黄海麻坑群沉积物磷的保存与转化及环境效应

基于对北黄海典型麻坑群海域某单位麻坑内部和外缘沉积物中不同赋存形态的磷、甲烷（CH₄）和硫化物等参数的分析,探讨了麻坑独特的环境中磷的转化与埋藏机制、沉积物-水体系磷的释放及对区域磷循环的影响.研究表明,沉积物中碎屑态磷（Det-P）是磷主要的赋存形态（>50%）,其次是有机磷（Org-P）、铁结合态磷（Fe-P）和自生态磷（Auth-P）,交换态磷（Exch-P）对总磷的贡献较小;麻坑内部与麻坑外缘处沉积物中溶解态活性磷（DRP）向水体的释放通量分别为2.84μmol/（cm²·a）和1.03μmol/（cm²·a）,对上层水体的贡献依次为19.6%和3.03%,是上层水体磷的重要来源.麻坑内外磷的埋藏速率与转化过程存在不同;研究区地下水的渗漏是磷的沉积速率和释放通量都普遍高的原因.北黄海麻坑区沉积物中磷的保存与转化还与浅层CH₄的逸出相关,潜在提高黄铁矿的生成速率.较高的沉积物-水界面磷通量必然对区域富营养化等生态环境问题产生深远影响,值得关注.     

新型厌氧多级喷动床及其厌氧氨氧化脱氮性能分析

为改善厌氧反应器内的流态,加快污泥的颗粒化和形成具有生态梯度的微生物生态系统,设计并制作了新型厌氧多级喷动床,实验测试了反应器的水力喷动、气体喷涌和污泥分层分级现象。在常温下,利用新型厌氧多级喷动床接种混合污泥,经过42 d的培养,成功启动厌氧氨氧化反应器,稳定运行18 d后,NH₄+-N、NO₂--N去除率均达到90%以上。启动60 d后,反应器底部出现大量粒径2 mm左右的颗粒污泥,且污泥具有良好的稳定性和沉降性能,沉降速度达到70 m/h。结果表明:厌氧多级喷动床因其特殊的水力结构,可有效加快污泥的颗粒化。     

Aerosol optical properties under different pollution levels in the Pearl River Delta (PRD) region of China

To clarify the aerosol hygroscopic growth and optical properties of the Pearl River Delta(PRD)region,integrated observations were conducted in Heshan City of Guangdong Province from October 19 to November 17,2014.The concentrations and chemical compositions of PM_(2.5),aerosol optical properties and meteorological parameters were measured.The mean value of PM_(2.5) increased from less than 35(excellent) to 35-75 μg/m~3(good) and then to greater than 75 μg/m~3(pollution),corresponding to mean PM_(2.5) values of 24.9,51.2,and 93.3 μg/m~3,respectively.The aerosol scattering hygroscopic growth factor(f(RH = 80%)) values were 2.0,2.12,and 2.18 for the excellent,good,and pollution levels,respectively.The atmospheric extinction coefficient(σext)and the absorption coefficient of aerosols(σ_(ap)) increased,and the single scattering albedo(SSA)decreased from the excellent to the pollution levels.For different air mass sources,under excellent and good levels,the land air mass from northern Heshan had lower f(RH) and σ_(sp) values.In addition,the mixed aerosol from the sea and coastal cities had lower f(RH) and showed that the local sources of coastal cities have higher scattering characteristics in pollution periods.     

Regulated emission characteristics of in-use LNG and diesel semi-trailer towing vehicles under real driving conditions using PEMS

On-road driving emissions of six liquefied natural gas(LNG) and diesel semi-trailer towing vehicles(STTVs) which met China Emission Standard IV and V were tested using Portable Emission Measurement System(PEMS) in northern China.Emission characteristics of these vehicles under real driving conditions were analyzed and proved that on-road emissions of heavy-duty vehicles(HDVs) were underestimated in the past.There were large differences among LNG and diesel vehicles, which also existed between China V vehicles and China IV vehicles.Emission factors showed the highest level under real driving conditions, which probably be caused by frequent acceleration, deceleration, and start-stop.NOx emission factors ranged from 2.855 to 20.939 g/km based on distance-traveled and 6.719–90.557 g/kg based on fuel consumption during whole tests, which were much higher than previous researches on chassis dynamometer.It was inferred from tests that the fuel consumption rate of the test vehicles had a strong correlation with NOx emission, and the exhaust temperature also affected the efficiency of Selected Catalytic Reduction(SCR) aftertreatment system, thus changing the NOx emission greatly.THC emission factors of LNG vehicles were 2.012–10.636 g/km, which were much higher than that of diesel vehicles(0.029–0.185 g/km).Unburned CH_4 may be an important reason for this phenomenon.Further on-road emission tests, especially CH_4 emission test should be carried out in subsequent research.In addition, the Particulate Number(PN) emission factors of diesel vehicles were at a very high level during whole tests, and Diesel Particulate Filter(DPF)should be installed to reduce PN emission.     

Development of a static test apparatus for evaluating the performance of three PM2.5 separators commonly used in China

PM_(2.5) separator directly affects the accuracy of PM_(2.5) sampling.The specification testing and evaluation for PM_(2.5) separator is particularly important,especially under China's wide variation of terrain and climate.In this study,first a static test apparatus based on polydisperse aerosol was established and calibrated to evaluate the performance of the PM_(2.5) separators.A uniform mixing chamber was developed to make particles mix completely.The aerosol concentration relative standard deviations of three test points at the same horizontal chamber position were less than 0.57%,and the particle size distribution obeyed logarithmic normal distribution with an R~2 of 0.996.The flow rate deviation between the measurement and the set point flow rate agreed to within ± 1.0% in the range of -40 to 50℃.Secondly,the separation,flow and loading characteristics of three cyclone separators(VSCC-A,SCC-A and SCC112) were evaluated using this system.The results showed that the 50% cutoff sizes(D_(50)) of the three cyclones were 2.48,2.47 and 2.44 μm when worked at the manufacturer's recommended flow rates,respectively.The geometric standard deviation(GSD) of the capture efficiency of VSCCA was 1.23,showed a slightly sharper than SCC-A(GSD = 1.27),while the SCC112 did not meet the relevant indicator(GSD = 1.2 ± 0.1) with a GSD = 1.44.The flow rate and loading test had a great effect on D_(50),while the GSD remained almost the same as before.In addition,the maintenance frequency under different air pollution conditions of the cyclones was summarized according to the loading test.     

Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

In this work, a series of Cu-ZSM-5 catalysts with different SiO₂/Al₂O₃ ratios (25, 50, 100 and 200) were synthesized and investigated in n-butylamine catalytic degradation. The n-butylamine can be completely catalytic degradation at 350°C over all Cu-ZSM-5 catalysts. Moreover, Cu-ZSM-5 (25) exhibited the highest selectivity to N₂, exceeding 90% at 350°C. These samples were investigated in detail by several characterizations to illuminate the dependence of the catalytic performance on redox properties, Cu species, and acidity. The characterization results proved that the redox properties and chemisorption oxygen primarily affect n-butylamine conversion. N₂ selectivity was impacted by the Brønsted acidity and the isolated Cu²⁺ species. Meanwhile, the surface acid sites over Cu-ZSM-5 catalysts could influence the formation of Cu species. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra was adopted to explore the reaction mechanism. The Cu-ZSM-5 catalysts are the most prospective catalysts for nitrogen-containing volatile organic compounds removal, and the results in this study could provide new insights into catalysts design for VOC catalytic oxidation.     

UV/H2O2 oxidation of tri(2-chloroethyl) phosphate: Intermediate products, degradation pathway and toxicity evaluation

Tri(2-chloroethyl) phosphate (TCEP) with the initial concentration of 5 mg/L was degraded by UV/H₂O₂ oxidation process. The removal rate of TCEP in the UV/H₂O₂ system was 89.1% with the production of Cl^? and PO₄^3? of 0.23 and 0.64 mg/L. The removal rate of total organic carbon of the reaction was 48.8% and the pH reached 3.3 after the reaction. The oxidative degradation process of TCEP in the UV/H₂O₂ system obeyed the first order kinetic reaction with the apparent rate constant of 0.0025 min^?1 (R²=0.9788). The intermediate products were isolated and identified by gas chromatography-mass spectrometer. The addition reaction of HO? and H₂O and the oxidation reaction with H₂O₂ were found during the degradation pathway of 5 mg/L TCEP in the UV/H₂O₂ system. For the first time, environment risk was estimated via the “ecological structure activity relationships” program and acute and chronic toxicity changes of intermediate products were pointed out. The luminescence inhibition rate of photobacterium was used to evaluate the acute toxicity of intermediate products. The results showed that the toxicity of the intermediate products increased with the increase of reaction time, which may be due to the production of chlorine compounds. Some measures should be introduced to the UV/H₂O₂ system to remove the highly toxic Cl-containing compounds, such as a nanofiltration or reverse osmosis unit.     

Chemical characteristics of road dust PM2.5 fraction in oasis cities at the margin of Tarim Basin

In order to understand the compositions characteristics of particulate matter with aerodynamic diameter less than 2.5 μm (PM_2.5) fraction in road dust (RD_2.5) of oasis cities on the edge of Tarim Basin, 30 road dust (RD) samples were collected in Kashi, Cele, and Yutian in the spring, 2018, and RD_2.5 was collected using the resuspension approach. Eight water-soluble ions, 39 trace elements and 8 fractions of carbon-containing species in PM_2.5 were analyzed. Ca²⁺ and Ca were the most abundant ions and elements in RD_2.5 (7.1% and 9.5%). Cl^- in RD_2.5 was affected not only by attributed to saline-alkali soils in oasis cities of the Tarim Basin and dust from Taklimakan Desert but also by human activities. Moreover, the organic carbon/elemental carbon (OC/EC) ratio indicated that carbon components in RD_2.5 in Cele town mainly come from fossil fuel combustion, while those in Yutian and Kashi mainly come from biomass combustion. It is noteworthy that high Ca in RD_2.5 was seriously affected by anthropogenic emissions, and high Na and K contents in RD_2.5 could be derived from soil and desert dust. It was estimated that Cd, Tl, Sn and Cr were emitted from anthropogenic emissions using the enrichment factor. The coefficients of divergence (COD) result indicated that the influence of local emission on road dust emission is greater than that of long-distance transmission. This study is the first time to comprehensively analyze the chemical characteristics of road dust in oasis cities, and the results provides the sources of road dust at the margin of Tarim Basin.     

Photodegradation of Hexafluoropropylene Oxide Trimer Acid under UV Irradiation

As a novel alternative to traditional perfluoroalkyl substances (PFASs), including perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), hexafluoroproplyene oxide trimer acid (HFPO-TA) has been detected worldwide in surface water. Moreover, recent researches have demonstrated that HFPO-TA has stronger bioaccumulation potential and higher hepatotoxicity than PFOA. To treat these contaminants e.g. PFOA and PFOS, some photochemical techniques by adding exogenous substances had been reported. However, there is still no report for the behavior of HFPO-TA itself under direct UV irradiation. The current study investigated the photo-transformation of HFPO-TA under UV irradiation in aqueous solution. After 72 hr photoreaction, 75% degradation ratio and 25% defluorination ratio were achieved under ambient condition. Reducing active species, i.e., hydrated electrons and active hydrogen atoms, generated from water splitting played dominant roles in degradation of HFPO-TA, which was confirmed by different effects of reaction atmospheres and quenching experiments. A possible degradation pathway was proposed based on the products identification and theoretical calculations. In general, HFPO-TA would be transformed into shorter-chain PFASs, including hexafluoropropylene oxide dimer acid (HFPO-DA), perfluoropropionic acid (PFA) and trifluoroacetate (TFA). This research provides basic information for HFPO-TA photodegradation process and is essential to develop novel remediation techniques for HFPO-TA and other alternatives with similar structures.     

Analytical methods and environmental processes of nanoplastics

The degradation of plastic debris may result in the generation of nanoplastics (NPs). Their high specific surface area for the sorption of organic pollutions and toxic heavy metals and possible transfer between organisms at different nutrient levels make the study of NPs an urgent priority. However, there is very limited understanding on the occurrence, distribution, abundant, and fate of NPs in the environment, partially due to the lack of suitable techniques for the separation and identification of NPs from complex environmental matrices. In this review, we first overviewed the state-of-the-art methods for the extraction, separation, identification and quantification of NPs in the environment. Some of them have been successfully applied for the field determination of NPs, while some are borrowed from the detection of microplastics or engineered nanomaterials. Then the possible fate and transport of NPs in the environment are thoroughly described. Although great efforts have been made during the recent years, large knowledge gaps still exist, such as the relatively high detection limit of existing method failing to detect ultralow masses of NPs in the environment, and spherical polystyrene NP models failing to represent the various compositions of NPs with different irregular shapes, which needs further investigation.