2018年春节期间京津冀地区污染过程分析

为了解2018年春节期间京津冀地区空气污染情况,利用近地面污染物浓度数据、激光雷达组网观测数据,结合WRF气象要素、颗粒物输送通量和HYSPLIT气团轨迹综合分析污染过程.结果表明,春节期间出现3次污染过程.春节前一次污染过程,各站点PM_2.5浓度均未超过200μg/m³;除夕夜,廊坊站点PM_2.5峰值浓度达到504μg/m³,是清洁天气的26倍;年初二~初五,各站点PM_2.5始终高于120μg/m³,且污染主要聚集在500m高度以下,北京地区存在高空传输,800m处最大输送通量达939μg/（m³·s）,此次重污染过程为一次典型的区域累积和传输过程.京津冀地区处于严格管控状态时,燃放烟花爆竹期间PM_2.5峰值浓度可达无燃放时PM_2.5峰值的3.2倍.为防止春节期间重污染现象的发生,需对静稳天气下燃放烟花炮竹采取预防对策.     

Density functional theory (DFT) studies of vanadium-titanium based selective catalytic reduction (SCR) catalysts

Based on density functional theory (DFT) and basic structure models, the chemical reactions on the surface of vanadium-titanium based selective catalytic reduction (SCR) denitrification catalysts were summarized. Reasonable structural models (non-periodic and periodic structural models) are the basis of density functional calculations. A periodic structure model was more appropriate to represent the catalyst surface, and its theoretical calculation results were more comparable with the experimental results than a non-periodic model. It is generally believed that the SCR mechanism where NH₃ and NO react to produce N₂ and H₂O follows an Eley-Rideal type mechanism. NH₂NO was found to be an important intermediate in the SCR reaction, with multiple production routes. Simultaneously, the effects of H₂O, SO₂ and metal on SCR catalysts were also summarized.     

Recent advances in catalytic decomposition of ozone

Ozone (O₃), as a harmful air pollutant, has been of wide concern. Safe, efficient, and economical O₃ removal methods urgently need to be developed. Catalytic decomposition is the most promising method for O₃ removal, especially at room temperature or even subzero temperatures. Great efforts have been made to develop high-efficiency catalysts for O₃ decomposition that can operate at low temperatures, high space velocity and high humidity. First, this review describes the general reaction mechanism of O₃ decomposition on noble metal and transition metal oxide catalysts. Then, progress on the O₃ decomposition performance of various catalysts in the past 30 years is summarized in detail. The main focus is the O₃ decomposition performance of manganese oxides, which are divided into supported manganese oxides and non-supported manganese oxides. Methods to improve the activity, stability, and humidity resistance of manganese oxide catalysts for O₃ decomposition are also summarized. The deactivation mechanisms of manganese oxides under dry and humid conditions are discussed. The O₃ decomposition performance of monolithic catalysts is also summarized from the perspective of industrial applications. Finally, the future development directions and prospects of O₃ catalytic decomposition technology are put forward.     

Effect of struvite and organic acids on immobilization of copper and zinc in contaminated bio-retention filter media

Few studies have been carried out to connect nutrient recovery as struvite from wastewater and sustainable utilization of the recovered struvite for copper and zinc immobilization in contaminated soil. This study revealed the effect of struvite on Cu and Zn immobilization in contaminated bio-retention soil in the presence of commonly exuded plant organic acids. The research hypothesis was that the presence of both struvite and organic acids may influence the immobilization of Cu and Zn in soil. The outcome of this research confirmed that more than 99% of Cu and Zn was immobilized in bio-retention filter media by struvite application. Water-soluble Cu and Zn concentrations of struvite treated soil were less than 1.83 and 0.86 mg/kg respectively, and these concentrations were significantly lower compared to the total Cu and Zn content of 747.05 mg/kg in the contaminated soil. Application of struvite to Cu- and Zn-contaminated soil resulted in formation of compounds similar to zinc phosphate tetrahydrate (Zn₃(PO₄)₂?4H₂O) and amorphous Cu and Zn phases. Struvite was effective in heavy metal remediation in acidic soil regardless of the presence of Ca impurities in struvite and the presence of plant organic acids in soil. Overall, this study revealed that struvite recovered from wastewater treatment plants has potential for use as an amendment for heavy metal remediation in contaminated bio-retention soil.     

基于边介数的省域生态廊道构建方法优化

我国城市建设和生态保护工作均对土地资源有大量需求,二者之间的矛盾在经济优先发展区表现尤为明显.为了有效地改善生态环境,管控土地利用并引导其变化发展,需要建设具备不可替代特征的省域生态廊道.最小累积阻力模型（minimum cumulative resistance,MCR）是识别生态廊道最常用、有效的模型,但在应用于省域尺度时,MCR模型识别的潜在廊道路由存在冗余的问题.因此,通过引入网络科学中的边介数指数（edge-betweenness）对MCR模型进行优化,计算潜在廊道路由的边介数指数值,选取出其中最为重要和简明的结构来连通生态源地,即提取潜在路由中的骨干路由（backbone route）和关键战略点（key strategic point）作为不可替代的结构来指导省域生态廊道建设.将优化后的MCR模型应用于广东省,构建了全长5 493 km的省域生态廊道,其中包含生态源地20处,关键战略点11个,骨干生态廊道29条.骨干路由与关键战略点构成的不可替代省域生态廊道（irreplaceable provincial corridor）能够实现"廊道数量和占地面积最少、连通性基本不变"的目标.研究显示,边介数能够对潜在路由进行优化筛选,识别出维护省域生态安全的关键结构;不可替代生态廊道能够指导省域生态规划和土地空间的发展利用,并为更高水平的生态安全环境提供了演进的基础;同时也为土地资源紧张的地区提供了建设生态廊道的参考与依据.      

Chemical characteristics of road dust PM2.5 fraction in oasis cities at the margin of Tarim Basin

In order to understand the compositions characteristics of particulate matter with aerodynamic diameter less than 2.5 μm (PM_2.5) fraction in road dust (RD_2.5) of oasis cities on the edge of Tarim Basin, 30 road dust (RD) samples were collected in Kashi, Cele, and Yutian in the spring, 2018, and RD_2.5 was collected using the resuspension approach. Eight water-soluble ions, 39 trace elements and 8 fractions of carbon-containing species in PM_2.5 were analyzed. Ca²⁺ and Ca were the most abundant ions and elements in RD_2.5 (7.1% and 9.5%). Cl^- in RD_2.5 was affected not only by attributed to saline-alkali soils in oasis cities of the Tarim Basin and dust from Taklimakan Desert but also by human activities. Moreover, the organic carbon/elemental carbon (OC/EC) ratio indicated that carbon components in RD_2.5 in Cele town mainly come from fossil fuel combustion, while those in Yutian and Kashi mainly come from biomass combustion. It is noteworthy that high Ca in RD_2.5 was seriously affected by anthropogenic emissions, and high Na and K contents in RD_2.5 could be derived from soil and desert dust. It was estimated that Cd, Tl, Sn and Cr were emitted from anthropogenic emissions using the enrichment factor. The coefficients of divergence (COD) result indicated that the influence of local emission on road dust emission is greater than that of long-distance transmission. This study is the first time to comprehensively analyze the chemical characteristics of road dust in oasis cities, and the results provides the sources of road dust at the margin of Tarim Basin.     

外加氮源影响下铁铝氧化物在土壤氮素转化中的作用

土壤中铁铝氧化物在团聚体稳定性和有机碳吸附方面具有重要作用,而氮添加对土壤氮循环影响的变化也可能与其有关,但是目前尚缺乏在氮循环方面的研究.为了探究铁铝氧化物在土壤氮素转化中的作用,选择福建省建瓯罗浮栲森林土壤为研究对象,采用选择性溶提技术准备不同的土壤——未经处理（T1）的土壤和去除游离态铁铝氧化物（T2）土壤、去除非晶质铁铝氧化物（T3）土壤、去除络合态铁铝氧化物（T4）土壤,在这些土壤中添加不同形态氮（40 mg/kg）——丙氨酸（氨基酸态氮,AA）、硫酸铵（铵态氮,AN）、硝酸钠（硝态氮,NAN）和亚硝酸钠（亚硝态氮,NIN）,进行室内培养试验,分析氮含量变化和氮素转化情况.结果表明:①与CK处理相比,AA和AN处理均增加了T1土壤中w（NH₄+-N）,NAN处理增加了w（NO₃--N）,但低于添加量,表明添加氨基酸和铵态氮均会促进氮矿化,添加硝态氮会增加NO₃--N的固定且抑制其硝化.②在CK处理下,与T1土壤相比,T2和T4土壤中w（NH₄+-N）、w（NO₃--N）和w（氨基酸）均降低,但T3土壤中w（NH₄+-N）和w（氨基酸）增加、w（NO₃--N）降低,表明土壤中游离态氧化铁铝和络合态氧化铁铝的存在有助于氮素矿化,非晶质氧化铁铝有助于硝化.③在不同氮处理下,各土壤的氮含量及其转化速率与CK处理规律相似.与CK处理相比,各氮处理均未显著增加T2和T4土壤中w（NH₄+-N）,且AA和AN处理均未影响T2、T3和T4土壤中w（NO₃--N）和w（氨基酸）.结果显示,氮添加并没有改变铁铝氧化物的作用,其中,矿化和氨化作用均表现为游离氧化铁铝>络合氧化铁铝>非晶质氧化铁铝,硝化作用表现为非晶质氧化铁铝>游离氧化铁铝>络合态氧化铁铝.因此,土壤铁铝氧化物的不同存在状态应该是调节氮素转化的重要土壤条件.      

基于野外原位抽注试验和同位素技术的含水层反硝化速率研究

反硝化作用是地下水硝酸盐污染去除最重要的过程.由于水文地质条件和水文地球化学环境的复杂性和不确定性,精准测定含水层反硝化速率是反硝化过程的研究难点.选取潮白河冲洪积扇中部中国环境科学研究院地下水创新野外基地作为研究区,基于野外原位试验和15N同位素示踪法提出一种含水层反硝化速率的测定方法.该方法综合体现了研究区实际水文地质条件和水文地球化学环境对反硝化作用的影响,并充分考虑了硝酸盐在含水层中稀释弥散作用对计算结果的影响.结果表明:①潮白河冲洪积扇中部某地地下26~28 m处于还原环境,含水介质以粉细砂为主,ρ（NO₃-N）平均值为2.77 mg/L.②地下26~28 m反硝化速率在349.52~562.99 μg/（kg·d）（以N计,下同）之间,平均值为450.31 μg/（kg·d）.通过与研究区含水介质、采样深度和硝酸盐背景值相似的国内外案例对比研究,初步评估结果处于合理区间.③测试结果具有一定不确定性,主要来自忽略中间产物NO₂-和NO的计算方法、扰动采样方法、N₂O的操作规范程度及采样频率等方面.研究方法为测定含水层硝酸盐速率研究提供了新的思路,研究结果可为地下水中硝酸盐转化过程机理研究、地下水硝酸盐污染修复及风险管控提供关键的理论支撑数据.      

长三角背景点夏季大气PM2.5中水溶性无机离子污染特征及来源解析

为研究长三角背景点夏季PM_2.5污染特征,于2018年5月30日—8月15日在上海市崇明岛对PM_2.5样品进行昼夜采集,并对其中水溶性无机离子(Cl-、NO₃-、SO₄2-、Na+、NH₄+、K+、Mg2+、Ca2+)进行了分析.运用PSCF(潜在源贡献)方法判别污染物排放源区,并结合PCA(主成分分析)和PMF(正交矩阵因子)源解析探究PM_2.5来源.结果表明:①观测期间崇明岛ρ(PM_2.5)平均值为(33±21)μg/m3,低于GB 3095—2012《环境空气质量标准》一级标准限值(35 μg/m3),但在部分时段存在显著超标现象,ρ(PM_2.5)最高值在120 μg/m3以上.②水溶性无机离子质量浓度平均值为(14±9.3)μg/m3,占PM_2.5的42.4%,其中SNA(SO₄2-、NO₃-、NH₄+三者统称)为主要离子,占水溶性离子总质量浓度的85.7%.③n(NH₄+)/n(SO₄2-)(NH₄+与SO₄2-的摩尔浓度比)显示,清洁期〔ρ(PM_2.5) < 15 μg/m3〕呈贫铵状态,过渡期〔15≤ρ(PM_2.5)≤35 μg/m3〕和污染期〔ρ(PM_2.5)>35 μg/m3〕均呈富铵状态;过渡期SNA主要以NH₄HSO₄和NH₄NO₃形式存在,而污染期则主要以(NH₄)₂SO₄和NH₄NO₃形式存在.④通过对两次典型污染事件进行离子相关性分析和PSCF分析发现,E1污染事件(5月30日—6月8日)为局地生物质燃烧型污染事件,E2污染事件(7月23日—8月1日)为区域传输污染事件.源解析结果进一步表明,两次典型污染事件期间气态污染物的二次转化对PM_2.5的贡献最显著,贡献率分别为62.8%和59.8%;其次是生物质燃烧,其贡献率分别为32.5%和20.1%;E2污染事件期间海盐源对崇明岛PM_2.5贡献率较高(16.6%),远超过E1污染事件期间对PM_2.5的贡献率(2.7%).研究显示,区域输送对崇明岛PM_2.5有显著贡献,二次颗粒物累积是崇明岛PM_2.5超标的主要原因.      

深圳市龙岗区大气颗粒物中多溴联苯醚的污染特征研究

为了解深圳市龙岗区大气颗粒物中多溴联苯醚的污染状况,于2017年1月、4月、8月和11月分别采集龙岗区大气颗粒物样品.利用气相色谱-质谱联用仪（GC/MS）对深圳市龙岗区4个功能区（工业区、商业区、居民区和生态区）的80个大气颗粒物样品进行检测,得到PBDEs（多溴联苯醚）8种单体（BDE-28、BDE-47、BDE-99、BDE-100、BDE-153、BDE-154、BDE-183、BDE-209）的质量浓度,同时研究了大气颗粒物中PBDEs质量浓度的时空分布特征.结果表明:①深圳市龙岗区大气颗粒物中ρ（∑₈PBDEs）（∑₈PBDEs为PBDEs 8种单体的加和）范围为0.07~77.80 pg/m3,ρ（∑₈PBDEs）年均值为（6.86±14.17）pg/m3.ρ（BDE-209）范围为0.01~76.23 pg/m3,年均值为（5.10±13.58）pg/m3,BDE-209为主要污染单体.② 4个功能区的ρ（∑₈PBDEs）平均值大小顺序依次为工业区（13.65 pg/m3）>商业区（7.75 pg/m3）>生态区（3.95 pg/m3）>居民区（2.19 pg/m3）,工业区是环境空气颗粒物中PBDEs的主要污染区.③ ρ（∑₈PBDEs）平均值的季节性变化规律为春季（13.32 pg/m3）>冬季（9.18 pg/m3）>秋季（2.17 pg/m3）>夏季（1.51 pg/m3）,符合深圳市亚热带海洋季风气温和气候对环境空气中颗粒物质量浓度的影响规律.研究显示,深圳市龙岗区大气颗粒物中PBDEs质量浓度处于较高水平,污染严重,建议减少含PBDEs产品的生产、使用和运输等活动,或找到更利于环境安全和人体健康的替代品,降低PBDEs对该地区的污染.