基于LOADEST和数字滤波的水源地基流氮素输出定量方法应用实例

地表直接径流和基流均是流域非点源氮/磷养分输出的重要水文途径.科学认识和定量模拟基流氮/磷养分输出对于准确解析水源地水体非点源污染来源至关重要.基于Load Estimator模型和数字滤波算法,建立了定量水源地基流氮素输出的方法体系.以浙江省珊溪水源地的玉泉溪流域为例,利用玉泉溪2010-01—2013-12期间逐月总氮(TN)水质监测数据和逐日流量数据,展示了该方法的计算过程.结果表明,本文建立的水源地基流氮素输出定量方法结果合理,模拟精度高,决定系数和纳什系数分别为0.83和0.80;玉泉溪流域2010—2013年TN负荷量为141.21～274.68 t·a~(-1),平均208.63 t·a~(-1),年基流TN负荷量为84.39～168.68 t·a~(-1),平均127.69 t·a~(-1);基流对玉泉溪年均TN负荷量贡献率高达60%以上,流域基流养分输出对地表水体的污染应引起足够重视.     

基于遥感尾气监测的柴油车气态污染物排放因子计算方法研究

采用遥感尾气测试系统实测了柴油车在实际道路工况下的CO、HC和NO排放特征,修正了排放因子的计算方法,并与车载排放测试系统（PEMS）实测结果进行了验证,获得了实测车辆的CO、HC和NO排放因子.测试结果显示,在各种遥感监测的工况下柴油车尾气中均含有较高浓度的氧气,未考虑氧气影响的燃烧方程反演获得的各污染物体积浓度计算值与PEMS实测值的偏差较大,且氧气浓度越大,偏差越大.经过氧气修正的燃烧方程反演计算的尾气浓度与PEMS实测值吻合度大幅提升,适用于实际工况下遥感检测车辆尾气的反演计算.修正算法得到CO、HC和NO的排放因子离散性较小,精确度较高,可以为量化柴油车尾气排放贡献提供科学依据.     

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.     

Adsorption of 17β-estradiol from aqueous solution by raw and direct/pre/post-KOH treated lotus seedpod biochar

Five biochars derived from lotus seedpod(LSP) were applied to examine and compare the adsorption capacity of 17β-estradiol(E2) from aqueous solution.The effect of KOH activation and the order of activation steps on material properties were discussed.The effect of contact time,initial concentration,p H,ionic strength and humic acid on E2 adsorption were investigated in a batch adsorption process.Experimental results demonstrated that the pseudo second-order model fitted the experimental data best and that adsorption equilibrium was reached within 20 hr.The efficiency of E2 removal increased with increasing E2 concentration and decreased with the increase of ionic strength.E2 adsorption on LSP-derived biochar(BCs) was influenced little by humic acid,and slightly affected by the solution p H when its value ranged from 4.0 to 9.0,but considerably affected at p H 10.0.Low environmental temperature is favorable for E2 adsorption.Chemisorption,π–π interactions,monolayer adsorption and electrostatic interaction are the possible adsorption mechanisms.Comparative studies indicated that KOH activation and the order of activation steps had significant impacts on the material.Post-treated biochar exhibited better adsorption capacity for E2 than direct treated,pretreated,and raw LSP biochar.Pyrolyzed biochar at higher temperature improved E2 removal.The excellent performance of BCs in removing E2 suggested that BCs have potential in E2 treatment and that the biochar directly treated by KOH would be a good choice for the treatment of E2 in aqueous solution,with its advantages of good efficiency and simple technology.     

Cytotoxicity of the soluble and insoluble fractions of atmospheric fine particulate matter

Inhaled atmospheric fine particulate matter(PM_(2.5)) includes soluble and insoluble fractions,and each fraction can interact with cells and cause adverse effects.PM_(2.5) samples were collected in Jinan,China,and the soluble and insoluble fractions were separated.According to physiochemical characterization,the soluble fraction mainly contains watersoluble ions and organic acids,and the insoluble fraction mainly contains kaolinite,calcium carbonate and some organic carbon.The interaction between PM_(2.5) and model cell membranes was examined with a quartz crystal microbalance with dissipation(QCM-D) to quantify PM_(2.5) attachment on membranes and membrane disruption.The cytotoxicity of the total PM_(2.5) and the soluble and insoluble fractions,was investigated.Negatively charged PM_(2.5) can adhere to the positively charged membranes and disrupt them.PM_(2.5)also adheres to negatively charged membranes but does not cause membrane rupture.Therefore,electrostatic repulsion does not prevent PM_(2.5) attachment,but electrostatic attraction induces remarkable membrane rupture.The human lung epithelial cell line A549 was used for cytotoxicity assessment.The detected membrane leakage,cellular swelling and blebbing indicated a cell necrosis process.Moreover,the insoluble PM_(2.5) fraction caused a higher cell mortality and more serious cell membrane damage than the soluble fraction.The levels of reactive oxygen species(ROS) enhanced by the two fractions were not significantly different.The findings provide more information to better understand the mechanism of PM_(2.5) cytotoxicity and the effect of PM_(2.5) solubility on cytotoxicity.     

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.     

贵州农村污水典型抗生素污染水平及生态风险

抗生素残留物是一种新兴的微污染物,广泛存在于各种环境介质及生物样品中,长期暴露在抗生素环境会对人体健康、生态环境产生一定的潜在威胁。由于农村污水排放量逐渐增大、农村地区对抗生素的不合理使用以及受经济、地理地形的限制大部分农村地区都缺乏完整的污水收集管网和污水治理设施,进而导致抗生素通过多种途径进入农村环境,可能会对农村生态环境产生一定的环境风险。为了解贵州农村污水中抗生素的污染水平及处理后污水对环境的影响,作者采用固相萃取—液相色谱—串联质谱(SPE-LC-MS)联用技术,选取贵州省3处典型农村地区,对农村污水治理设施进出水中典型抗生素(包括6种磺胺类、3种四环素类、1种喹诺酮类抗生素)的浓度水平进行分析。结果表明,3处农村污水治理设施进水和出水中均检出不同程度的抗生素,浓度范围分别在ND～417.57 ng/L和ND～253.68 ng/L,其中土霉素浓度最高,进出水的浓度分别为417.57、253.68 ng/L;其次是氧氟沙星,在进出水中的最高浓度分别为278.75、183.73 ng/L。3处农村污水治理设施对抗生素的去除率在-58.32%～45.52%,对目标抗生素的去除率较低。与国内外其他地区农村污水相比,所选地区的进出水中抗生素的浓度较高。通过生态风险评估发现,经处理后的污水中均含有一种RQ≥1的抗生素物质,并且发现氧氟沙星为处理后污水中的高风险污染物,污水的排放会对环境造成一定的生态风险。     

天津市河流生态完整性评价

对河流生态健康状况进行评价,可为河流治理和生态修复提供依据.基于2018年8—9月天津市河流现场调查获取的物理、化学和生物群落指标（浮游动物、浮游植物、底栖动物、鱼类、水生大型植物、陆生植物）数据,构建包含物理完整性、化学完整性和生物完整性在内的河流IEI（index of ecological integrity,生态完整性指数）评价体系,对天津市河流生态健康状况进行评价.根据生物栖息地评分和水质状况确定参照点位,采用标准化方法筛选候选指标,应用层次分析法计算三部分指标权重,最终得出天津市河流生态健康评价结果.结果表明:①IEI评价结果显示,天津市河流生态健康状况等级为“健康”的样点占18.8%,“较好”的样点占28.1%,“一般”的样点占40.6%,“较差”的样点占6.3%,“差”的样点占6.3%,天津市河流生态健康状况整体处于“一般”水平.②相关性分析表明,ρ（NH₄+-N）和ρ（COD_Mn）超标是造成天津市水质达不到功能区标准的主要原因,同时也是影响河流生态健康的主要因素.研究显示,IEI评价法能够较为敏感地响应研究区面临的环境压力,适用于评价研究区河流生态健康.