A review of gas-phase chemical mechanisms commonly used in atmospheric chemistry modelling

The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species. Since the first tropospheric chemical mechanism was proposed in the 1960s, various mechanisms including Master Chemical Mechanism (MCM), Carbon Bond Mechanism (CBM), Statewide Air Pollution Research Center (SAPRC) and Regional Atmospheric Chemistry Mechanism (RACM) have been developed for different research purposes. This work summarizes the development and applications of these mechanisms, introduces their compositions and lumping methods, and compares the ways the mechanisms treat radicals with box model simulations. CBM can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM, whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in RACM. The photolysis rates of some oxygenated compounds are low in SAPRC07, which may result in underestimation of radical levels. As an explicit chemical mechanism, MCM describes the chemical processes of primary pollutants and their oxidation products in detail. MCM can be used to investigate certain chemical processes; however, due to its large size, it is rarely used in regional model simulations. A box model case study showed that the chemical behavior of OH and HO₂ radicals and the production of ozone were well described by all mechanisms. CBM and SAPRC underestimated the radical levels for different chemical treatments, leading to low ozone production values in both cases. MCM and RACM are widely used in box model studies, while CBM and SAPRC are often selected in regional simulations.     

Pollution characteristics and health risk assessment of polycyclic aromatic hydrocarbons and nitrated polycyclic aromatic hydrocarbons during heating season in Beijing

Polycyclic aromatic hydrocarbons(PAHs) and their nitrated derivatives(NPAHs) attract continuous attention due to their outstanding carcinogenicity and mutagenicity. In order to investigate the diurnal variations, sources, formation mechanism, and health risk assessment of them in heating season, particulate matter(PM) were collected in Beijing urban area from December 26, 2017 to January 17, 2018. PAHs and NPAHs in PM were quantitatively analyzed via gas chromatography-mass spectrometry(GC-MS). ...     

生物炭施用对紫色土旱坡地土壤氮流失形态及通量的影响

明确生物炭施用对紫色土旱坡地土壤氮流失形态及通量的影响,为提升紫色土旱坡地耕地质量及减少紫色土旱坡地农业面源污染发生风险提供科学依据.以油菜/玉米轮作农田生态系统为研究对象,通过田间试验,研究了不施肥(对照)、常规施肥、优化施肥及生物炭(化肥减量配施生物炭)这4个处理对紫色土旱坡地地表径流和壤中流氮素流失形态及通量的影响.结果表明:①在各施肥处理中,常规处理总径流量最大,为16 133 L·a~(-1),生物炭处理总径流量最小,为11 893 L·a~(-1).各施肥处理以壤中流为主要径流方式,壤中流流失量占总流失量的61.80%～68.60%;与对照(不施肥处理)相比,其余各施肥处理泥沙流失量均有所降低,其中常规处理降低的效果最明显.②铵态氮主要通过地表径流流失,占总流失通量的86.51%～96.58%;铵态氮流失通量最大的为施生物炭处理[0.69 kg·(hm~2·a)~(-1)].③各施肥处理产流中的颗粒态氮浓度均高于对照处理,且常规施肥处理的颗粒态氮流失通量最大,为2.87 kg·(hm~2·a)~(-1).④各施肥处理的壤中流和地表径流中的全氮浓度和硝态氮浓度均存在极显著正相关关系(P0.01).硝态氮是全氮流失的主要形态,且二者均以壤中流为主要流失途径;全氮通过壤中流流失占比为72.86%～89.13%,且常规施肥处理的全氮总流失通量最大,为35.58 kg·(hm~2·a)~(-1),而施生物炭处理全氮总流失通量最小,为21.49 kg·(hm~2·a)~(-1).化肥减量配施生物炭能明显降低径流量和氮的流失通量,可有效阻控农业面源污染发生的风险.     

珠江三角洲地区冬季硫、氮干沉降的来源解析

采用WRF-CMAQ模式对珠江三角洲地区2015年1月进行数值模拟,结合CMAQ的集成源解析方法ISAM对S、N及其干沉降的来源贡献进行分析.结果表明：珠江三角洲地区S、N干沉降量高值主要分布在广佛交界处以及珠江口附近,其逐日变化趋势主要受质量浓度变化影响,但在部分时间段受干沉降速率的影响亦相当显著.珠江三角洲区域内排放源对于S干沉降的平均贡献占比为36.2%,与其质量浓度区域内贡献占比相当,SO₂干沉降速率增加以及背景风场变弱会使区域内贡献占比增加;区域内源对于N干沉降的平均贡献占比为32.4%,远小于其质量浓度区域内贡献占比,当NO₂质量浓度减少,使得HNO₃的质量浓度和干沉降量减少时,区域内贡献占比增加.对于珠江三角洲典型城市,广州S干沉降的本地贡献为27.7%,N为14.2%;江门S干沉降的本地贡献为9.6%,N为8.8%.2个城市对比而言,广州受本地的影响较江门显著,江门受其上风方向广州和佛山两市输送的影响显著,但当背景风场减弱时,江门本地贡献会有明显增加.     

太湖流域典型城镇水环境芳香胺类污染特征

利用固相萃取-气相色谱/串联质谱法(SPE-GC-MS/MS),对太湖流域上游城镇常州武南地区的地表水体和典型排放源中的4种芳香胺类污染物(AAs)进行连续2年监测,综合分析了2018~2019年间AAs的污染及浓度特征.结果表明,武南地区河网中目标AAs的总浓度范围为相似文献   

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.     

Isolation and characterization of a strain with high microbial attachment in aerobic granular sludge

Aerobic granule is a special microbial aggregate associated with biofilm structure. The formation of aerobic granular sludge is primarily depending on its bacterial community and relevant microbiological properties. In this experiment, a strain with high microbial attachment was isolated from aerobic granular sludge, and the detailed characteristics were examined. Its high attachment ability could reach 2.34 (OD_600nm), while other low attachment values were only around 0.06-0.32, which indicated a big variation among the different bacteria. The strain exhibited a very special morphology with many fibric fingers under SEM observation. A distinctive behaviour was to form a spherical particle by themselves, which would be very beneficial for the formation and development of granular sludge. The EPS measurement showed that its PN content was higher than low attachment bacteria, and 3D-EEM confirmed that there were some different components. Based on the 16S rRNA analysis, it was identified to mostly belong to Stenotrophomonas. Its augmentation to particle sludge cultivation demonstrated that the strain could significantly promote the formation of aerobic granule. Conclusively, it was strongly suggested that it might be used as a good and potential model strain or chassis organism for the aerobic granular sludge formation and development.     

铝穹顶储罐雷击损伤及燃爆风险研究

针对铝穹顶储罐雷击问题,开展了回击后长持续时间雷电流分量作用下的铝合金板烧蚀损伤试验研究,分析了铝穹顶储罐损伤及油气燃爆风险。结果表明:当直流分量为164 C时,2 mm铝板发生穿孔,铝穹顶储罐存在雷击燃爆风险;当直流分量≤157 C时,未穿孔,背面温度最高为480℃,存在燃爆风险,铝穹顶储罐存在雷击燃爆风险;当直流分量196 C时,4 mm铝板发生穿孔;当直流分量为196 C时,6 mm铝板未发生穿孔,背面温升为125℃,小于205℃,铝穹顶储罐不存在雷击燃爆风险。