滇黔桂岩溶区河漫滩土壤重金属含量、来源及潜在生态风险

利用全国地球化学基准计划在滇黔桂岩溶区35个点位采集的70件河漫滩表、深层土壤样品,分析了As、Cd、Cr、Cu、Hg、Ni、Pb和Zn 8种重金属元素含量特征,探究了重金属来源、污染状况及潜在生态风险.结果表明,8种重金属元素含量大部分均高于全国土壤背景值,在滇东南地区含量最高,桂西北地区最低.表层土壤Cd、Hg明显富集,As、Cr、Cu、Ni与深层土壤含量相当;As、Cd、Hg、Pb、Zn在农田、菜地中明显高于深层土壤,Cr、Cu和Ni在各类土地中与深层土壤相当.因子分析结果显示,表层土壤中Cd、Cr、Cu、Ni受地质背景控制,As、Pb、Zn既与地质背景有关,也受人为活动影响,Hg受人为活动影响较严重;深层土壤中Cd、Cr、Cu、Ni、Cr、Zn继承了区域母岩特征,As、Hg和Pb受地质背景和人为活动双重影响.地累积指数法和富集因子法污染评价结果表明,研究区河漫滩表层土壤中Cd、Hg污染较重,As、Cr、Cu、Ni、Pb、Zn大部分为轻度污染或无污染.各重金属潜在生态风险指数高低顺序依次为Hg > Cd > As > Cu > Ni > Pb > Cr > Zn,Cd和Hg的生态风险指数之和占综合指数的82.43%,生态风险最高;滇东南地区重金属潜在风险综合指数最高,具重度生态风险.     

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.     

基于全过程治理的环境规制减排机制研究——来自长江经济带数据的实证检验

基于2007~2017年长江经济带11个省市的面板数据,利用中介效应模型探究全过程治理视域下政府主导型和市场激励型2类环境规制的减排机制.研究发现,政府主导型环境规制和市场激励型环境规制对SO₂排放均具有显著的抑制作用,其影响系数分别为-0.154和-0.209.其中政府主导型环境规制在源头防控、过程控制和末端治理的全过程都起到显著的减排效应,而市场激励型环境规制只通过末端治理实现减排.因此,尽管市场激励型环境规制具有低成本、高效率的优点,但考虑到源头防控和过程控制在生态环境保护中发挥的根本性作用,对于经济结构和经济发展方式较为落后的地区和行业,仍要重视以政府为主导的环境规制,通过因地制宜、合理科学地运用环境规制工具以实现高效的全过程污染治理.     

雨水管道沉积物中典型无机氮的干期粒径分布

以南京江北新区分流制雨水管道沉积物为研究对象,考察不同粒径沉积物中铵态氮（NH₃-N）和硝态氮（NO₃^--N）干期分布特征,分析其随干期长度的变化关系,并探讨沉积物理化性质及微生物菌群结构对NH₃-N和NO₃^--N干期分布的影响.结果表明：粒径≤0.075mm的沉积物中NH₃-N占比最高（交通区30.8%,商业区36.7%）;交通区粒径≤0.075mm的沉积物中NO₃^--N占比最高（33.0%）,而商业区粒径0.075~0.15mm沉积物中NO₃^--N占比最高（34.4%）;干期长度与交通区0.075~0.15mm粒径段的沉积物中NO₃^--N含量及商业区粒径≥0.3mm的沉积物中NH₃-N含量之间的相关性均最显著;雨水管道沉积物中NH₃-N和NO₃^--N的干期分布与O-H和N-H等官能团、表面极性和亲水性、微观形貌等有一定关联;交通区雨水管道沉积物中Gemmobacter等反硝化优势菌种（相对丰度总和为20.15%）对NO₃^--N干期分布影响更显著.     

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 substituents in hydroxyl radical-mediated degradation of azo pyridone dyes: Theoretical approaches on the reaction mechanism

Understanding the degradation behavior of azo dyes in photocatalytic wastewater treatment is of fundamental and practical importance for their application in textile-processing and other coloration industries. In this study, quantum chemistry, as density functional theory, was used to elucidate different degradation pathways of azo pyridone dyes in a hydroxyl radical (HO^?)-initiated photocatalytic system. A series of substituted azo pyridone dyes were synthesized by changing the substituent group in the para position of the benzene moiety, ranging from strong electron-donating to strong electron-withdrawing groups. The effect of dye molecular structure on the photocatalytic degradation reaction mechanism was analyzed and quantification of substituent effects on the thermodynamic and kinetics parameters was performed. Potential energy surface analysis revealed the most susceptible reaction site for the HO^? attack. The calculated reaction barriers are found to be strongly affected by the nature of substituent group with a good correlation using Hammett σ_p constants and experimentally determined reaction rates. The stability of pre-reaction complexes and transition state complexes were analyzed applying the distortion-interaction model. The increased stability of the transition state complexes with the distancing from the substituent group has been established.     

杭州湾北岸36种挥发性有机物污染特征及来源解析

为研究杭州湾北岸VOCs（挥发性有机物）的浓度水平、组成特征、反应活性和潜在来源,采用GC-FID在线监测系统对杭州湾北岸环境大气中的36种VOCs开展了为期1 a（2017年12月-2018年11月）的连续观测,采用LOH（VOCs的·OH消耗速率）和OFP（O₃生成潜势）2种方法估算了大气VOCs的反应活性,并利用PMF（正定矩阵因子分解）和CPF（条件概率函数）模型分析其来源.结果表明:①φ（VOCs）小时平均值在冬季（26.47×10-9）最高,夏季（9.76×10-9）最低;全年φ（VOCs）小时平均值为21.24×10-9,其中烷烃、烯烃+炔烃、芳香烃、卤代烃的贡献率分别为33.24%、34.13%、15.63%、17.00%;φ（烷烃）、φ（芳香烃）和φ（卤代烃）呈较明显的昼夜变化特征,φ（烯烃）和φ（炔烃）无明显昼夜变化趋势.②大气VOCs的总LOH和OFP分别为9.39 s-1和220.57 μg/m3,KOH（·OH反应速率常数）和MIR（最大增量反应活性）系数的平均值分别为17.34×10-12 cm3/（molecule·s）和3.31;KOH和MIR系数的平均值分别与间/对-二甲苯的KOH和乙苯的MIR系数接近,表明大气VOCs的化学反应活性较强;VOCs关键活性物种为异戊二烯、乙烯、丙烯、甲苯、二甲苯和顺-2-丁烯.③特征物种相关性分析表明,杭州湾北岸大气存在老化现象,异戊烷和正戊烷受煤燃烧源影响较大,二甲苯和乙苯受溶剂排放源影响较大,甲苯和苯除受机动车尾气影响外,还受其他排放源影响.④PMF和CPF模型来源分析表明,大气VOCs主要来自石化工业源、燃料挥发源、生物质燃烧和煤燃烧源、机动车排放源和溶剂使用源,其中,机动车排放源主要来自西北方向,其他源主要来自西北、西和西南方向.研究显示,杭州湾北岸大气VOCs来源复杂,受周边工业区的影响较大.      

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.