贵阳市花溪城区大气PM2.5中碳质气溶胶的变化特征及来源解析

碳质气溶胶作为大气气溶胶的重要组成部分,对大气环境质量、人类健康及全球气候变化有着重要的影响.为探究贵阳市花溪城区大气细颗粒物（PM_2.5）中碳质气溶胶的变化特征及来源,于2020年不同季节开展大气PM_2.5原位观测研究,利用热/光学碳分析仪（DRI Model 2015）测定大气PM_2.5的碳质组分.结果表明,观测期间大气ρ（PM_2.5）、ρ[总碳质气溶胶（TCA）]、ρ[有机碳（OC）]、ρ[二次有机碳（SOC）]和ρ[元素碳（EC）]的平均值分别为：（39.7±22.3）、（14.1±7.2）、（7.6±3.9）、（4.4±2.6）和（2.0±1.0）μg·m^-3,OC/EC的平均值为（3.9±0.8）.ρ（PM_2.5）、ρ（TCA）、ρ（OC）、ρ（SOC）和ρ（EC）呈现冬季最高[（52.6±28.6）、（17.0±9.6）、（9.1±5.2）、（6.1±3.9）和（2.4±1.2）μg·m^-3],夏季最低[（25.1±7.1）、（11.6±3.6）、（6.3±1.9）、（3.7±1.2）和（1.6±0.6）μg·m^-3]的季节变化特征.OC/EC季节变化呈现：夏季（4.2±0.8）>冬季（3.8±0.9）>秋季（3.8±0.5）>春季（3.7±0.9）,表明花溪城区各季节均存在SOC生成.SOC与OC呈现显著相关（R²=0.9）,且随着大气氧化性增强,SOC浓度呈增加趋势.OC与EC各季节均呈现较好相关性,其中秋季最高（R²=0.9）,其他3个季节偏低（R²为0.74~0.75）,表明二者具有共同来源.通过OC/EC值范围初步判断碳质气溶胶来源于机动车尾气排放、燃煤排放和生物质燃烧排放.为了进一步定量解析主要排放源对碳质气溶胶的贡献,利用PMF模型对碳质气溶胶来源解析,结果表明贵阳市花溪城区碳质气溶胶主要来源为燃煤源（29.3%）、机动车排放源（21.5%）和生物质燃烧源（49.2%）.     

炉内喷钙脱硫技术及其主要影响因素简述

本文介绍国外炉内喷钙脱硫技术的最新发展,综述影响脱硫效率的各种因素.简介芬兰Tampella有限公司开发的LIFAC技术和国外有关利用吸收剂再循环等方式提高脱硫率和钙利用率的研究结果,展望了炉内喷钙脱硫技术的发展前景.     

Spatial and Temporal Comparison of Polycyclic Aromatic Hydrocarbons and Spheroidal Carbonaceous Particles in Remote European Lakes

Spheroidal carbonaceous particles (SCP) and polycyclicaromatic hydrocarbons (PAH) have been measured in the dated sediment cores of 10 remote lakes distributed across Europe. The geographic trends were evaluated by examination of the superficial sediment fluxes and total sediment inventories. The highest levels of both markers were observed in the Eastern European lakes whereas the minimal values corresponded to the lake located in the Arctic. However, this SCP-PAH correlation was not observed after exclusion of the end member lakes from the series. The temporal trends of both pollutant markers are consistent with the history of pyrolytic emissions over Europe. However, the downcore SCP distributions are shorter than the PAH profiles in nearly all lakes. The differences are probably related to the different size particle fractions involved in the measurement of each marker, >5 and >1 m for SCP and PAH, respectively. Thus, the two proxies probably reflect pollution inputs from closer (SCP) and more distant sites (PAH).     

Influence of fuel moisture, charge size, feeding rate and air ventilation conditions on the emissions of PM, OC, EC, parent PAHs, and their derivatives from residential wood combustion

Controlled combustion experiments were conducted to investigate the influence of fuel charge size, moisture, air ventilation and feeding rate on the emission factors (EFs) of carbonaceous particulate matter, parent polycyclic aromatic hydrocarbons (pPAHs) and their derivatives from residential wood combustion in a typical brick cooking stove. Measured EFs were found to be independent of fuel charge size, but increased with increasing fuel moisture. Pollution emissions from the normal burning under an adequate air supply condition were the lowest for most pollutants, while more pollutants were emitted when an oxygen deficient atmosphere was formed in the stove chamber during fast burning. The impacts of these factors on the size distribution of emitted particles was also studied. Modified combustion efficiency and the four investigated factors explained 68%, 72%, and 64% of total variations in EFs of PM, organic carbon, and oxygenated PAHs, respectively, but only 36%, 38% and 42% of the total variations in EFs of elemental carbon, pPAHs and nitro-PAHs, respectively.     

碳质气溶胶(OC/EC)新型观测方法对比分析

基于热光反射法（IMPROVE A）和热光透射法（RT-Quartz）二种协议分析方法和新型OC/EC分析方法对济南市碳质气溶胶含量进行了对比观测.结果表明,协议方法在OC/EC的观测过程中因分析定义会造成碳质气溶胶质量浓度高估或者低估,且膜采样系统使离线分析的OC约为在线的1.65倍,而新型OC/EC测量方法相对于2种协议方法,去除了原理上和环境参数（如VOCs）可能导致的误差,在OC/EC/TC测量结果上均有一定优势,在实际运行中更具有准确性、稳定性和实用性,更加适合颗粒物中OC/EC长期业务化在线测量.     

城市间PM2.5源的碳成分谱比较

为了解我国不同城市PM_2.5源的碳成分谱特征和地域差异,采集沈阳市、十堰市和乌鲁木齐市的燃煤源、柴油车尾气源、汽油车尾气源和餐饮源样品,使用热光透射法分析PM_2.5中的总碳（TC）、有机碳（OC）和元素碳（EC）,以及细分的8种碳组分（OC1,OC2,OC3,OC4,EC1,EC2,EC3和OPC_T）,构建各类污染源碳成分谱.结果表明：3个城市4类源TC/PM_2.5从高到低分别为：餐饮源（65.1%±8.4%）、柴油车尾气源（46.2%±9.5%）、汽油车尾气源（37.7%±3.5%）和燃煤源（17.3%±8.0%）;OC/TC在餐饮源中最高（98.0%±0.5%）,EC/TC在柴油车尾气源中最高（38.6%±8.5%）.3个城市同类源的碳组分含量受污染源细分后的不同类型影响有一定差异,但归一化处理后总体仍表现为燃煤源中OC2（14%~30%）和OC3（13%~23%）含量最高,柴油车尾气源中EC2（22%~56%）含量最高,汽油车尾气源中OC2（24%~41%）、OC1（16%~42%）和OC3（12%~26%）含量最高,餐饮源中OC2（21%~43%）和OC3（23%~49%）含量最高.不同污染源的OC/EC值为燃煤源在0.4~7.6之间,柴油车尾气源在0.2~5.6之间,汽油车尾气源在1.1~38.5之间,餐饮源在6.4~170.2之间.分歧系数结果显示3个城市不同源的碳成分谱具有差异性,同类源的碳成分谱具有相似性.将3个城市同类源碳成分谱合并后利用化学质量平衡灵敏度矩阵得到OC2,OC3,OC4,EC1和OPC_T可共同作为燃煤源的标识组分;EC2是柴油车尾气源的标识组分;OC1,OC2和OC3可共同作为汽油车尾气源的标识组分;OC2和OC3可共同作为餐饮源的标识组分.沈阳市、十堰市和乌鲁木齐市相同污染源相似的碳成分谱和一致的标识碳组分可为国内其他城市相关研究提供数据参考.     

Formation of sulfur oxide groups by SO2 and their roles in mercury adsorption on carbon-based materials

The presence of SO₂ display significant effect on the mercury (Hg) adsorption ability of carbon-based sorbent. Yet the adsorption and oxidation of SO₂ on carbon with oxygen group, as well as the roles of different sulfur oxide groups in Hg adsorption have heretofore been unclear. The formation of sulfur oxide groups by SO₂ and their effects on Hg adsorption on carbon was detailed examined by the density functional theory. The results show that SO₂ can be oxidized into SO₃ by oxygen group on carbon surface. Both C-SO₂ and C-SO₃ can improve Hg adsorption on carbon site, while the promotive effect of C-SO₂ is stronger than C-SO₃. Electron density difference analyses reveal that sulfur oxide groups enhance the charge transfer ability of surface unsaturated carbon atom, thereby improving Hg adsorption. The experimental results confirm that surface active groups formed by SO₂ adsorption is more active for Hg adsorption than the groups generated by SO₃.     

菏泽市冬季大气PM2.5和PM10中碳组分来源解析

为研究菏泽市冬季大气颗粒物中碳组分的污染特征和来源,于2016年1月采集菏泽市冬季大气PM_2.5和PM₁₀样品,基于热光反射法分析样品中OC（有机碳）、EC（元素碳）及8个碳组分[OC1、OC2、OC3、OC4、EC1、EC2、EC3和OP（裂解碳）]的含量,并计算得到ρ（Char-EC）（Char-EC为燃料燃烧后固体残渣中的EC）和ρ（Soot-EC）（Soot-EC为燃烧后气相挥发物质再凝结形成的EC）,以定性识别大气颗粒物中碳组分的来源.结果表明,菏泽市冬季大气颗粒物样品中碳组分浓度处于较高水平,PM_2.5中的ρ（OC）、ρ（EC）分别为26.34、9.22 μg/m3,PM₁₀中ρ（OC）、ρ（EC）分别为31.82、10.71 μg/m3.采样期间大气PM_2.5中碳组分（OC、EC、OC1、OC2、OC3、OC4、EC1、EC2、EC3、Char-EC、Soot-EC）浓度与PM₁₀中相应各组分浓度的比值均大于0.5（0.60~0.90）,表明碳组分多集中于细粒子（PM_2.5）.大气颗粒物样品中各碳组分浓度具有明显空间差异,各点位大气PM_2.5和PM₁₀中ρ（OC）均显著高于ρ（EC）（T检验,P < 0.05）.菏泽市冬季大气PM_2.5和PM₁₀中Char-EC/Soot-EC（二者质量浓度之比）分别为10.04、8.00,并且存在显著的空间差异性（T检验,P < 0.05）.PMF（正定矩阵因子分解法）解析结果表明,菏泽市冬季大气PM_2.5和PM₁₀中碳组分来源主要有4类,包括两类柴油车（1类排放的碳组分中以EC2为主,定义为柴油车-1;1类排放的碳组分中以EC3为主,定义为柴油车-2）、汽油车、生物质燃烧和燃煤混合源,对大气PM_2.5中碳组分的分担率分别为13.98%、5.13%、24.47%、41.97%,对大气PM₁₀中碳组分的分担率分别为16.08%、8.21%、18.34%、47.35%.可见,菏泽市冬季大气PM_2.5和PM₁₀中碳的主要来源是柴油车、汽油车、生物质燃烧和燃煤.      

新型铁铜锰复合氧化物颗粒吸附剂As(Ⅲ)吸附行为与机制研究

以壳聚糖为黏合剂,采用包覆法制备了一种新型除砷吸附剂——颗粒状铁铜锰复合氧化物(GFCM). GFCM吸附剂为不完全球状,直径0.7～1.0 mm,可以有效地将As(Ⅲ)氧化成As(V),并对形成的As(V)具有良好的吸附效果. GFCM对As(Ⅲ)的最大吸附容量(pH 7.0)为56.5 mg·g~(-1),显著优于目前已报道的多数颗粒状除砷吸附剂.溶液pH在5.0～9.0范围内, GFCM对As(Ⅲ)均有较好的吸附效果,离子强度则对砷吸附效果影响较小.共存阴离子对As(Ⅲ)吸附具有抑制作用,影响的大小顺序为:PO■ SiO■ CO■ Cl~- SO■.吸附As(Ⅲ)后的GFCM可用NaOH溶液进行有效脱附再生,可重复使用.在As(Ⅲ)的去除过程中,吸附剂中锰氧化物的主要作用是氧化As(Ⅲ),铁氧化物与铜氧化物的主要作用是吸附As(Ⅲ)与氧化形成的As(V),且铜氧化物有助于增强GFCM的砷吸附性能.