基于AIS轨迹修复的船舶排放空间表征改进方法与应用

基于船舶自动识别系统（Automatic Identification System,AIS）数据表征船舶排放是目前船舶排放空间表征的主流方法,但AIS船舶轨迹点缺失会造成船舶排放量低估和船舶空间分布表征错误,进而影响船舶排放控制区的划分.为改进船舶排放空间表征,本研究以2013年广东省AIS船舶数据为例,采用基于时间和经纬度的三次样条方法对AIS船舶轨迹进行修复,结合动力法计算船舶排放,分析对比AIS轨迹修复前后船舶排放表征的差异,并利用空气质量模型和卫星观测评估AIS轨迹修复对船舶排放表征和广东沿海空气质量模拟的改进效果.结果表明：轨迹修复后广东省海域船舶轨迹点总数由4685773个增至5746664个,船舶NO_x排放量增加了0.6%.对于轨迹点与排放缺失集中的粤东海域,轨迹修复后船舶轨迹点数增加了88%,NO_x排放量在广东省船舶排放量的占比提升至22%,特别是在粤东重点修复海域NO_x排放量增加了2.7倍.原始轨迹在广东省海域较为稀疏,在粤东海域有明显轨迹缺失;轨迹修复后广东省海域船舶轨迹更为密集,粤东海域船舶轨迹得以补充,船舶排放空间分布更连贯.对比模拟结果与卫星观测结果,轨迹修复后粤东重点修复海域船舶模拟浓度与观测浓度的偏差由51%减至6%,总体上船舶排放模拟结果更接近卫星观测结果.     

MnCeOx/沸石催化剂对工业典型VOCs的催化性能

以沸石为载体制备了锰铈复合氧化物催化剂（记为:MnCeO_x/沸石催化剂）,探究了催化剂对工业典型VOCs的二元催化性能,并对催化剂进行BET、XRD及SEM表征。结果表明:Ce的加入,促进了Mn的分散,提高了MnCeO_x/沸石催化剂的活性;当n（Mn）∶n（Ce）为1∶1,负载率为20%,焙烧温度为500℃时,催化剂的活性最高,其对甲苯的起燃温度（T₅₀）和完全燃烧温度（T₉₀）分别为155,255℃;单组分实验中,催化剂对3种有机物均表现出较高活性,转化率达到90%时的反应温度均在275℃以下,其活性顺序为乙酸乙酯>甲苯>丙酮,主要受反应活化能大小及分子极性的影响;二元催化实验中,由于竞争吸附的影响,3种物质的T₅₀和T₉₀较单组分均分别提高了8~13,14~38℃。     

基于在线监测+模型的海绵城市建设径流水量控制效果研究

以青岛市海绵城市典型项目区为研究区,通过收集、整理和概化汇水区资料,构建了研究区降雨径流模型——SWMM模型。利用2018年雨季的降雨-径流实时监测数据,进行了模型关键参数的率定和模型验证,研究了海绵城市建设在削减径流量、增加入渗与滞蓄雨量方面的定量效果。结果显示:海绵改造后,不同降雨强度下形成径流的雨量占总雨量的平均比例由56%下降至29%;下渗雨水的平均比例由40%增加至60%,滞蓄深度由0.63 mm增加至5 mm。海绵改造前后研究区场降雨径流总量控制率变化显著,当以1~10年一遇的短历时（120 min）设计降雨作为模型边界条件进行模拟时,海绵化改造后场次降雨径流总量控制率提高了26%~34%,认为研究区基本达到了海绵城市关于水量控制的建设要求。     

Tuning the fill percentage in the hydrothermal synthesis process to increase catalyst performance for ozone decomposition

The performance of Ce-OMS-2 catalysts was improved by tuning the fill percentage in the hydrothermal synthesis process to increase the oxygen vacancy density. The Ce-OMS-2 samples were prepared with different fill percentages by means of a hydrothermal approach (i.e. 80%, 70%, 50% and 30%). Ce-OMS-2 with 80% fill percentage (Ce-OMS-2-80%) showed ozone conversion of 97%, and a lifetime experiment carried out for more than 20?days showed that the activity of the catalyst still remained satisfactorily high (91%). For Ce-OMS-2-80%, Mn ions in the framework as well as K ions in the tunnel sites were replaced by Ce⁴⁺, while for the others only Mn ions were replaced. O₂-TPD and H₂-TPR measurements proved that the Ce-OMS-2-80% catalyst possessed the greatest number of mobile surface oxygen species. XPS and XAFS showed that increasing the fill percentage can reduce the AOS of Mn and augment the amount of oxygen vacancies. The active sites, which accelerate the elimination of O₃, can be enriched by increasing the oxygen vacancies. These findings indicate that increasing ozone removal can be achieved by tuning the fill percentage in the hydrothermal synthesis process.     

Role of glycine on sulfuric acid-ammonia clusters formation: Transporter or participator

Glycine(Gly) is ubiquitous in the atmosphere and plays a vital role in new particle formation(NPF).However,the potential mechanism of its on sulfuric acid(SA)-ammonia(A)clusters formation under various atmospheric conditions is still ambiguous.Herein,a(Gly)_x·(SA)_y·(A)_z(z≤x+y≤3) multicomponent system was investigated by using density functional theory(DFT) combined with Atmospheric Cluster Dynamics Code(ACDC) at different temperatures and precursor concentrations.The results show that Gly,with one carboxyl(-COOH) and one amine(-NH_2) group,can interact strongly with SA and A in two directions through hydrogen bonds or proton transfer.Within the relevant range of atmospheric concentrations,Gly can enhance the formation rate of SA-A-based clusters,especially at low temperature,low [SA],and median [A].The enhancement(R) of Gly on NPF can be up to 340 at T=218.15 K,[SA]=10~4,[A]=10~9,and [Gly]=10~7 molecules/cm~3.In addition,the main growth paths of clusters show that Gly molecules participate into cluster formation in the initial stage and eventually leave the cluster by evaporation in subsequent cluster growth at low [Gly],it acts as an important "transporter" to connect the smaller and larger cluster.With the increase of [Gly],it acts as a "participator" directly participating in NPF.     

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.     

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.     

Dynamic nano-Ag colloids cytotoxicity to and accumulation by Escherichia coli: Effects of Fe3+, ionic strength and humic acid

Released Ag ions or/and Ag particles are believed to contribute to the cytotoxicity of Ag nanomaterials, and thus, the cytotoxicity and mechanism of Ag nanomaterials should be dynamic in water due to unfixed Ag particle:Ag⁺ ratios. Our recent research found that the cytotoxicity of PVP-Ag nanoparticles is attributable to Ag particles alone in 3 hr bioassays, and shifts to both Ag particles and released Ag⁺ in 48 hr bioassays. Herein, as a continued study, the cytotoxicity and accumulation of 50 and 100 nm Ag colloids in Escherichia coli were determined dynamically. The cytotoxicity and mechanisms of nano-Ag colloids are dynamic throughout exposure and are derived from both Ag ions and particles. Ag accumulation by E. coli is derived mainly from extracellular Ag particles during the initial 12 hr of exposure, and thereafter mainly from intracellular Ag ions. Fe³⁺ accelerates the oxidative dissolution of nano-Ag colloids, which results in decreasing amounts of Ag particles and particle-related toxicity. Na⁺ stabilizes nano-Ag colloids, thereby decreasing the bioavailability of Ag particles and particle-related toxicity. Humic acid (HA) binds Ag⁺ to form Ag⁺-HA, decreasing ion-related toxicity and binding to the E. coli surface, decreasing particle-related toxicity. HA in complex conditions showed a stronger relative contribution to toxicity and accumulation than Na⁺ or Fe³⁺. The results highlighted the cytotoxicity and mechanism of nano-Ag colloids are dynamic and affected by environmental factors, and therefore exposure duration and water chemistry should be seriously considered in environmental and health risk assessments.     

Revealing the changes of bacterial community from water source to consumers tap: A full-scale investigation in eastern city of China

This study profiled the bacterial community variations of water from four water treatment systems, including coagulation, sedimentation, sand filtration, ozonation-biological activated carbon filtration (O₃-BAC), disinfection, and the tap water after the distribution process in eastern China. The results showed that different water treatment processes affected the bacterial community structure in different ways. The traditional treatment processes, including coagulation, sedimentation and sand filtration, reduced the total bacterial count, while they had little effect on the bacterial community structure in the treated water (before disinfection). Compared to the traditional treatment process, O₃-BAC reduced the relative abundance of Sphingomonas in the finished water. In addition, ozonation may play a role in reducing the relative abundance of Mycobacterium. NaClO and ClO₂ had different effects on the bacterial community in the finished water. The relative abundance of some bacteria (e.g. Flavobacterium, Phreatobacter and Porphyrobacter) increased in the finished water after ClO₂ disinfection. The relative abundance of Mycobacterium and Legionella, which have been widely reported as waterborne opportunistic pathogens, increased after NaClO disinfection. In addition, some microorganisms proliferated and grew in the distribution system, which could lead to turbidity increases in the tap water. Compared to those in the finished water, the relative abundance of Sphingomonas, Hyphomicrobium, Phreatobacter, Rheinheimera, Pseudomonas and Acinetobacter increased in the tap water disinfected with NaClO, while the relative abundance of Mycobacterium increased in the tap water disinfected with ClO₂. Overall, this study provided the detailed variation in the bacterial community in the drinking water system.     

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.