祁连山东端地表及地下水水化学时空变化特征

于2016~2017年5~9月采集祁连山东端（乌鞘岭、古浪、天祝）的地表水和地下水样品进行水化学分析,综合运用统计分析、Piper三线图、Gibbs图以及离子比值等方法探究了祁连山东端地表水和地下水主要离子组成特征、来源以及时空变化.结果表明,祁连山东端地表水和地下水化学组成中优势阳离子为Ca²⁺和Na⁺,Ca²⁺的平均浓度为76.897mg/L,占比73.89%;Na⁺的浓度为16.592mg/L,占比15.94%.优势阴离子为HCO₃^-和SO₄^2-,HCO₃^-浓度190.117mg/L,占比68.71%;其次是SO₄^2-,平均值为67.565mg/L,占比为24.42%.乌鞘岭河水、地下水,天祝河水、地下水的水化学类型为HCO₃^--Ca²⁺型,古浪河水、地下水水化学类型为HCO₃^--Ca²⁺-Mg²⁺型,处于水化学易变区.不同水体离子来源于岩石风化,主要受碳酸盐与硅酸盐风化溶解共同作用控制,人类活动在一定程度上贡献了水体的离子来源.不同水体主要离子浓度的时间变化特征各不相同,整体上大部分水体的离子浓度随时间变化不明显,总体趋势较平缓.     

Spatial Convergence in Major Dissolved Ion Concentrations and Implications of Headwater Mining for Downstream Water Quality

Spatial patterns in major dissolved solute concentrations were examined to better understand impact of surface coal mining in headwaters on downstream water chemistry. Sixty sites were sampled seasonally from 2012 to 2014 in an eastern Kentucky watershed. Watershed areas (WA) ranged from 1.6 to 400.5 km² and were mostly forested (58%–95%), but some drained as much as 31% surface mining. Measures of total dissolved solutes and most component ions were positively correlated with mining. Analytes showed strong convergent spatial patterns with high variability in headwaters (<15 km² WA) that stabilized downstream (WA > 75 km²), indicating hydrologic mixing primarily controls downstream values. Mean headwater solute concentrations were a good predictor of downstream values, with % differences ranging from 0.55% (Na⁺) to 28.78% (Mg²⁺). In a mined scenario where all headwaters had impacts, downstream solute concentrations roughly doubled. Alternatively, if mining impacts to headwaters were minimized, downstream solute concentrations better approximated the 300 μS/cm conductivity criterion deemed protective of aquatic life. Temporal variability also had convergent spatial patterns and mined streams were less variable due to unnaturally stable hydrology. The highly conserved nature of dissolved solutes from mining activities and lack of viable treatment options suggest forested, unmined watersheds would provide dilution that would be protective of downstream aquatic life.     

Toward Explaining Nitrogen and Phosphorus Trends in Chesapeake Bay Tributaries, 1992–2012

Understanding trends in stream chemistry is critical to watershed management, and often complicated by multiple contaminant sources and landscape conditions changing over varying time scales. We adapted spatially referenced regression (SPARROW) to infer causes of recent nutrient trends in Chesapeake Bay tributaries by relating observed fluxes during 1992, 2002, and 2012 to contemporary inputs and watershed conditions. The annual flow‐normalized nitrogen flux to the bay from its watershed declined by 14% to 127,000 Mg (metric tons) between 1992 and 2012, due primarily (more than 80% of the decline) to reduced point sources. The remainder of the decline was due to reduced atmospheric deposition (13%) and urban nonpoint sources. Agricultural inputs, which contribute most nitrogen to the bay, changed little, although trends in the average nitrogen yield (flux per unit area) from cropland and pasture to streams in some settings suggest possible effects of evolving nutrient applications or other land management practices. Point sources of phosphorus to local streams declined by half between 1992 and 2012, while nonpoint inputs were relatively unchanged. Annual phosphorus delivery to the bay increased by 9% to 9,570 Mg between 1992 and 2012, however, due mainly to reduced retention in the Susquehanna River at Conowingo Reservoir.     

Methylated and thiolated arsenic species for environmental and health research——A review on synthesis and characterization

Hundreds of millions of people around the world are exposed to elevated concentrations of inorganic and organic arsenic compounds, increasing the risk of a wide range of health effects. Studies of the environmental fate and human health effects of arsenic require authentic arsenic compounds. We summarize here the synthesis and characterization of more than a dozen methylated and thiolated arsenic compounds that are not commercially available. We discuss the methods of synthesis for the following14 trivalent(Ⅲ) and pentavalent() arsenic compounds: monomethylarsonous acid(MMA~Ⅲ), dicysteinylmethyldithioarsenite(MMA~Ⅲ(Cys)_2), monomethylarsonic acid(MMA~Ⅴ),monomethylmonothioarsonic acid(MMMTAⅤ) or monothio-MMA~Ⅴ, monomethyldithioarsonic acid(MMDTA~Ⅴ) or dithio-MMA~Ⅴ, monomethyltrithioarsonate(MMTTA~Ⅴ) or trithio-MMA~Ⅴ,dimethylarsinous acid(DMA~Ⅲ), dimethylarsino-glutathione(DMA~Ⅲ(SG)), dimethylarsinic acid(DMA~Ⅴ), dimethylmonothioarsinic acid(DMMTA~Ⅴ) or monothio-DMAⅤ, dimethyldithioarsinic acid(DMDTA~Ⅴ) or dithio-DMA~Ⅴ, trimethylarsine oxide(TMAO~Ⅴ), arsenobetaine(AsB), and an arsenicin-A model compound. We have reviewed and compared the available methods,synthesized the arsenic compounds in our laboratories, and provided characterization information. On the basis of reaction yield, ease of synthesis and purification of product, safety considerations, and our experience, we recommend a method for the synthesis of each of these arsenic compounds.     

基于调查的中国秸秆露天焚烧污染物排放清单

基于2010年初农村能源消费情况的问卷调查,获得全国分省秸秆露天焚烧比例,在此基础上确定秸秆露天焚烧的活动水平,采用排放因子法建立中国秸秆露天焚烧的污染物排放清单. 结果表明,中国农村秸秆露天焚烧平均比例为20.8%. 2009年全国28个省区(不包括西藏自治区、天津市、上海市、港澳台地区,下同)秸秆露天焚烧的PM_2.5、BC、OC、SO₂、NO_x、CO、NMVOC、NH₃、CH₄和CO₂排放量分别138.1×104、6.4×104、41.1×104、8.7×104、41.8×104、594.6×104、94.4×104、8.0×104、44.2×104和14 355.4×104 t. 稻谷、玉米和小麦是露天焚烧的三大作物秸秆,其对污染物排放的贡献合计约为87%. 秸秆露天焚烧排放量最高的前3位分别为湖南省、河南省和安徽省, 秸秆露天焚烧比例分别43.1%、20.8%和39.7%. 污染排放的高值区主要集中在华北和华中地区. 95%置信区间下的不确定性分析结果显示,PM_2.5、BC、OC、SO₂、NO_x、CO和NMVOC排放的不确定性范围分别为-60%~83%、-78%~147%、-73%~135%、-48%~75%、-49%~78%、-91%~155%和-67%~94%. 2015年初对六省(湖南省、广东省、江苏省、河南省、黑龙江省和辽宁省)农村能源消费调查的结果显示,2014年江苏省、湖南省和广东省的秸秆露天焚烧比例较2009年均有下降,而辽宁省、黑龙江省和河南省则相对上升. 研究显示,秸秆禁烧政策已取得初步成效,建议国家有关部门进一步加大秸秆禁烧政策的推行力度,完善相关政策措施.      

大气汞均相和非均相化学反应过程研究进展

作为环境中汞传输的最重要通道,大气在汞的全球生物地球化学循环和传输扩散中起着极其关键的作用.大气环境成分复杂,汞在随大气环境传递过程中会经历复杂的化学反应,并导致不同形态之间相互转化,这也成为影响大气汞远距离传输尺度的关键因素.本文主要对大气汞在不同相界面之间的分配过程和主要影响因素(包括相界面的物理化学性质和外部环境条件等)进行了总结;对大气Hg0主要氧化反应过程(卤族元素氧化和O_3、OH·氧化)进行了阐述;对大气Hg~(2+)还原反应过程,尤其是光致还原反应等进行了梳理.如何综合运用野外监测分析和室内模拟等,利用微观分子表面分析等新技术明确大气汞均相、非均相反应过程,并将反应机理与大气汞传输过程模拟系统融合,将是未来大气汞研究的重要内容之一.     

基于ANFIS改进的大气腐蚀环境缺失数据填补方法

目的针对大气腐蚀中重要环境数据缺失的复杂问题,提出一种相关因素(Relevance Factors)和自适应神经模糊推理系统(Adaptive Neuro-Fuzzy Inference System)结合的方法(RF-ANFIS)对缺失数据进行填补。方法首先采用相关因素方法计算缺失数据和多项环境因素间的相关程度,筛选出相关系数较大的因子,然后应用ANFIS构建缺失数据与所选环境因子的关系模型。最后以二氧化硫数据为具体对象,采用北京2015年的气象数据对所建立的模型进行检验。结果经过改进的RF-ANFIS模型在最优情况下样本均方误差为0.696,在14个测试样本中有13个相对误差在20%以内,针对有限样本的数据分析中更为适用。结论该方法有效提高了大气腐蚀环境数据缺失的填补精度,对在数据缺失情况下预测大气腐蚀速率具有重要意义。     

固体颗粒沉积对7B04 铝合金初期大气腐蚀行为的影响

目的研究Na Cl,C,Si O2三种固体颗粒对7B04铝合金初期大气腐蚀行为的影响。方法通过对三种固体颗粒沉积试样进行户内暴露试验,结合质量增量测试、腐蚀形貌观察、微区电化学测试等手段研究7B04铝合金在不同固体颗粒沉积下的初期腐蚀行为。结果经过不同周期暴露试验后,Na Cl与Si O2颗粒沉积7B04铝合金在腐蚀初期即有点蚀萌生,且腐蚀质量增量随暴露时间呈上升趋势;C颗粒沉积7B04铝合金在暴露后期出现少量点蚀,无明显腐蚀质量增量。三种颗粒沉积后7B04铝合金表面电位呈不均匀分布,并随暴露时间的增加,电位分布发生了变化。结论在25℃,RH为95%条件下,Na Cl与Si O2颗粒沉积均可诱发7B04铝合金的大气腐蚀,而C颗粒沉积则无诱发作用。     

长沙市大气中总挥发性有机物分布特征、变化规律及污染对策研究

为调查长沙市大气中TVOC的分布特征及变化规律,研究其污染控制措施,按照相关标准和技术规范,在不同的功能区划和行政区划内合理布设12个监测点位,分季节采集样品,使用热脱附－气相色谱法进行检测,利用反距离权重插值和遥感解译等方法进行综合分析。结果表明：长沙市大气中苯与甲苯（ B／T）特征比值为0．58,汽车尾气是长沙市苯系物和TVOC的主要来源;长沙市不同的工业区TVOC浓度有显著差异,工业区合理布局,增加绿化面积,可以有效的降低TVOC浓度。     

以GDP-PM2.5达标为约束的东莞大气环境容量及承载力研究

东莞市计划到2017年PM_(2.5)年均浓度达到国家二级标准(35μg·m~(-3)),GDP年均增长率至少不低于7%.面对复合型为特征的PM_(2.5)大气污染,传统的环境容量和承载力计算方法具有局限性.因此,本文基于经济、气象、能源、环境等关键信息,利用系统动力学(SD)建立了GDPPM_(2.5)宏观动态统计模型.考虑到PM_(2.5)年均浓度等统计值本身就是污染物不断生成又不断扩散、沉降达到动态平衡的综合结果.因此,SD模型可不从理化角度去模拟复杂的大气传输和扩散过程,而是通过引入各污染物的比例系数μ,构建转化率η,建立GDP、PM_(2.5)年均浓度、五大污染物(VOCs、SO2、NOx、NH3、一次PM_(2.5))排放量等变量之间的逻辑联系,为分析和预测工作奠定基础.同时,本文梳理了大气环境压力、承载力和容量的定义,强调了三者之间的相互作用、密不可分的动态关系,建设性地提出了度量承载力的11项指标(5个显性、6个隐性).最后,利用模型模拟预测了"综合治理"模式下2012—2020年间以GDP-PM_(2.5)达标为约束的五大污染物的大气环境压力、容量和承载力.结果表明,预计PM_(2.5)浓度达标约在2017年上半年,对应的SO_2、NO_x、VOCs、NH_3、一次PM_(2.5)容量分别为84987、138849、100875、7751、17402 t;承载力隐性部分各项阈值分别为GDP总量7074亿元、新增绿色GDP 737亿元、煤炭2120万t(以标煤计)、石油552万t(以标煤计)、天然气663万t(以标煤计)、新能源630万t(以标煤计);承载力显性部分各阈值(相对于2012年5年累积减排量)分别为SO264271 t、NOx128831 t、VOCs 108337 t、NH34070 t、一次PM_(2.5)35863 t.本研究为东莞市大气减排提供了具体目标和参考数值.