污水分析方法监测城市毒品滥用长期趋势

毒品滥用问题是全球广泛关注的社会问题,对城市毒品滥用情况进行长期监测具有重要意义.采用污水流行病学的方法,对大连市毒品的滥用情况进行连续长期调查.2020～2021年采集大连市22个污水处理厂的进口污水,通过气相色谱衍生化方法分析测定甲基苯丙胺、海洛因、氯胺酮、摇头丸和可卡因的生物标志物的浓度,即其尿液代谢产物甲基苯丙胺、吗啡、氯胺酮、摇头丸和苯甲酰芽子碱.结果表明,2020年p(甲基苯丙胺)、p(吗啡)和p(氯胺酮)均值分别为23.69、23.21和2.40 ng·L-1;2021年均值分别为20.64、20.92和0.47 ng·L-1,在所有的污水样品中均未检测出摇头丸和苯甲酰芽子碱,根据相关信息估算5种毒品的人均滥用量,并结合往年监测数据分析大连市这5种毒品的滥用趋势.甲基苯丙胺和海洛因滥用量均在2019年有上升趋势,2020大幅度下降,2021年基本保持不变;氯胺酮的滥用则一直处于较低水平.本研究为大连市实时监控毒品滥用情况提供科学依据,对防治毒品犯罪具有重要意义.     

Effects of reductive inorganics and NOM on the formation of chlorite in the chlorine dioxide disinfection of drinking water

Chlorine dioxide (ClO₂) disinfection usually does not produce halogenated disinfection by-products, but the formation of the inorganic by-product chlorite (ClO₂^–) is a serious consideration. In this study, the ClO₂^– formation rule in the ClO₂ disinfection of drinking water was investigated in the presence of three representative reductive inorganics and four natural organic matters (NOMs), respectively. Fe²⁺ and S^2– mainly reduced ClO₂ to ClO₂^– at low concentrations. When ClO₂ was consumed, the ClO₂^– would be further reduced by Fe²⁺ and S^2–, leading to the decrease of ClO₂^–. The reaction efficiency of Mn²⁺ with ClO₂ was lower than that of Fe²⁺ and S^2–. It might be the case that MnO₂ generated by the reaction between Mn²⁺ and ClO₂ had adsorption and catalytic oxidation on Mn²⁺. However, Mn²⁺ would not reduce ClO₂^–. Among the four NOMs, humic acid and fulvic acid reacted with ClO₂ actively, followed by bovine serum albumin, while sodium alginate had almost no reaction with ClO₂. The maximum ClO₂^– yields of reductive inorganics (70%) was higher than that of NOM (around 60%). The lower the concentration of reductive substances, the more ClO₂^– could be produced by per unit concentration of reductive substances. The results of the actual water samples showed that both reductive inorganics and NOM played an important role in the formation of ClO₂^– in disinfection.     

长江口邻近海域沉积物中厌氧氨氧化细菌分布特征研究

海洋生态系统氮素循环对维持海洋生态收支平衡具有重要意义,由厌氧氨氧化细菌(anaerobic ammonia-oxidizing bacteria,ANAMMOX Bacteria)推动的厌氧氨氧化过程是海洋氮素移除的重要途径.本研究采用荧光定量PCR(q PCR)技术,并结合环境理化因子,分析了2011年夏季长江口邻近海域沉积物中厌氧氨氧化细菌的种群丰度分布特征.结果表明,厌氧氨氧化细菌的种群丰度在长江口邻近海域的空间分布与环境因子密切相关,总有机碳含量、盐度、铵盐浓度对长江口邻近海域沉积物中厌氧氨氧化细菌的种群丰度具有重要调控作用.厌氧氨氧化细菌的丰度分布与总有机碳含量呈显著正相关关系(P0.01,r=0.69),同时又随亚硝酸盐浓度、溶解氧浓度的升高而降低,而盐度对厌氧氨氧化细菌丰度分布的影响较为复杂.     

菌株Desulfovibrio sp. CMX的DNRA性能和影响因素

微生物的硝酸盐异化还原为铵(DNRA)过程对自然界中铵根离子的存在和转化具有重要影响,然而关于SRB菌株DNRA过程影响和机制尚未探明.本文考察了实验室筛选的SRB菌株Desulfovibrio sp.CMX的DNRA能力、影响因素及其影响机制.结果表明,无外加氮源的情况下,分别以10 mmol·L-1NO_3~-和NO_2~-作为唯一电子受体,菌株Desulfovibrio sp.CMX最终NH_4~+生成率分别达到85.8%和97.3%,且无N2和N2O等副产物产生.实验探究了不同外加氮源、不同初始浓度的SO_4~(2-)、S~(2-)对菌株DNRA过程的影响.酵母浸粉作为外加氮源可促进菌株的生长和代谢从而促进菌株DNRA过程;SO_4~(2-)对于NO_3~-还原为NO_2~-阶段起促进作用,而对NO_2~-还原为NH_4~+阶段起抑制作用,综合两方面影响,最终表现出对菌株DNRA过程的抑制作用;S~(2-)对菌株生长及DNRA过程都表现出抑制作用,且S~(2-)浓度越高抑制作用越强,当S~(2-)浓度达到6 mmol·L-1后,S~(2-)对于NO_3~-还原为NO_2~-阶段的抑制作用强于NO_2~-还原为NH_4~+阶段的抑制作用,NO_3~-还原为NO_2~-速率低于NO_2~-还原为NH_4~+速率,此时体系中不再有NO_2~-的积累.     

Synthesis and kinetics investigation of meso-microporous Cu-SAPO-34 catalysts for the selective catalytic reduction of NO with ammonia

A series of meso-microporous Cu-SAPO-34 catalysts were successfully synthesized by a one-pot hydrothermal crystallization method, and these catalysts exhibited excellent NH_3-SCR performance at low temperature. Their structure and physic chemical properties were characterized by means of X-ray diffraction patterns(XRD), Scanning electron microscopy(SEM), Transmission electron microscopy(TEM), N_2 sorption-desorption, nuclear magnetic resonance(NMR), Inductively Coupled Plasma-Atomic Emission spectrometer(ICP-AES), X-ray absorption spectroscopy(XPS),Temperature-programmed desorption of ammonia(NH_3-TPD), Ultraviolet visible diffuse reflectance spectroscopy(UV-Vis DRS) and Temperature programmed reduction(TPR).The analysis results indicate that the high activities of Cu-SAPO-34 catalysts could be attributed to the enhancement of redox property, the formation of mesopores and the more acid sites. Furthermore, the kinetic results verify that the formation of mesopores remarkably reduces diffusion resistance and then improves the accessibility of reactants to catalytically active sites. The 1.0-Cu-SAPO-34 catalyst exhibited the high NO conversion( 90%) among the wide activity temperature window in the range of 150–425℃.     

全球大气硫循环及区域交叉影响

二氧化硫和硫酸盐是硫的重要存在形式,是影响环境空气质量的重要大气污染物.硫酸盐气溶胶是影响全球气候变化的重要大气组分,大气中的硫酸盐气溶胶生命周期短,其浓度空间差异大、时间变化显著.在区域尺度乃至全球尺度研究其迁移转化和区域交叉影响,具有十分重要的科学意义.本研究以2010年SO_2全球排放清单为基础,应用国际通用大气化学模式(Mozart-4),模拟全球大气硫的迁移转化及其季节变化和空间分布特征,并分析全球不同区域间的交叉影响.结果表明:1SO_2柱浓度全球年均值为424.73μg S·m~(-2),中东及南亚最高,达3629.27μg S·m~(-2),南美最低,为181.06μg S·m~(-2).2硫酸盐柱浓度全球年均值为1572.86μg S·m~(-2),东亚年均硫酸盐柱浓度最高,达4556.58μg S·m~(-2),南美最低,为1014.33μg S·m~(-2).3冬季SO_2柱浓度高于其他春夏秋3季,夏季硫酸盐柱浓度高于冬季,主要是由于冬季低温使SO_2不易转化为硫酸盐.4硫酸盐表现出明显的全球迁移特征,全球各区域间交叉影响显著.东亚的净输出量最大,达4.01 Tg S·a~(-1).非洲、中亚及俄罗斯硫酸盐柱浓度的外源影响比例分别高达80.54%和73.00%.     

利用膜进样质谱连续走航测定表层海水O2/Ar比值和pCO2

利用HIDEN公司HPR40溶解气体质谱分析仪,通过实验探索和实际应用,建立了连续走航高频率同时测定海水中O₂、Ar和CO₂等多种气体的分析方法。通过选择硅树脂膜的循环水取样器、进样流量为220 mL/min、进样平衡温度低于海水2℃等实验条件,建立了船载连续走航系统,实现了利用膜进样质谱仪（MIMS）连续走航测定表层海水O₂/Ar比值和pCO₂。所用仪器稳定性良好,连续测定12 h大气鼓泡48 h后的海水样品获得O₂、Ar和CO₂的精密度分别为1.57%、3.75%和2.21%,O₂/Ar的精密度为2.61%;该方法的重复性好,10 d内绘制7条CO₂工作曲线斜率的相对标准偏差RSD=4.18%。应用该方法在南海北部陆坡19.8°N～20.8°N,114.7°E～115°E断面进行调查并取得了很好的效果,结果表明:该调查断面的生物氧过饱和量Δ（O₂/Ar）为0.56%±1.02%,其变化范围为-2.52%至3.34%,调查断面的pCO₂值为361.53±40.46μatm。该方法具有直接、快速、高时空分辨率测定多种溶解气体的优点,为认识多组分气体的高分辨时空分布格局,深入开展我国陆架边缘海生物过饱和氧、海洋群落净生产力和pCO₂动力学研究提供了新方法。     

Regeneration of commercial selective catalyst reduction catalysts deactivated by Pb and other inorganic elements

The regeneration of commercial SCR(Selective Catalyst Reduction) catalysts deactivated by Pb and other elements was studied.The deactivated catalyst samples were prepared by chemical impregnation with mixed solution containing K_2SO_4,Na_2SO_4,CaSO_4,Pb(NO_3)_2and NH_4H_2PO_4.A novel method combining Ethylenediaminetetraacetic acid disodium salt(EDTA-2Na) and H_2SO_4solution(viz.catalysts treated by dilute EDTA-2Na and H_2SO_4 solution in sequence) was used to recover the activity of deactivated samples,and the effect was compared with single H_2SO_4,oxalic acid,acetic acid,EDTA or HNO_3 solutions.The surface structure,acidity and reducibility of samples were characterized by N_2adsorption–desorption,inductively coupled plasma optical emission spectrometer(ICP-OES),scanning electron microscopy(SEM),X-ray diffraction(XRD),X-ray fluorescence(XRF),H-2-temperature programmed section(H_2-TPR),NH3-temperature programmed desorption(NH3-TPD) and in situ DRIFTS.Impurities caused a decrease of specific surface area and surface reducibility,as well as Br?nsted acid sites,and therefore led to severe deactivation of the SCR catalyst.The use of an acid solution alone possibly eliminated the impurities on the deactivated catalyst to some extent,and also increased the specific surface area and Br?nsted acid sites and promoted the surface reducibility,thus recovered the activity partially.The combination of EDTA-2Na and H_2SO_4 could remove most of the impurities and improve the activity significantly.The removal of Pb should be an important factor for regeneration.Due to a high removal rate for Pb and other impurities,the combination of EDTA-2Na and H_2SO_4 solutions provided the best efficiency.     

Estimating emissions from crop residue open burning in China based on statistics and MODIS fire products

With the objective of reducing the large uncertainties in the estimations of emissions from crop residue open burning, an improved method for establishing emission inventories of crop residue open burning at a high spatial resolution of 0.25°× 0.25° and a temporal resolution of1 month was established based on the moderate resolution imaging spectroradiometer(MODIS) Thermal Anomalies/Fire Daily Level3 Global Product(MOD/MYD14A1). Agriculture mechanization ratios and regional crop-specific grain-to-straw ratios were introduced to improve the accuracy of related activity data. Locally observed emission factors were used to calculate the primary pollutant emissions. MODIS satellite data were modified by combining them with county-level agricultural statistical data, which reduced the influence of missing fire counts caused by their small size and cloud cover. The annual emissions of CO_2, CO, CH_4,nonmethane volatile organic compounds(NMVOCs), N_2O, NO_x, NH_3, SO_2, fine particles(PM2.5),organic carbon(OC), and black carbon(BC) were 150.40, 6.70, 0.51, 0.88, 0.01, 0.13, 0.07, 0.43,1.09, 0.34, and 0.06 Tg, respectively, in 2012. Crop residue open burning emissions displayed typical seasonal and spatial variation. The highest emission regions were the Yellow-Huai River and Yangtse-Huai River areas, and the monthly emissions were highest in June(37%).Uncertainties in the emission estimates, measured as 95% confidence intervals, range from a low of within ±126% for N_2O to a high of within ± 169% for NH_3.     

中国页岩气开发过程环境管理现状与对策分析研究

中国页岩气资源储量丰富,随着页岩气商业勘探开发的不断推进,引发的生态环境问题日益突出.从页岩气开采工艺来看,开发对水、大气、土壤及生态地质环境等都有一定的影响.此外,中国页岩气开发过程中还存在法规标准体系不健全、监管机制缺乏、环境准入机制不明等问题.因此,针对页岩气开发所带来的环境风险,亟需完善法律法规与标准体系、严格监督管理、制定开发环境规划.同时,建设环保示范工程,加大环保科研投入,降低页岩气开发的环境影响,实现页岩气开发的绿色可持续发展.