尿素废水生物处理技术原理与工艺研究进展

尿素废水的处理是当前亟需解决的难题,其中生物处理法因具有工艺流程短,成本低,抗冲击负荷,不产生二次污染等优点,在尿素废水的处理中备受青睐.本文基于尿素生物水解法原理,从机理上深入分析了脲酶的发展历程,酶学结构与水解机制,并对传统生物尿素脱氮法的应用进行了系统梳理.此外,为了更好地理解厌氧氨氧化菌降解尿素的潜能及在实际工程中的应用,本文分别从微生物学和工程应用的角度总结了相关研究结果.最后提出了尿素废水生物处理研究的建议与展望,以期为实际工程应用提供有力的理论基础和技术支持.     

N. europaea/Nc. mobilis谱系在垃圾渗滤液处理中的脱氨贡献

为了解垃圾渗滤液处理系统中菌群结构与脱氨效果的关系,采用16S rRNA基因高通量测序技术分析了15个实际垃圾渗滤液处理系统中的自养氨氧化细菌（AOB）的群落结构,监测了其中1个处理系统中的AOB群落结构的周年变化,并采集实际垃圾渗滤液开展了为期45d的模拟试验.结果表明,Nitrosomonas属是垃圾渗滤液处理系统中的优势自养氨氧化细菌,其相对丰度与脱氨活性呈显著正相关（P<0.05）.在此菌属中,N.europaea、N.eutropha和N.halophila的相对丰度与脱氨活性显著正相关（P<0.05）,这3种菌在系统发育上同属于N.europaea/Nitrosococcus mobilis谱系,说明该谱系是实际垃圾渗沥液处理系统中的优势AOB类群,并对垃圾渗滤液脱氨有重要贡献.     

钒基催化剂同步去除燃煤烟气中甲苯与NOx研究

采用不同工艺制备V₂O₅-WO₃-MoO_x/TiO₂堇青石整体式催化剂,以甲苯和NO为探针分子,考察了Mo的负载量、涂覆方法、粘结剂的种类等制备工艺对整体式催化剂性能的影响,用XRD、SEM-EDS、FT-IR、BET等技术对催化剂进行了表征分析.结果表明,采用涂敷法,以添加量为1%的甲基纤维素为粘结剂所制备的V1W6Mo3/TiO₂堇青石蜂窝陶瓷整体式催化剂具有最优活性和稳定性（T₉₀为307℃,负载率为28.26%,脱落率为6.81%）,在燃煤烟气中具有优异的同步去除VOCs与NO性能,甲苯去除率可达99%,NO去除率为100%,N₂选择性为99%.XRD、SEM-EDS表明V、W、Mo活性组分分布均匀且高度分散.FT-IR证明添加甲基纤维素的整体式催化剂具有优异的抗硫性能.     

催化氧化除锰活性滤料去除地下水中双酚A性能

以催化氧化除锰活性滤料（简称“活性滤料”）为研究对象,考察了地下水中锰污染对于活性滤料去除双酚A效能的影响.结果表明,进水中含有高浓度锰（5mg/L）时,会显著降低活性滤料对于双酚A的去除能力;同时,双酚A也会降低活性滤料对锰的去处能力.双酚A脱附实验结果表明,脱附的双酚A量不足双酚A去除总量的10%,且双酚A去除过程中初期总有机碳（TOC）去除率保持在12%~25%,之后持续保持在0.1%~4%,表明活性滤料去除双酚A存在吸附过程,但是以氧化去除为主.扫描电子显微镜（SEM）和X射线衍射（XRD）分析结果表明,双酚A的去除会导致滤料表面微观形态改变以及新物相的生成;傅里叶变换红外光谱（FTIR）结果表明双酚A的去除会消耗滤料表面羟基基团,且表面残留络合物.本文研究分析提出活性滤料去除双酚A的主要步骤包括双酚A首先吸附到活性滤料表面形成络合物、活性滤料与表面络合物发生氧化反应,部分反应物中间体脱附3个过程.     

Efficient degradation of Rhodamine B by magnetically recoverable Fe3O4-modified ternary CoFeCu-layered double hydroxides via activating peroxymonosulfate

Environment-friendly nano-catalysts capable of activating peroxymonosulfate (PMS) have received increasing attention recently. Nevertheless, traditional nano-catalysts are generally well dispersed and difficult to be separated from reaction system, so it is particularly important to develop nano-catalysts with both good catalytic activity and excellent recycling efficiency. In this work, magnetically recoverable Fe₃O₄-modified ternary CoFeCu-layered double hydroxides (Fe₃O₄/CoFeCu-LDHs) was prepared by a simple co-precipitation method and initially applied to activate PMS for the degradation of Rhodamine B (RhB). X-ray diffraction (XRD), fourier transform infrared spectrometer (FT-IR), scanning electron microscope (SEM), transmission electron microscopy (TEM), Brunauer-Emmett-Teller method (BET), and vibrating sample magnetometer (VSM) were applied to characterize morphology, structure, specific surface area and magnetism. In addition, the effects of several key parameters were evaluated. The Fe₃O₄/CoFeCu-LDHs exhibited high catalytic activity, and RhB degradation efficiency could reach 100% within 20 min by adding 0.2 g/L of catalyst and 1 mmol/L of PMS into 50 mg/L of RhB solution under a wide pH condition (3.0-7.0). Notably, the Fe₃O₄/CoFeCu-LDHs showed good super-paramagnetism and excellent stability, which could be effectively and quickly recovered under magnetic condition, and the degradation efficiency after ten cycles could still maintain 98.95%. Both radicals quenching tests and electron spin resonance (ESR) identified both HO? and SO₄^?? were involved and SO₄^?? played a dominant role on the RhB degradation. Finally, the chemical states of the sample's surface elements were measured by X-ray photoelectron spectroscopy (XPS), and the possible activation mechanism in Fe₃O₄/CoFeCu-LDHs/PMS system was proposed according to comprehensive analysis.     

Comparing dark- and photo-Fenton-like degradation of emerging pollutant over photo-switchable Bi2WO6/CuFe2O4: Investigation on dominant reactive oxidation species

The extensive use of tetracycline hydrochloride (TCH) poses a threat to human health and the aquatic environment. Here, magnetic p-n Bi₂WO₆/CuFe₂O₄ catalyst was fabricated to efficiently remove TCH. The obtained Bi₂WO₆/CuFe₂O₄ exhibited 92.1% TCH degradation efficiency and 50.7% and 35.1% mineralization performance for TCH and raw secondary effluent from a wastewater treatment plant in a photo-Fenton-like system, respectively. The remarkable performance was attributed to the fact that photogenerated electrons accelerated the Fe(III)/Fe(II) and Cu(II)/Cu(I) conversion for the Fenton-like reaction between Fe(II)/Cu(I) and H₂O₂, thereby generating abundant ?OH for pollutant oxidation. Various environmental factors including H₂O₂ concentration, initial pH, catalyst dosage, TCH concentration and inorganic ions were explored. The reactive oxidation species (ROS) quenching results and electron spin resonance (ESR) spectra confirmed that ?O₂^? and ?OH were responsible for the dark and photo-Fenton-like systems, respectively. The degradation mechanisms and pathways of TCH were proposed, and the toxicity of products was evaluated. This work contributes a highly efficient and environmentally friendly catalyst and provides a clear mechanistic explanation for the removal of antibiotic pollutants in environmental remediation.     

Comprehensive and high-resolution emission inventory of atmospheric pollutants for the northernmost cities agglomeration of Harbin-Changchun, China: Implications for local atmospheric environment management

Using a bottom-up estimation method, a comprehensive, high-resolution emission inventory of gaseous and particulate atmospheric pollutants for multiple anthropogenic sectors with typical local sources has been developed for the Harbin-Changchun city agglomeration (HCA). The annual emissions for CO, NOx, SO₂, NH₃, VOC_S, PM_2.5, PM₁₀, BC and OC during 2017 in the HCA were estimated to be 5.82 Tg, 0.70 Tg, 0.34 Tg, 0.75 Tg, 0.81Tg, 0.67 Tg, 1.59 Tg, 0.12 Tg and 0.26 Tg, respectively. For PM₁₀ and SO₂, the emissions from industry processes were the dominant contributors representing 54.7% and 49.5%, respectively, of the total emissions, while 95.3% and 44.5% of the total NH₃ and NOx emissions, respectively, were from or associated with agricultural activities and transportation. Spatiotemporal distributions showed that most emissions (except NH₃) occurred in November to March and were concentrated in the central cities of Changchun and Harbin and the surrounding cities. Open burning of straw made an important contribution to PM_2.5 in the central regions of the northeastern plain during autumn and spring, while domestic coal combustion for heating purposes was significant with respect to SO₂ and PM_2.5 emissions during autumn and winter. Furthermore, based on Principal Component Analysis and Multivariable Linear Regression model, air temperature, relative humidity, electricity and energy consumption, and the urban and rural population were optimized to be representative indicators for rapidly assessing the magnitude of regional atmospheric pollutants in the HCA. Such indicators and equations were demonstrated to be useful for local atmospheric environment management.     

Marine aquaculture regulates dissimilatory nitrate reduction processes in a typical semi-enclosed bay of southeastern China

Marine aquaculture in semi-enclosed bays can significantly influence nutrient cycling in coastal ecosystems. However, the impact of marine aquaculture on the dynamics of dissimilatory nitrate reduction processes (DNRPs) and the fate of reactive nitrogen remain poorly understood. In this study, the rates of DNRPs and the abundances of related functional genes were investigated in aquaculture and non-aquaculture areas. The results showed that marine aquaculture significantly increased the denitrification (DNF) and dissimilatory nitrate reduction to ammonium (DNRA) rates and decreased the rate of anaerobic ammonium oxidation (ANA), as compared with non-aquaculture sites. DNF was the dominant pathway contributing to the total nitrate reduction, and its contribution to the total nitrate reduction significantly increased from 66.72% at non-aquaculture sites to 78.50% at aquaculture sites. Marine aquaculture can significantly affect the physicochemical characteristics of sediment and the abundances of related functional genes, leading to variations in the nitrate reduction rates. Although nitrate removal rates increased in the marine aquaculture area, ammonification rates and the nitrogen retention index in the aquaculture areas were 2.19 and 1.24 times, respectively, higher than those at non-aquaculture sites. Net reactive nitrogen retention exceeded nitrogen removal in the aquaculture area, and the retained reactive nitrogen could diffuse with the tidal current to the entire bay, thereby aggravating N pollution in the entire study area. These results show that marine aquaculture is the dominant source of nitrogen pollution in semi-enclosed bays. This study can provide insights into nitrogen pollution control in semi-enclosed bays with well-developed marine aquaculture.     

Effect of alkaline earth metal promoter on catalytic activity of MnO2 for the complete oxidation of toluene

Herein, Na⁺ and Ca²⁺ are introduced to MnO₂ through cation-exchange method. The presence of Na⁺ and Ca²⁺ significantly enhance the catalytic activity of MnO₂ in toluene oxidation. Among them, the Ca-MnO₂ catalyst exhibits the best catalytic activity (T₅₀ = 194°C, T₉₀ = 215°C, E_a = 57.2 kJ/mol, reaction rate 8.40 × 10^?10 mol/(sec?m²) at 210°C. T₅₀ and T₉₀: the temperature of 50% and 90% toluene conversion; E_a: apparent activation energy) and possess high tolerance against 2.0 vol.% water vapor. Results reveal that the increased acidic sites of the MnO₂ sample can enhance the adsorption of gaseous toluene, and the mobility of oxygen species and the content of reactive oxygen species in the catalyst are significantly improved due to the formed oxygen vacancy. Thus these two factors result in excellent catalytic performance for toluene oxidation combining with the weak CO₂ adsorption ability.     

Identification of close relationship between atmospheric oxidation and ozone formation regimes in a photochemically active region

Understanding ozone (O₃) formation regime is a prerequisite in formulating an effective O₃ pollution control strategy. Photochemical indicator is a simple and direct method in identifying O₃ formation regimes. Most used indicators are derived from observations, whereas the role of atmospheric oxidation is not in consideration, which is the core driver of O₃ formation. Thus, it may impact accuracy in signaling O₃ formation regimes. In this study, an advanced three-dimensional numerical modeling system was used to investigate the relationship between atmospheric oxidation and O₃ formation regimes during a long-lasting O₃ exceedance event in September 2017 over the Pearl River Delta (PRD) of China. We discovered a clear relationship between atmospheric oxidative capacity and O₃ formation regime. Over eastern PRD, O₃ formation was mainly in a NO_x-limited regime when HO₂/OH ratio was higher than 11, while in a VOC-limited regime when the ratio was lower than 9.5. Over central and western PRD, an HO₂/OH ratio higher than 5 and lower than 2 was indicative of NO_x-limited and VOC-limited regime, respectively. Physical contribution, including horizontal transport and vertical transport, may pose uncertainties on the indication of O₃ formation regime by HO₂/OH ratio. In comparison with other commonly used photochemical indicators, HO₂/OH ratio had the best performance in differentiating O₃ formation regimes. This study highlighted the necessities in using an atmospheric oxidative capacity-based indicator to infer O₃ formation regime, and underscored the importance of characterizing behaviors of radicals to gain insight in atmospheric processes leading to O₃ pollution over a photochemically active region.