南京大气臭氧浓度的季节变化及其对主要作物影响的评估

近年来,近地面O_3浓度呈不断上升趋势,高浓度O_3会影响作物的生长导致产量降低.本文利用2014~2016年南京市近地面O_3浓度的连续观测数据,分析了O_3浓度的变化特征及其对冬小麦和水稻产量与经济损失的影响.结果表明,2014~2016年南京市O_3年平均浓度分别为62.9、68.6和69.1μg·m-3,O_3浓度和超标日数均呈现逐年增加的趋势.季节平均的O_3浓度大小的顺序为:夏季、春季、秋季和冬季.四季O_3浓度的日变化均为明显的"单峰型",峰值出现在15:00~16:00,谷值出现在07:00~08:00.2014~2016年冬小麦生长季期间AOT40的数值分别为10.5、14.4和9.4μL·L~(-1)·h,水稻生长季期间AOT40的数值分别为8.5、20.0和25.6μL·L~(-1)·h.近地面O_3对冬小麦的影响要高于水稻,其中,2014~2016年O_3造成冬小麦减产范围为21.4%~32.8%,每年的经济损失达15 076.6~27 799.6万元,造成水稻减产范围为8.1%~24.3%,每年的经济损失达19 747.2~68 075.7万元.     

制革废水处理过程中磺胺类抗生素和抗性细菌的分布特征

针对两家制革厂废水处理过程中3种磺胺类抗生素和磺胺类抗性细菌的丰度和分布特性以及两个不同工艺污水处理厂对抗生素的去除规律做了相关研究.结果表明,3种抗生素在两家制革污水处理过程中均有检出,水样中3种抗生素的总质量浓度在59.1~706.7 ng·L~(-1)之间;两家制革厂废水处理剩余污泥中3种抗生素的总含量分别为4 388 ng·kg~(-1)和2 979.4ng·kg~(-1),与市政污水处理厂中的抗生素含量相差不大.不同的污水处理工段对3种抗生素去除效果不同,但去除效率均大于70%.生物处理单元对抗生素的去除率相对较高,而厌氧池是去除抗生素的主要阶段(去除率50%).两个制革厂的进出水和剩余污泥中共筛选出8株抗性细菌,这8个分离菌株可分为5个菌属.进出水中的抗性细菌含量介于9.37×10~3~5.08×10~5CFU·mL~(-1)之间,剩余污泥中的磺胺类抗性细菌含量较高分别为1.17×10`7CFU·g~(-1)和7.2×10~6CFU·g~(-1).两个制革污水处理厂对磺胺甲唑抗性细菌的去除率分别达到了1.34 log和2.15 log.     

聊城冬季一重污染过程PM2.5污染特征及成因分析

北方秋冬季为重污染过程频发季节,为了解聊城市冬季重污染过程中PM_(2.5)及化学组分污染特征,于2016年1月7~11日在聊城市区开展PM_(2.5)样品采集并分析了其中水溶性离子、碳成分及无机金属元素这3种化学组分,并对污染特征及成因进行了分析.结果表明,此次污染过程PM_(2.5)浓度呈现明显的倒V字型,平均浓度为238.3μg·m~(-3),超过国家环境空气质量标准(GB 3095-2012)二级浓度限值2.2倍;NH_4~+、NO_3~-和SO_4~(2-)为PM_(2.5)的主要水溶性离子成分;随污染加重或减轻,NH_4~+、SO_4~(2-)、NO_3~-、Cl-和Mg~(2+)浓度呈现增加或降低趋势,而Ca~(2+)变化趋势与之相反.污染鼎盛时,NH_4~+、NO_3~-和SO_4~(2-)浓度分别为48.96、68.45和80.55μg·m~(-3),达到起始阶段的6.29、7.31和7.84倍;过程期间OC和EC的浓度为20.8~60.2μg·m~(-3)和3.0~7.5μg·m~(-3),OC浓度高于EC且变化幅度明显偏大;过程期间各日无机金属元素浓度和分别为10.2、22.4、16.0、19.6和8.2μg·m~(-3),富集因子(EF)结果显示,各元素EF均小于10,未被富集,表明污染过程中其主要来源于地壳等自然源;PM_(2.5)质量浓度重构结果表明,有机物(OM)、SO_4~(2-)和NO_3~-为PM_(2.5)的主要组分,其次为NH_4~+、地壳物质和其他离子,EC和微量元素含量相对较低.随着PM_(2.5)污染加重,二次无机盐(SO_4~(2-)、NO_3~-及NH_4~+)浓度及所占比例均随之增加,OM浓度随之增加但比例有所下降,而地壳物质浓度及比例均下降,表明二次无机转化是此次污染过程的主要原因,主要受燃煤和机动车排放影响.     

基于稳定碳同位素技术的干旱区绿洲土壤有机碳向无机碳的转移

应用稳定碳同位素技术测定土壤无机碳稳定碳同位素组成(soil inorganic carbonδ13C,SICδ13C),并对干旱区绿洲土壤无机碳进行区分,结合土壤有机碳(soil organic carbon,SOC)与SIC含量关系进一步探讨SOC向SIC转移的碳量.结果表明,4种类型土壤SICδ13C值差异性极显著(P0.01),风沙土SICδ13C值最高且为正,均值为(0.32±0.04)‰,随土层深度增加而增加,说明风沙土原生性碳酸盐占绝对优势;灌漠土、棕漠土和盐碱土SIC的δ13C均值分别(-0.30±0.24)‰、(-1.96±0.66)‰和(-1.24±0.49)‰,随土层变化均呈先降低后逐渐增大的趋势,说明灌漠土原生性碳酸盐占优势,棕漠土和盐碱土发生性碳酸盐相对前者占优势.风沙土、灌漠土、棕漠土和盐碱土的发生性碳酸盐占SIC比例均值分别为1.33%、4.72%、15.01%、35.71%,均小于50%,说明干旱区绿洲土壤发生性碳酸盐比例总体水平较低.风沙土、灌漠土、棕漠土和盐碱土在土壤发生性碳酸盐形成或重结晶过程中固定土壤CO2的量分别为0.30、2.44、4.96、12.40 g·kg~(-1),其中固定来自大气CO2量平均为0.18、0.79、1.45、8.67 g·kg~(-1),来自SOC氧化分解转化为CO2的量分别为0.06、0.83、1.62、1.86g·kg~(-1),说明盐碱土、棕漠土SOC的贡献相对较高,灌漠土、风沙土较低;对土壤固定CO2量的来源比较发现,风沙土、盐碱土固定土壤CO2的量来自大气CO2量较高,SOC的贡献较低,而灌漠土、棕漠土固定来自SOC氧化分解CO2的量较高,大气贡献较低.研究区整体SOC向SIC的碳转移量介于0.03~2.38 g·kg~(-1)之间,平均每千克土壤固定1.09 g的CO2,说明干旱区绿洲土壤发生性碳酸盐所占比例较低,SOC的贡献较少.     

塔里木盆地北缘绿洲不同连作年限棉田土壤有机碳、无机碳含量与环境因子的相关性

农田土壤碳库是土壤碳库的重要组成部分,易受人类活动调节且固碳减排潜力巨大,研究土壤有机碳、无机碳含量特征及其与环境因子的关系有助于深入理解土壤生态过程,为全球碳收支平衡研究提供理论支持.本文以塔里木盆地北缘绿洲为靶区,分析土壤碳库特征,结合冗余分析、通径分析,探究土壤有机碳、无机碳含量及其与环境因子的相关关系.结果表明:(1)同一土层不同连作年限棉田土壤有机碳、无机碳含量存在显著差异(P0.05),随连作年限增加,有机碳含量呈先增加后减少趋势,而无机碳含量呈先减少后增加趋势;同一连作年限棉田不同土层土壤有机碳、无机碳含量存在显著差异(P0.05),有机碳含量均在0~20 cm层达到最大值,而无机碳含量均在20~50 cm层达到最大值.(2)通过冗余分析得出环境因子对土壤碳库特征影响的重要性排序为:磷酸酶活性p H值蔗糖酶活性过氧化氢酶活性全氮速效磷速效钾土壤含水量脲酶活性电导率;磷酸酶活性、p H值、蔗糖酶活性、过氧化氢酶活性、全氮、速效磷、速效钾与土壤有机碳、无机碳含量呈极显著相关关系(P0.01);土壤含水量、脲酶活性与土壤有机碳、无机碳含量表现为显著相关(P0.05).(3)通径分析表明,速效钾对有机碳含量直接作用显著,是影响有机碳含量的主要因素,而脲酶活性对无机碳含量直接作用显著,是影响无机碳含量的主要因素.干旱半干旱区土壤有机碳、无机碳含量研究是评价农田生态系统土壤碳的"源/汇"效应的基础数据,对研究全球碳收支平衡和陆地碳循环机制具有重要意义.     

长期侧流提取对EBPR系统除磷及其磷回收性能的影响

实验采用交替厌氧/好氧(An/O)运行模式的SBR反应器,考察310 d内分3个批次提取侧流比为0、1/4、1/3、1/2的厌氧放磷上清液后EBPR系统的脱氮除磷效果及相应的磷回收性能.结果表明,整个实验阶段系统对COD和氨氮的去除较为稳定,出水均能满足《城镇污水处理厂污染物综合排放标准》一级A标准,总氮去除因厌氧阶段反硝化不断增强有所提升,达标率由88.2%显著上升至98.6%.然而,随着厌氧上清液提取次数的增多,系统释磷能力整体下降,但前两个批次中系统除磷均稳定高效,去除率在90%以上,相应地出水磷达标率大于75%,仅第3批次实验中侧流比为1/2时系统除磷率出现大幅波动,最低降为54.2%,并贡献该批次出水磷不达标率的60%,说明长期提取1/2侧流比不利于主流工艺出水稳定维持.研究还发现,长期进行侧流磷回收实验有利于污泥减量,且对污泥沉降性能影响不大.因此,在EBPR系统内长期提取适当侧流比的厌氧上清液以进行磷回收与主流工艺同步高效脱氮除磷具有可行性.     

Carbonaceous and nitrogenous disinfection byproduct precursor variation during the reversed anaerobic–anoxic–oxic process of a sewage treatment plant

Disinfection byproduct(DBP)precursors in wastewater during the reversed anaerobic–anoxic–oxic(A~2/O)process,as well as their molecular weight(MW)and polarity-based fractions,were characterized with UV scanning,fluorescence excitation emission matrix,Fourier transform infrared and nuclear magnetic resonance spectroscopy.Their DBP formation potentials(DBPFPs)after chlorination were further tested.Results indicated that the reversed A~2/O process could not only effectively remove the dissolved organic carbon(DOC)and dissolved total nitrogen in the wastewater,but also affect the MW distribution and hydrophilic–hydrophobic properties of dissolved organic matter(DOM).The accumulation of low MW and hydrophobic(HPO)DOM was possibly due to the formation of soluble microbial product-like(SMP-like)matters in the reversed A~2/O treatment,especially in the anoxic and aerobic processes.Moreover,DOM in the wastewater displayed a high carbonaceous disinfection byproduct formation potential(C-DBPFP)in the fractions of MW100 k Da and MW5 k Da,and revealed an increasing tendency of nitrogenous disinfection byproduct formation potential(N-DBPFP)with decrease of MW.For polarity-based fractions,the HPO fraction of wastewater showed significantly higher C-DBPFP and N-DBPFP than hydrophilic and transphilic fractions.Therefore,although the reversed A~2/O process could remove most DBP precursors by DOC reduction,it led to the enhancement of DBPFP with the formation and accumulation of low MW and HPO DOM.In addition,strong correlations between C-DBPFPs and SUVA,and between N-DBPFPs and DON/DOC,were observed in the wastewater,which might be helpful for DBPFP prediction in wastewater and reclaimed water chlorination.     

Concurrent catalytic removal of typical volatile organic compound mixtures over Au-Pd/α-MnO2 nanotubes

α-MnO_2 nanotubes and their supported Au-Pd alloy nanocatalysts were prepared using hydrothermal and polyvinyl alcohol-protected reduction methods, respectively. Their catalytic activity for the oxidation of toluene/m-xylene, acetone/ethyl acetate, acetone/m-xylene and ethyl acetate/m-xylene mixtures was evaluated. It was found that the interaction between Au-Pd alloy nanoparticles and α-MnO_2 nanotubes significantly improved the reactivity of lattice oxygen, and the 0.91 wt.% Au0.48 Pd/α-MnO_2 nanotube catalyst outperformed the α-MnO_2 nanotube catalyst in the oxidation of toluene, m-xylene, ethyl acetate and acetone. Over the0.91 wt.% Au0.48 Pd/α-MnO_2 nanotube catalyst,(i) toluene oxidation was greatly inhibited in the toluene/m-xylene mixture, while m-xylene oxidation was not influenced;(ii) acetone and ethyl acetate oxidation suffered a minor impact in the acetone/ethyl acetate mixture; and(iii) m-xylene oxidation was enhanced whereas the oxidation of the oxygenated VOCs(volatile organic compounds) was suppressed in the acetone/m-xylene or ethyl acetate/m-xylene mixtures. The competitive adsorption of these typical VOCs on the catalyst surface induced an inhibitive effect on their oxidation, and increasing the temperature favored the oxidation of the VOCs. The mixed VOCs could be completely oxidized into CO_2 and H_2 O below 320°C at a space velocity of 40,000 m L/(g·hr). The 0.91 wt.% Au0.48 Pd/α-MnO_2 nanotube catalyst exhibited high catalytic stability as well as good tolerance to water vapor and CO_2 in the oxidation of the VOC mixtures. Thus, the α-MnO_2 nanotube-supported noble metal alloy catalysts hold promise for the efficient elimination of VOC mixtures.     

Insights into the formation of secondary organic carbon in the summertime in urban Shanghai

To investigate formation mechanisms of secondary organic carbon(SOC) in Eastern China,measurements were conducted in an urban site in Shanghai in the summer of 2015. A period of high O_3 concentrations(daily peak 120 ppb) was observed, during which daily maximum SOC concentrations exceeding 9.0 μg/(C·m~3). Diurnal variations of SOC concentration and SOC/organic carbon(OC) ratio exhibited both daytime and nighttime peaks. The SOC concentrations correlated well with O_x(= O_3+ NO_2) and relative humidity in the daytime and nighttime, respectively, suggesting that secondary organic aerosol formation in Shanghai is driven by both photochemical production and aqueous phase reactions. Single particle mass spectrometry was used to examine the formation pathways of SOC. Along with the daytime increase of SOC, the number fraction of elemental carbon(EC) particles coated with OC quickly increased from 38.1% to 61.9% in the size range of 250–2000 nm, which was likely due to gas-to-particle partitioning of photochemically generated semi-volatile organic compounds onto EC particles. In the nighttime, particles rich in OC components were highly hygroscopic, and number fraction of these particles correlated well with relative humidity and SOC/OC nocturnal peaks. Meanwhile, as an aqueous-phase SOC tracer, particles that contained oxalate-Fe(III) complex also peaked at night. These observations suggested that aqueous-phase processes had an important contribution to the SOC nighttime formation. The influence of aerosol acidity on SOC formation was studied by both bulk and single particle level measurements, suggesting that the aqueous-phase formation of SOC was enhanced by particle acidity.