基于机器学习的郑州市大气PM2.5与O3浓度预测方法及气象因子的影响分析

近年来,我国面临着细颗粒物(PM_2.5)污染形势依然严峻以及臭氧(O₃)污染日益凸显的双重压力.为进一步准确预测郑州市大气PM_2.5与O₃浓度并探明气象因子的影响,本研究使用2018-2022年郑州市大气污染物和气象因子逐时数据,结合统计学单因素分析和机器学习LightGBM模型多因素分析,建立了一种基于长时间序列数据的PM_2.5与O₃浓度预测及气象因子影响分析的综合分析方法.结果表明：(1)训练后的LightGBM模型能够较好地预测PM_2.5污染,准确率达80.8%;对O₃污染预测的准确率为52.5%.(2)郑州市大气PM_2.5浓度与气压呈正相关,与比湿和环境温度均呈负相关;大气O₃ 8 h滑动平均浓度(O₃-8 h浓度)与比湿和太阳辐射均呈正相关,与气压呈负相关.(3)有利的气象条件可能是2021年PM_2.5年均浓度得到显...     

京津冀臭氧变化特征及与气象要素的关系

基于2014~2017年京津冀13座城市的O₃-8h数据,分析O₃时间变化特征及污染状况.在此基础上,结合同期气象数据研究近地层O₃浓度与气象要素的关系.结果表明：2014~2017年京津冀区域O₃-8h整体呈上升趋势,增长率为4.50μg/m³.区域内O₃污染整体加重,北京、保定O₃污染较为严重;2014~2015年O₃浓度与超标情况的月变化主要呈单峰型变化,峰值出现在5月;而2016~2017年为不规则双峰型变化,峰值出现在5~6月和9月.与气象因子的相关性表明：气象要素对O₃的影响具有明显的季节差异,其中春、夏、秋季气温是影响O₃浓度变化的主要因素,而在冬季相对湿度与风速为影响O₃浓度变化的主要因素.此外,分析表明北京、天津、石家庄3大城市夏季形成高浓度O₃的阈值明显不同.     

珠江三角洲秋季典型O3污染的气象条件及贡献量化

利用自组织神经网络分析法,对珠江三角洲2013~2017年秋季海平面气压和全风速场进行大样本客观分型.结果表明,影响O₃的天气类型共有7种,由污染程度高低分为高、中、低3类,对应的平均O₃超标率分别为32.3%, 12.0%和4.2%.对比2017年和2016年秋季O₃污染天气分型下促发O₃污染的气象因子差异,2017年秋季高污染型O₃天气形势出现的天数比2016年增多,且中污染型天气形势出现时,2017年的局地污染气象条件更为不利.采用WRF-CAMx模式通过改变气象场输入来量化气象条件贡献,并用实测变化减去气象变化以推算排放贡献.结果表明,气象条件变化导致O₃浓度上升的贡献率为29.8%,而排放的变化引起O₃浓度下降的贡献率为7.1%.在2017年秋季开展的O₃污染防治专项行动指导下的珠江三角洲O₃前体物控制措施,有效缓解了部分由于不利气象条件而引起的O₃污染浓度上升.不利气象条件是导致2017年秋季O₃浓度升高的重要成因.     

不同时间尺度气象要素与空气污染关系的KZ滤波研究

空气污染状况受气象要素和污染源排放的共同影响,为了评估大气污染控制措施的效果,需将由污染源排放的浓度数据分离出来.本文利用KZ滤波方法将天津市6个监测站点2015~2017年逐日的O₃、PM_2.5和PM₁₀浓度资料和6个同期气象数据分解为长期分量、短期分量和季节分量,计算各分量对原始时间序列方差的贡献.采用逐步回归法建立O₃及颗粒物3种分量与相应尺度气象要素的线性模型.结果表明,上述3种污染物浓度数据经分解后,季节分量对总方差贡献最大,其次为短期分量;气温和相对湿度是影响O₃季节和短期分量的主要气象因素,其中温度占主导地位,且呈现正相关,与相对湿度呈负相关;风速、气压、降水与颗粒物的短期及季节浓度变化呈负相关,相对湿度与之呈正相关,温度与短期分量呈正相关、与季节分量的变化呈负相关;经逐步回归消除气象影响的PM₁₀的长期分量有波动下降的趋势,PM_2.5浓度在2017年年初有所上升,其余部分有下降趋势,O₃长期分量浓度有所上升;这几年间颗粒物污染控制措施的效果较为显著,O₃污染有所加重.     

城市臭氧污染特征与高影响气象因子：以苏州为例

近年来城市臭氧(O₃)污染问题日益突出,影响O₃污染的关键气象因子尚不明确,因此分析典型城市——苏州的O₃污染特征,探究O₃污染的高影响气象因子,对该区域大气污染防治具有重要意义.基于苏州环境监测中心2015～2020年4～9月逐小时O₃浓度数据及同期气象观测资料,应用相关分析和机器学习方法对其开展相关分析研究.结果表明：(1) 6年间O₃污染高发季,O₃污染超标率均达20%以上,O₃污染日数和以O₃为首要污染物的污染日数占比均逐年上升,O₃污染问题日益凸显;(2) O₃浓度存在单峰日变化特点,谷值出现在07:00前后,峰值出现在15:00～16:00;其与气温和太阳辐射能的日内变化趋势较一致,但其浓度峰值出现时刻又滞后于二者. 2017年和2019年O₃有典型的“周末效应”,周末较高的太阳辐照度对O₃浓...     

基于广义相加模型的北京市2018—2022年地面臭氧气象影响要素研究

臭氧污染是制约北京市环境空气质量持续改善的关键因子,气象是导致臭氧浓度超过国家标准的重要因素,探究气象要素与臭氧浓度之间的关系,对有效治理臭氧污染具有重要意义.本文分析了2018—2022年北京市地面臭氧浓度的演变特征,并利用气象要素和臭氧日最大8 h滑动平均浓度(O₃-8 h)观测数据,基于广义相加模型和合成少数过采样技术,构建了适用于北京的臭氧非线性回归预测模型,识别了影响北京市O₃-8 h浓度日际变化气象因子的重要程度.结果显示：(1)近5年北京市臭氧浓度仍处于高位波动阶段,5—9月是臭氧浓度超标最严重的时期.(2)回归模型对高浓度臭氧具有良好的预测能力,其对北京市5—9月O₃-8 h浓度变化的方差解释率为83.3%.(3)基于回归模型发现,日最高气温、风向、紫外辐射强度、相对湿度、风速、地表平均气压与O₃-8 h浓度之间均有显著的非线性关系,其中,日最高气温、风向和紫外辐射强度为主导O₃-8 h浓度变化的气象要素.在高温、主导风向为偏南风、紫外辐射强度较强的气象条件下,...     

山东省环境空气中PM2.5与O3的复合污染特征与时空变化趋势

山东省PM_2.5-O₃复合污染特征突出,空间差异性明显,本文基于2016—2020年国控和省控环境空气自动监测站监测数据以及同期各气象代表站气象监测数据,分析PM_2.5和O₃时空分布的变化特征,初步探究其与气象因子及前体物的关系. 结果表明:①2016—2020年山东省空气质量逐步改善,优良天数比例上升了7.1%,重污染天数比例下降了3.5%. 除O₃年评价值上升9.6%以外,SO₂、PM₁₀、PM_2.5、CO和NO₂的浓度均下降,降幅依次为61.3%、29.8%、28.6%、26.3%和11.4%. 各市PM_2.5年评价值均下降(范围为18.4%~34.9%);除德州市外,其他15市O₃年评价值均上升,滨州市的升幅(30.8%)最大. 1月PM_2.5平均浓度最高,呈现先下降后上升的年变化趋势,6月O₃平均浓度最高,且逐年上升. ②山东省PM_2.5和O₃均呈现内陆地区高于沿海地区的分布特征,PM_2.5浓度在西部内陆地区较高,O₃浓度在中北部内陆地区较高,PM_2.5-O₃复合污染特征在中西部地区较明显. 统计期间共计出现PM_2.5-O₃复合污染日224 d,分布在2—11月,出现天数逐年减少. ③为探究PM_2.5-O₃复合污染的影响因素及气象特征,进行相关性分析及气象因子阈值筛查,结果表明,PM_2.5日均浓度和O₃_8 h (臭氧日最大8小时滑动平均值)与其主要前体物和气象因子均呈现相反的相关关系,且对不同因子的响应有一定区域性差异. 当气温为14.9~24.1 ℃、相对湿度为55.5%~75.1%、风速为0.6~2.9 m/s、气压为992.8~1 018.8 hPa时PM_2.5-O₃复合污染易于发生,该条件下大部分城市的气温、相对湿度和气压平均值介于PM_2.5和O₃污染单独发生时的对应因子平均值,但平均风速小于PM_2.5和O₃污染单独发生的平均风速. 研究显示,“十三五”期间山东省PM_2.5浓度波动下降,O₃浓度波动上升,二者的协同关系日趋明显,气象因素对PM_2.5和O₃的生成和累积有一定影响.      

深圳臭氧污染的环境气象特征分析

基于2015—2020年深圳污染物浓度监测资料、自动气象站资料以及再分析格点资料,分析了对深圳O₃浓度有显著影响的环境气象特征.结果表明：(1)深圳O₃的月均浓度变化规律与其他主要污染物不同,O₃月均浓度的峰值出现在10月,恰好是夏季风向冬季风转换的季节.(2)从地面气象要素来看,深圳O₃的浓度与气温及相对湿度的关系最为密切,当气温大于29℃的时候,开始出现O₃浓度超标的情况,当气温大于32℃时O₃的浓度和超标率均大幅增加.当相对湿度为40%～55%时,O₃浓度超标率以及O₃浓度均值达到最高.(3)后向轨迹统计分析表明,易导致深圳出现O₃污染的气流路径主要有3条,分别是东北福建路径、东北江西路径和西北粤西北路径,全部来自偏北的内陆地区.而对深圳O₃污染存在影响的潜在源区多位于深圳的东北部和北部.(4)气流的垂直运动对深圳O₃污染有着显著影响.污染日...     

海陆风对宁波东南滨海郊区大气臭氧变化特征及预测的影响

当前我国沿海发达城市群大气臭氧(O₃)污染严重,且污染的发生和发展受沿海气象条件影响明显.作为海岸附近典型的大气环流,海陆风对沿海地区大气污染物的生成和消散具有重要潜在贡献.本研究基于对2020年1月—2022年3月宁波沿海地区近地面空气质量和气象因子的连续监测,分析了海陆风对我国典型沿海城市大气O₃浓度及其时间变化的影响.同时,在区分有、无海陆风的不同情景下,利用线性回归和随机森林模型对O₃浓度进行了模拟预测.结果表明,海陆风可显著促进沿海地区大气O₃浓度的升高和污染事件的发生,海陆风日的O₃浓度明显高于无海陆风日.与无海陆风发生时段相比,春、夏、秋、冬四季海陆风发生时段的O₃超标率分别升高了19%、18%、38%和6%.海陆风天气下近地面大气相对静稳,污染物的局地循环和积聚是O₃浓度升高的主要原因.随机森林模型对O₃浓度的拟合效果明显优于线性回归模型,且全参数(气象因子和污染物)模型优于气象参数模型.在区分海...     

2015—2020年中国臭氧污染时空演化及其与厄尔尼诺-南方涛动的关系研究

为研究2015—2020年我国近地面臭氧(O₃)污染时空演化特征以及厄尔尼诺-南方涛动(ENSO)对我国O₃污染的影响,本文基于2015—2020年我国近1 500个监测站点的O₃浓度数据(不包括港澳台地区数据),综合运用空间自相关、热点分析、异常值分析及回归分析,研究2015—2020年我国O₃污染的时空演化、浓度异常特征及其与ENSO事件和气象因素的关系.结果表明：(1)2015—2019年我国O₃污染集聚效应不断增强,但2020年显著降低.(2)我国O₃浓度呈先升高(2015—2018年)后下降(2018—2020年)的特征,2017年、2018年O₃年均浓度分别较上一年升高8.72%、1.76%,2019年、2020年O₃年均浓度分别较上一年下降3.60%、3.66%.除2019年、2020年外,O₃浓度高值聚集区站点的O₃浓度峰值和高值天数(日均值大于120μ...     

Effects of two sludge application on fractionation and phytotoxicity of zinc and copper in the soil

The potential harm of heavy metals is a primary concern in application of sludge to the agricultural land. A pot experiment was conducted to evaluate the effect of two sludges on fractionation of Zn and Cu in soil and their phytotoxicity to pakchoi. The loamy soil was mixed with 0%, 20%, 40%, 60% and 80% (by weight) of digested sewage sludge (SS) and composted sludge (SC). The additions of both sludges caused a significant raise in all fractions, resulting in that exchangeable (EXCH) and organic bound (OM) became predominance of Zn and organic bound Cu occupied the largest portion. There was more available amount of Zn and Cu in SS treatments than SC treatments. During the pot experiment, the concentration of Zn in EXCH, carbonate (CAR) and OM and Cu in EXCH and OM fractions decreased in all treatments, so their bioavailability reduced. Germination rate and plant biomass decreased when the addition rate was high and the best yield appeared in 20% mixtures at the harvest of pakchoi. The two sludges increased tissue contents of Zn and Cu especially in the SS treatments. Zn in pakchoi was not only in relationship to ΔEXCH and ΔCAR forms but also in ΔOM forms in the sludge-soil mixtures. Tissue content of Cu in pakchoi grown on SC-soils could not be predicted by ΔEXCH. These correlation rates between Zn and Cu accumulation in pakchoi and variation of different fractions increased with time, which might indicate that sludges represented stronger impacts on the plant in long-term land application.     

Intraspecific differences in effects of co-contamination of cadmium and

A hydroponic experiment was carried out to study intraspecific differences in the effects of different concentrations of cadmium (Cd)(0-10 mg/L) and arsenate (As(V)) (0-8 mg/L) on the growth parameters and accumulation of Cd and As in six wheat varieties Jing-9428, Duokang-1, Jingdong-11, Jing-411, Jingdong-8 and Zhongmai-8. The endpoints of wheat seedlings, including seed germination,biomass, root length and shoot height, decreased with increasing the Cd and As concentrations. Significant differences in seed germination, biomass, root length, shoot height and the accumulation of Cd and As were observed between the treatments and among the varieties (p ＜ 0.05). The lethal dosage 50% were about 20, 80, 60, 60, 80 and 20 mg As/L for Jing-9428, Duokang-1, Jingdong-11,Jing-411, Jingdong-8 and Zhongmai-8, respectively, and the corresponding values for Cd were about 30, 80, 20, 40, 60 and 10 mg Cd/L, respectively. Among the six varieties, Duokang-1 was found to be the most resistant to Cd and As toxicity, and Zhongmai-8 was the most sensitive to Cd and As co-contamination. The resistance of the six varieties was found dependant on the seedling uptake of Cd and As. Duokang-1 was the most suitable for cultivation in Cd and As co-contaminated soils.     

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.     

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.     

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.     

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.     

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.     

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.     

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.