基于不同废污泥源的短程反硝化快速启动及稳定性

为探究不同废污泥源快速启动短程反硝化和实现稳定NO_2~--N积累的可行性,在3个完全相同的SBR反应器(S1、S2和S3)分别接种:实验室城市污水反硝化除磷系统排泥、城市污水厂剩余污泥及河涌底泥,比较其短程反硝化启动快慢和NO_2~--N积累特性,考察系统短程反硝化活性和NO_3~--N→NO_2~--N转化性能,并从微生物学角度分析反应器功能菌群特征.结果表明,在乙酸钠为唯一碳源、高碱度和适宜COD/NO_3~--N比进水条件下,3个SBR短程反硝化反应器在短时间内均能够成功启动,系统平均NO_3~--N→NO_2~--N转化率为S1 S2 S3(75. 92% 73. 36% 69. 90%).同时发现持续低温条件下S1和S2呈现不同程度的短程反硝化性能恶化趋势,但S3能够稳定维持良好NO_2~--N积累性能.微生物高通量测序表明,变形菌门和拟杆菌门居PD系统主导地位,3个短程反硝化反应器NO_2~--N积累关键功能菌属Thauera属丰度差异明显:S3 S1 S2(25. 09% 4. 71% 3. 60%),表明S3具备稳定高效的NO_2~--N积累性能,同时高丰度Thauera属可能是维持低温短程反硝化活性的重要原因.     

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.     

亚氧化钛膜电极电化学特性及其处理印染工业废水的效能研究

电化学氧化法具有稳定高效、操作灵活、集成度高等特点,在处理难降解有机废水领域具有独特优势.电化学废水处理过程通常受限于传质速率,而膜电极有望解决这一瓶颈问题.亚氧化钛膜电极（TiSO-ME）的化学结构与电化学性质结果显示,经过高温还原法制备的TiSO-ME电极主要由Ti₄O₇和少量Ti₅O₉组成,大孔体积占总孔体积的92.7%,平均孔径为0.508 μm.电化学测试结果表明,TiSO-ME具有良好的导电性、高析氧电位和电化学稳定性.过滤试验结果表明,在0.82×10^-3~3.14×10^-3 mL·cm^-2·s^-1范围内膜通量与传质系数成正比.在电流密度为8 mA·cm^-2,膜通量为2.31×10^-3 mL·cm^-2·s^-1的条件下,电解1.5 h即可有效处理实际印染工业废水,sCOD去除率高达96.07%,电流效率可达24.22%,电能消耗较不存在膜通量时降低了32.99%.TiSO-ME能够实现废水在膜孔结构内部的穿流式操作,有效克服旁流式操作传质受限的问题,在小规模分散式工业废水处理中有着重要的研究价值和发展潜力.     

电场与MnxCey催化剂在苯氧化反应中的协同效应及机理探究

挥发性有机物（VOCs）大量排放已成为日益严重的环境问题,为了实现VOCs的高效去除,本文采用自蔓延燃烧合成法制备了一系列锰铈复合氧化物催化剂,将稳恒直流电场引入典型VOCs气体苯的催化氧化过程,并基于不同电场条件下催化剂的理化性质表征结果进行机理分析.实验结果表明,Mn_xCe_y催化剂对含苯废气的去除有良好的效果,稳恒直流电场显著促进了催化剂的活性,其中Mn₁Ce₃的催化性能最佳,电流为5 mA时,Mn₁Ce₃催化剂在155℃可达到50%的苯转化率,在202.4℃可达到90%的苯转化率,对应的转化温度T₅₀和T₉₀比传统方法分别降低了62.4℃和48.3℃,且电场中的反应活化能由52.32 kJ·mol^-1降低至32.31 kJ·mol^-1.根据实验现象及表征结果,发现协同效应与活性位点的快速持续再生及活性氧物种的转化有关,由此提出苯在Mn_xCe_y催化剂上的氧化机理及电场协同催化的反应模型.     

金属改性对SAPO-34低温还原NO性能的影响

采用浸渍法制备金属改性SAPO-34分子筛催化剂,分析比较了不同单金属（Cu或Co）及不同比例双金属（Cu：Co=1：1、3：1、5：1,质量比）改性催化剂对NO的催化还原性能,评价了不同催化剂的N₂选择性,并采用扫描电子显微镜（SEM）、比表面积测试、X射线衍射分析（XRD）、NH₃-程序升温脱附（NH₃-TPD）等表征手段对催化剂的物化性能进行了分析.结果表明,单金属Cu改性催化剂具有较宽的温度区间,在250~450℃范围内NO的转化率始终保持在100%;双金属改性使NO转化率保持为100%的最低温度下降了25~50℃,显著拓宽了低温段窗口,其中,Cu₃Co₁/SAPO-34催化剂的低温催化还原性能最好,200℃即可实现100%的NO转化率,175℃下的转化率也高达80%以上.Cu-Co双金属改性SAPO-34分子筛催化剂具有优异的低温催化还原NO性能,具有在机动车尾气、工业废气的低温脱硝治理领域应用的潜力.     

稻田NO3-还原耦合As(III)氧化过程及微生物群落特征

以华南稻田土壤为研究对象通过构建微宇宙体系,研究了淹水稻田自养硝酸盐还原耦合As（III）氧化过程及其微生物群落结构组成.结果表明,NO₃^-的添加促进了稻田土壤中As（III）的氧化,在未添加NO₃^-的处理（Soil+As（III））以及灭菌处理（Sterilized soil+As（III）+NO₃^-）中As（III）未发生明显的氧化;在Soil+As（III）+NO₃^-处理中,NO₃^-有少量被还原,而在Soil+NO₃^-处理中,NO₃^-没有被还原.通过16S rRNA高通量分析在NO₃^-还原耦合As（III）氧化体系中微生物群落结构特征,在Soil+As（III）+NO₃^-处理中shannon指数相对较低为8.19,土壤微生物群落多样性降低,其中在门水平上主要优势菌群为变形菌门Proteobacteria（33%）、绿弯菌门Chloroflexi（11%）、浮霉菌门Planctomycetes（12%）;在属水平上主要的优势菌属为Gemmatimonas（7.4%）以及少量的Singulisphaera、Thermomonas、Bacillus.NO₃^-的添加能够促进稻田土壤中自养As（III）氧化,并且影响着稻田土壤中微生物群落组成.     

Treatability studies of naphthalene in soil,water and air with persulfate activated by iron(Ⅱ)

Chemical oxidation was applied to an artificially contaminated soil with naphthalene (NAP). Evaluation of NAP distribution and mass reduction in soil, water and air phases was carried out through mass balance. Evaluation of NAP distribution and mass reduction in soil, water and air phases was carried out through mass balance. The importance of the air phase analysis was emphasized by demonstrating how NAP behaves in a sealed system over a 4 hr reaction period. Design of Experiments method was applied to the following variables: sodium persulfate concentration [SP], ferrous sulfate concentration [FeSO₄], and pH. The system operated with a prefixed solid to liquid ratio of 1:2. The following conditions resulted in optimum NAP removal [SP] = 18.37 g/L, [FeSO₄] = 4.25 g/L and pH = 3.00. At the end of the 4 hr reaction, 62% of NAP was degraded. In the soil phase, the chemical oxidation reduced the NAP concentration thus achieving levels which comply with Brazilian and USA environmental legislations. Besides the NAP partitioning view, the monitoring of each phase allowed the variabilities assessment over the process, refining the knowledge of mass reduction. Based on NAP distribution in the system, this study demonstrates the importance of evaluating the presence of semi-volatile and volatile organic compounds in the air phase during remediation, so that there is greater control of the system as to the distribution and presence of the contaminant in the environment. The results highlight the importance of treating the contaminant in all its phases at the contaminated site.     

Effects of SO2 and H2O on low-temperature NO conversion over F-V2O5-WO3/TiO2 catalysts

F-V_2 O_5-WO3/Ti02 catalysts were prepared by the impregnation method.As the content of F ions increased from 0.00 to 0.35 wt.%,the NO conversion of F-V_2 O_5-WO_3/TiO_2 catalysts initially increased and then decreased.The 0.2 F-V_2 O_5-WO_3/TiO_2 catalyst(0.2 wt.% F ion)exhibited the best denitration(De-NOx) performance,with more than 95% NO conversion in the temperature range 160-360℃,and 99.0% N2 selectivity between 110 and 280℃.The addition of an appropriate amount of F ions eroded the surface morphology of the catalyst and reduced its grain size,thus enhancing the NO conversion at low temperature as well as the sulfur and water resistance of the V_2 O_5-WO3/Ti02 catalyst.After selective catalytic reduction(SCR) reaction in a gas flow containing SO_2 and H_2 O,the number of NH3 adsorption sites,active component content,specific surface area and pore volume decreased to different degrees.Ammonium sulfate species deposited on the catalyst surface,which blocked part of the active sites and reduced the NO conversion performance of the catalyst.On-line thermal regeneration could not completely recover the catalyst activity,although it prolonged the cumulative life of the catalyst.In addition,a mechanism for the effects of S02 and H_2 O on catalyst NO conversion was proposed.     

Density functional theory (DFT) studies of vanadium-titanium based selective catalytic reduction (SCR) catalysts

Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH₃ and NO react to produce N₂ and H₂O follows an Eley-Rideal type mechanism. NH₂NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H₂O, SO₂ and metal on SCR catalysts were also summarized.     

Effect of NOx and SO2 on the photooxidation of methylglyoxal: Implications in secondary aerosol formation

Methylglyoxal(CH_3COCHO,MG),which is one of the most abundant α-dicarbonyl compounds in the atmosphere,has been reported as a major source of secondary organic aerosol(SOA).In this work,the reaction of MG with hydroxyl radicals was studied in a 500 L smog chamber at(293±3) K,atmospheric pressure,(18±2)% relative humidity,and under different NOx and SO_2.Particle size distribution was measured by using a scanning mobility particle sizer(SMPS) and the results showed that the addition of SO_2 can promote SOA formation,while different NOx concentrations have different influences on SOA production.High NOx suppressed the SOA formation,whereas the particle mass concentration,particle number concentration and particle geometric mean diameter increased with the increasing NOx concentration at low NOx concentration in the presence of SO_2.In addition,the products of the OH-initiated oxidation of MG and the functional groups of the particle phase in the MG/OH/SO_2 and MG/OH/NOx/SO_2 reaction systems were detected by gas chromatography mass spectrometry(GC-MS) and attenuated total reflection fourier transformed infrared spectroscopy(ATR-FTIR) analysis.Two products,glyoxylic acid and oxalic acid,were detected by GC-MS.The mechanism of the reaction of MG and OH radicals that follows two main pathways,H atom abstraction and hydration,is proposed.Evidence is provided for the formation of organic nitrates and organic sulfate in particle phase from IR spectra.Incorporation of NOx and SO_2 influence suggested that SOA formation from anthropogenic hydrocarbons may be more efficient in polluted environment.