芬顿氧化技术在废水处理中的进展研究

随着中国水环境形势的日益严峻以及造纸、印染、制药等行业废水排放标准的提高,传统的废水深度处理工艺已经很难满足污染物去除的要求。在查阅大量国内外最新相关技术文献的基础上,介绍了芬顿氧化技术降解废水中污染物的机理,对比了芬顿氧化试剂的浓度、投加量以及反映时间等因素对COD、色度、总磷等水质指标去除率的影响因素,综述了芬顿氧化法在处理焦化废水、印染废水、农药废水、制药废水、造纸废水等难降解工业废水中的应用研究进展。     

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.     

零价铁-过二硫酸盐连续运行体系去除水中硝基苯

水中硝基苯(NB)的高毒性对人体健康具有极大的危害,因此,本文建立了零价铁-过二硫酸盐(Fe0-PS)连续运行体系以降解水中NB.研究结果表明,单独Fe0柱可还原降解NB,Fe0对不同浓度NB的还原效果均较好,随着流速的减慢及初始pH的降低,NB还原效果变好;但还原体系中总有机碳(TOC)基本没有去除,只是生成了中间产物苯胺(AN).Fe0-PS联合体系中,随着PS的投加,产生的Fe2+活化PS,发生了类Fenton反应,从而使还原产物AN得以氧化降解,TOC去除率可达54.8%;随着Fe0填充量的增加,氧化产物Fe2+随之增加,还原产物AN随之减少.可见,Fe0-PS连续运行体系,以Fe2+为媒介巧妙结合还原与氧化作用,能有效去除NB.     

臭氧氧化水溶液中对乙酰氨基酚的机制研究

采用间歇实验的方法,研究了臭氧氧化降解水溶液中对乙酰氨基酚的影响因素和机制.结果表明,臭氧能够有效降解水溶液中的对乙酰氨基酚,降解过程符合伪一级动力学模型(R2>0.992).臭氧浓度、HCO-3和pH值均影响对乙酰氨基酚的降解过程,添加HCO-3、提高pH值和适当增大臭氧浓度均可提高其降解效果.气相色谱/质谱和离子色谱检测结果表明,在对乙酰氨基酚臭氧氧化的过程中,首先生成对苯酚及一系列含有羧基的酸类产物,继而被进一步氧化;依据中间产物,探讨了对乙酰氨基酚可能的降解反应途径.TOC检测仪的检测结果显示,对乙酰氨基酚的最终矿化程度较低.在对乙酰氨基酚的初始浓度为20 mg·L-1及臭氧浓度为9.10 mg·L-1时,反应130 min后,矿化程度仅为16.42%.     

Pseudomonas sp. QJX-1的锰氧化特性研究

从锰矿土壤样品中分离、纯化出1株高效锰氧化细菌(QJX-1),经16S rDNA序列鉴定为Pseudomonas sp.QJX-1.研究表明,Pseudomonas sp.QJX-1含有锰氧化的必需成分多铜氧化酶基因CumA,当初始Mn2+为5.05 mg·L-1,菌密度D600为0.020时,该菌可在48 h内将Mn2+转化,且转化率高达99.4%.在寡营养条件下该菌锰氧化速率较富营养条件下有显著提高;添加石英砂滤料促使生物膜的快速形成,进而促进Mn2+的生物转化.根据研究结果推测地下水处理过程中生物锰氧化速率较快.     

Ti/SnO2-Sb2O5/PbO2电极的制备及降解不同污染物性能研究

采用溶胶凝胶法和电沉积法分别制备了Ti/SnO2-Sb2O5/PbO2电极的中间层和表面活性层,并通过XRD和SEM对电极的中间层和表面活性层进行了相关表征.结果表明,制得的电极表面为β型PbO2,表面形貌均匀致密.同时,采用线性伏安扫描和交流阻抗测试对电极的电化学性能进行了测试.结果表明,电解液中污染物的存在可提高电极的析氧电位,中间层的制备可以有效提高电极的催化性能.另外,通过测定电极对苯酚、靛蓝胭脂红、甲基橙3种不同类型污染物的去除率、COD去除率,研究了该电极对不同类型有机物的降解规律.结果表明,在相同条件下该电极对靛蓝胭脂红的去除速率较高且所需电压最低,降解1 h时靛蓝胭脂红去除率即达100%,甲基橙降解3 h时其COD去除率高达55%.     

不同氧化锰矿物与砷的交互作用

利用从土壤铁锰结核中分离筛选得到的1株锰氧化细菌(芽孢杆菌,Bacillus sp.)GY16合成生物氧化锰,与化学合成的水钠锰矿进行比较,研究了不同氧化锰对As的氧化吸附特征.结果表明,生物氧化锰和化学氧化锰对As(Ⅲ)均有强烈的氧化作用,化学氧化锰对As(Ⅲ)的氧化速率要高于生物氧化锰,而单位物质的量的生物氧化锰对As(Ⅲ)的氧化量可达化学氧化锰的5倍,并且对As(Ⅴ)有非常明显的吸附作用,而化学氧化锰对As(Ⅴ)的吸附量则非常少.此外,随着生物氧化锰与As(Ⅲ)/As(Ⅴ)反应的进行,生物氧化锰对As(Ⅲ)/As(Ⅴ)的氧化吸附速率均逐渐降低.随着pH的增加,生物氧化锰对As(Ⅲ)的氧化量及As(Ⅴ)的吸附量均呈现出明显的下降趋势,但是化学氧化锰对As(Ⅴ)的吸附量却有微弱的增加.研究结果可为生物氧化锰应用于环境修复提供可靠的技术支撑.     

碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝

在课题组前期研究的基础上,以碳纳米管(MWCNTs)为载体制备了Fe3O4/MWCNTs复合物并作为催化剂,以染料亚甲基蓝(MB)为降解对象,研究了该催化剂催化H2O2对亚甲基蓝溶液的降解特性及其影响因素,并考察了催化剂的重复使用效果,探讨了催化反应的机理.结果表明,在pH值3~8的范围内,催化反应体系都能有效降解MB,最佳pH值为3.5.随着催化剂投量的增加,MB的降解率明显提高,500 mg·L-1催化剂投量条件下,MB的降解率最高.随着H2O2初始浓度的增加,MB的降解率增加,10 mmol·L-1时MB的降解率最高.溶液中共存的阴离子会降低MB的降解率.在最佳条件,即温度25℃、H2O2浓度10 mmol·L-1、催化剂浓度500 mg·L-1的条件下,0.20 mmol·L-1MB在30 min内的降解率达到99.1%.催化剂重复使用后仍然具有较好的催化活性,说明Fe3O4在MWCNTs表面负载比较牢固,催化剂具有反复使用的能力.催化反应机理是催化剂催化H2O2产生羟基自由基,高活性的羟基自由基氧化MB.     

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%.     

Wintertime peroxyacetyl nitrate (PAN) in the megacity Beijing: Role of photochemical and meteorological processes

Previous measurements of peroxyacetyl nitrate(PAN) in Asian megacities were scarce and mainly conducted for relative short periods in summer. Here, we present and analyze the measurements of PAN, O3, NOx, etc., made at an urban site(CMA) in Beijing from 25 January to 22 March 2010. The hourly concentration of PAN averaged 0.70 × 10 9mol/mol(0.23 × 10 9–3.51 × 10 9mol/mol) and was well correlated with that of NO2but not O3, indicating that the variations of the winter concentrations of PAN and O3in urban Beijing are decoupled with each other. Wind conditions and transport of air masses exert very significant impacts on O3, PAN, and other species. Air masses arriving at the site originated either from the boundary layer over the highly polluted N-S-W sector or from the free troposphere over the W-N sector. The descending free-tropospheric air was rich in O3, with an average PAN/O3ratio smaller than 0.031, while the boundary layer air over the polluted sector contained higher levels of PAN and primary pollutants, with an average PAN/O3ratio of 0.11. These facts related with transport conditions can well explain the observed PAN-O3decoupling. Photochemical production is important to PAN in the winter over Beijing. The concentration of the peroxyacetyl(PA) radical was estimated to be in the range of 0.0014 × 10 12–0.0042 × 10 12 mol/mol. The contributions of the formation reaction and thermal decomposition to PAN's variation were calculated and found to be significant even in the colder period in air over Beijing, with the production exceeding the decomposition.