧氧化去除BZF的效果较为显著.采用BET、XRD和UV-Vis等表征手段对两种催化剂的表面结构和组成进行分析,结果表明两种催化剂的比表面积、总孔体积存在相同的变化规律(RM相似文献   

Homogeneous and heterogeneous reactions of anthracene with selected atmospheric oxidants

The reactions of gas-phase anthracene and suspended anthracene particles with O3 and O3-NO were conducted in a 200-L reaction chamber, respectively. The secondary organic aerosol (SOA) formations from gas-phase reactions of anthracene with O3 and O3-NO were observed. Meanwhile, the size distributions and mass concentrations of SOA were monitored with a scanning mobility particle sizer (SMPS) during the formation processes. The rapid exponential growths of SOA reveal that the atmospheric lifetimes of gas-phase anthracene towards O3 and O3-NO are less than 20.5 and 4.34 hr, respectively. The particulate oxidation products from homogeneous and heterogeneous reactions were analyzed with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). Gas chromatograph/mass spectrometer (GC/MS) analyses of oxidation products of anthracene were carried out for assigning the time-of-flight (TOF) mass spectra of products from homogeneous and heterogeneous reactions. Anthrone, anthraquinone, 9,10- dihydroxyanthracene, and 1,9,10-trihydroxyanthracene were the ozonation products of anthracene, while anthrone, anthraquinone, 9-nitroanthracene, and 1,8-dihydroxyanthraquinone were the main products of anthracene with O3-NO.