超低改造下中国火电排放清单及分布特征

本研究基于2018年火电在线监测和环境统计等数据,自下而上编制了中国高分辨率火电行业排放清单,并核算了排放浓度、排放因子和排放量.结果表明超低排放政策效果显著：2018年火电SO₂、NO_x和烟尘平均排放浓度分别为37.57、56.71和7.41mg ·m^-3.比2015年分别下降58.71%、43.12%和60.79%;中国燃煤机组的SO₂、NO_x和烟尘平均排放因子分别为0.30、0.48和0.06 g ·kg^-1,比2015年分别下降55.2%、36.84%和62.5%;中国火电SO₂、NO_x、烟尘和PM_2.5总排放量分别为72.14、118.38、14.90和13.59万t ·a^-1,比2015年分别下降41.32%、19.29%、48.12%和40.39%.     

超低排放改造后燃煤电厂常规大气污染物排放特征

基于海口电厂"超低排放"燃煤机组在线监测数据和实测结果，研究颗粒物、SO₂、NO_x排放特征，分析颗粒物粒径分布和化学成分谱.结果显示，"超低排放"机组颗粒物、SO₂、NO_x排放浓度均值分别为（1.57±0.81）、（15.15±6.23）和（40.10±3.63）mg·m^-3，均满足超低排放限值要求.TSP、PM₁₀、PM_2.5、PM₁、SO₂、NO_x的排放因子均值分别为0.0099、0.0098、0.0092、0.0065、0.1131、0.2882 kg·t^-1，排放因子集中在很窄的区间内，呈正态或偏正态分布，与未进行超低改造研究结果比较，排放因子减小了1~2个数量级.颗粒物数浓度分布呈双峰分布，数浓度峰值粒径为0.027 μm和0.641 μm；质量浓度呈单峰分布，峰值粒径为1.100 μm.PM₁₀、PM_2.5、PM₁的成分谱差异很小，其主要化学组分为SO₄^2-、Ca、NH₄⁺、NO₃^-、OC，在PM₁₀中质量占比分别为29.41%±0.94%、12.09%±1.95%、9.49%±2.35%、6.96%±0.49%、4.93%±0.57%；在PM_2.5中质量占比分别为29.18%±1.58%、12.72%±1.77%、9.21%±2.01%、5.31%±0.13%、4.33%±0.72%；在PM₁中质量占比分别为29.04%±3.15%、17.99%±3.61%、8.42%±1.50%、4.445±0.08%、5.075±0.07%.     

工业燃煤链条炉细粒子排放特征研究

链条燃煤锅炉是当前我国工业锅炉的最主要应用炉型,其容量占到了工业锅炉总容量的85%,是重要的大气污染物排放源之一.本研究在3个地区选取了5种典型容量的链条炉,应用自行设计的二级稀释系统现场测试其细粒子（PM_2.5）和各种气态污染物的排放特征.结果表明,链条炉烟气中的PM_2.5质量粒径呈单峰或双峰分布,第1个峰值在0.14 μm处,第2个峰值在1 μm后;湿法除尘和旋风除尘对PM_1.0的细粒子仍具有有效的去除效率;在相同或相似除尘控制技术的条件下,PM_2.5的排放水平随锅炉容量的增大而减小.在PM_2.5中,SO^2-₄是最丰富的离子,质量分数在20%～54%范围内;C是最丰富的元素,质量分数在7.5%～31.8%之间,其次是S,质量分数为8.4%～18.7%.采用碳平衡法计算得出PM_2.5、NO_x和SO₂的排放因子分别为0.046～0.486 　g·kg^-1、 1.63～2.47　g·kg^-1、 1.35～9.95　g·kg^-1,这为建立我国的工业锅炉排放清单及大气污染来源分析提供了必要的基础数据.     

湖南省大气污染物排放与人体暴露水平研究

基于吸入因子概念,建立了污染物排放造成的人体暴露的计算方法.应用CALPUFF长距离扩散模型和多元回归分析对湖南省17个电厂(24个排放源)的一次细颗粒(PM_2.5)、SO₂和NO_x排放进行了研究.结果表明,在半径500km范围内,PM_2.5、SO₄^2-和NO₃^-的平均吸入因子分别为9.73×10^-6、2.39×10^-6和2.47×10^-6.回归分析表明,PM_2.5的吸入因子与烟囱高度及人口数量有很高的相关性(R²=0.83),SO₄^2--吸入因子与烟囱高度无关,与人口数量有较好的相关性(R²=0.64),而NO₃的吸入因子与烟囱高度、人口数量的相关性较高(R²=0.74).基于回归方程和人口分布地图,对湖南省污染排放的吸入因子进行区划,得到的吸入因子等值图反映了人口分布对吸入因子的影响,可用于对该地区的排放源造成的健康影响进行快速评价.     

城市机动车排放因子隧道试验研究

选取典型城市隧道进行机动车排放因子测试,应用隧道试验原理,通过连续48h的现场采样监测,获得了隧道内机动车排放污染物NO_x.CO、SO₂、PM₁₀、VOC和HC浓度、交通参数(车型、车速、交通流量)和气象参数(如风速、风量、温度、湿度)等实测数据.通过质量平衡计算出隧道内机动车NO_x.CO、SO₂、PM₁₀和HC的平均排放因子分别为1.379、15.404、0.142、0.637、1.857g·(km·辆)^-1.并在此基础上应用多元回归方法计算出8大类机动车各种排放污染物的单车排放因子.结果反映目前中国城市机动车污染物排放水平及各污染物排放特征.     

典型石化企业排放空气质量影响模拟研究

基于惠州市大亚湾区2017年大气污染源排放清单,利用WRF-CMAQ模型系统量化评估了大亚湾区某典型石化企业在关停和增产排放情景下对周边空气质量的影响.清单结果显示该企业2017年SO₂、NO_x、PM₁₀、PM_2.5、CO和VOCs的排放量分别为212 、1744 、455 、359 、1458 和6446 t,在严格落实等量替代及减排措施后,该石化企业虽然产能翻倍,但VOCs排放量同比2017年显著减少了30%,其它污染物排放量增加了6%~19%.模拟结果显示2017年该石化企业排放对大亚湾区NO₂、PM₁₀、PM_2.5和O₃的浓度贡献分别为0.91、0.64、0.54和-0.08 μg·m^-3,完全关闭该企业排放后对周边站点NO₂改善效果最大（可使邻近管委会子站NO₂浓度下降1.24 μg·m^-3,下降百分比为5.10%）,但由于NO的滴定效应,该企业NO_x减排对周边管委会子站和霞涌子站的O₃浓度均有轻微负贡献;该石化企业的增产改造对周边O₃浓度降低影响明显,周边站点中O₃浓度最高可下降2.45 μg·m^-3（下降幅度为1.72%）,大亚湾区O₃浓度整体也可下降1.45 μg·m^-3.此外,受秋冬季不利扩散条件以及主导上风向污染传输影响,该企业在1月和10月对管委会子站NO₂、PM₁₀和PM_2.5的浓度贡献较大,由于冬季低温导致光化学反应自由基活性降低,该企业在1月对管委会子站O₃浓度负贡献显著.     

成都市冬季3次灰霾污染过程特征及成因分析

基于成都市大气环境超级观测站气态污染物和PM_2.5中组分在线监测数据,对2019~2020年成都市3次灰霾污染过程气象要素和组分特征进行分析,采用CMB模型模拟获得研究期间PM_2.5污染来源及变化趋势,剖析各污染过程成因.结果表明：① 3次污染过程均发生在相对湿度和温度持续上升,风速和边界层高度持续降低的不利气象条件下,日均相对湿度均大于70%,日均温度均大于8℃,日均风速均低于0.8 m ·s^-1,日均边界层高度均低于650 m;② 3次污染过程中主要组分均为NO₃^-、OC、NH₄⁺和SO₄^2-,其中NO₃^-质量浓度和占比污染时段较清洁时段增长倍数均高于其他组分,分别增加了1.47~2.09倍和0.22~0.35倍,NO₃^-是成都市冬季PM_2.5污染的关键组分;③ 3次污染过程SOR均值为0.40,NOR均值为0.27,SO₂和NO_x的二次转化程度较高,SO₂向SO₄^2-转化以夜间非均相氧化反应为主,NO_x向NO₃^-转化以非均相水解反应为主;④ 3次过程变化特征略有不同,过程Ⅰ呈现出明显的二次硝酸盐主导的特征,过程Ⅱ PM_2.5浓度上升过程中主要受燃煤排放影响,PM_2.5浓度高值时段主要受NO₃^-影响,过程Ⅲ总体仍为二次硝酸盐主导的特征,但部分污染时段化石燃料燃烧源排放有所增加;⑤二次硝酸盐、二次硫酸盐、机动车和燃煤源为研究期间主要污染来源,PM_2.5浓度与二次硝酸盐贡献率正相关,与扬尘源贡献率负相关.     

上海市秋季典型大气高污染过程中颗粒物的化学组成变化特征

于2010年10月1日至11月30日在上海市城区对大气中颗粒物质量浓度及细粒子化学组分进行了在线连续观测,获得了秋季大气灰霾和沙尘等典型污染过程中颗粒物质量浓度和化学组成的变化特性.观测结果显示,在大气灰霾污染过程中PM₁₀和PM_2.5的日均最高浓度分别达到216~293 μg·m^-3和130~204 μg·m^-3,PM_2.5/PM₁₀的比值在65%以上,总的可溶性无机离子(TWSII)占PM_2.5质量浓度的50%以上,有机碳(OC)和元素碳(EC)的总和占25%~30%.二次可溶性离子(SO₄^2-, NO₃^-, NH₄⁺)占TWSII的83.3%~87.5%,OC/EC的比值在5左右,表明在灰霾污染过程中二次组分对PM_2.5的贡献较大;沙尘天气以粗粒子污染为主,TWSII、OC和EC分别仅占PM_2.5质量浓度的27.2%、13.4%和2.0%,二次可溶性离子(SO₄^2-, NO₃^-, NH₄⁺)占TWSII的55.7%,Ca²⁺、Mg²⁺等地壳组分的比例较灰霾天气明显升高.研究结果还显示,SO₄^2-和NO₃^-等二次离子组分的生成与颗粒物中硫与氮的氧化速率有关,在大气灰霾过程中硫转化率(SOR)和氮转化率(NOR)值较高,分别为0.24±0.10和0.15±0.06,说明SO₂通过二次反应生成SO₄^2-的能力较强,在污染的环境下高浓度的NO₂更有利于向NO₃^-转化.     

2015—2017年天水市大气污染物变化特征及来源分析

据天水市2015-2017年大气污染物（SO₂、NO₂、CO、O₃、PM_2.5和PM₁₀）的监测数据及气象资料,分析了天水市大气污染物的浓度变化特征,并利用排放源清单和HYSPLIT模型对污染物来源进行了解析.结果表明：①天水市空气质量有所下降,总体优良率达84.9%.SO₂、NO₂、CO均达标,污染物以颗粒物和O₃为主.②一次污染物SO₂、NO₂、CO、PM_2.5和PM₁₀浓度具有相似的季节变化和日变化特征,冬季最高,夏季最低,日变化呈早晚双峰型.二次污染物O₃夏季浓度最高,冬季最低,日变化呈单峰型.③天水市空气质量主要受污染物的本地排放和外来输送的影响,本地民用和工业部门对SO₂、CO、PM_2.5和PM₁₀的贡献最大,交通和工业部门对NO_x的分担率最高,民用部门是CO的最大排放源;西北和东部气流是污染物外来的最主要输送路径.此外,污染物在城市大气中的稀释、扩散和转移也受当地气象因素（气温、降水、风向等）的影响.     

关中盆地NO2和SO2对颗粒物污染的协同效应

基于WRF-Chem模式模拟了关中盆地2019年1月2—14日一次颗粒物污染事件,评估了NO_x和SO₂减排及其在颗粒物污染中的协同作用对PM_2.5污染的影响。敏感性实验结果表明：NO_x减排可使PM_2.5中硝酸盐含量下降,但大气中O₃浓度上升,大气氧化能力增强,其他二次组分上升,导致PM_2.5下降不明显;SO₂人为源减排可使硫酸盐质量浓度下降,但由于硫酸盐在PM_2.5中占比较低,当SO₂减排75%时,PM_2.5仅下降1.74%;当减排比例较高时,NO_x和SO₂同时减排更有利于颗粒物污染防治。PM_2.5质量浓度在NO_x和SO₂同时减排75%时比分开减排75%时多下降0.75%,主要是硫酸盐下降所致;对气溶胶含水量进行分析,发现NO_x对气溶胶含水量影响较大,当NO_x减排75%时,气溶胶含水量可下降15.51%;此外,NO_x和SO₂同时减排比分开减排时气溶胶含水量更低,更不利于二次颗粒物生成。     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

Degradation of metabolites accumulated of benzo[a]pyrene by coupling Penicillium Chrysogenum with KMnO4

Several main metabolites of benzo[a]pyrene （BaP） formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone （BP 1,6- quinone）, trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene （BP 7,8-diol）, 3-hydroxybenzo[a]pyrene （3-OHBP）, were identified by high-performance liquid chromatography （HPLC）. The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that （1） the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; （2） the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; （3） the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% （w/v）, concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.     

Impact of atrazine and nitrogen fertilizers on the sorption of chlorotoluron in soil and model sorbents

Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.     

Distribution and ecological effect of mercury in Laogang landfill, Shanghai, China

Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury （HgT）, combinative mercury （Hgc） and gaseous mercury （HgG）, and content of total organic carbon （TOC）, but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of （HgG,/HgT）1992〉（HgG/HgT）1996〉〉（HgG/HgT）2000. A simple outline of Hg release in landfill could be drawn： with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants （e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum） are capable of enriching more Hg than herbaceous plants.     

EDTA-enhanced phytoremediation of lead contaminated soil by Bidens maximowicziana

Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

Decomposition of alachlor by ozonation and its mechanism

Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.     

Enzymatic oxidation of aqueous pentachlorophenol

The influence of the nonionic surfactant Tween 80 on pentachlorophenol （PCP） oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration （CMC）. Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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