上甸子区域背景站VOCs污染特征及其对臭氧生成贡献

大气中的挥发性有机物(volatile organic compounds,VOCs)作为对流层臭氧和二次有机气溶胶的前体物,在光化学反应和细颗粒物污染中发挥着重要的作用.本研究于2017年9月1～27日在上甸子区域背景站开展VOCs的连续在线观测,对VOCs的浓度水平,时空变化特征,化学反应活性及其对臭氧生成的贡献进行了研究,并运用特征物种比值法对初始VOCs的来源进行了分析.结果表明, 2017年9月上甸子站总VOCs平均体积分数为12.53×10~(-9),其中,烷烃是体积分数最大的组分,占到了总VOCs的65.3%,其次是烯烃和芳香烃,分别占到了总VOCs的26.7%和6.5%.从大气化学活性来看,上甸子站总的L~(·OH)(·OH损耗率)为5.2 s~(-1),其中C4～C5烯烃占到了61%,其次是C2～C3烯烃,占到了12.8%.VOCs的臭氧生成潜势平均值为36.5×10~(-9),烯烃是贡献最大的组分,占到了71.2%.烯烃中又以C4～C5烯烃的贡献最为突出,而体积分数较大的烷烃对臭氧生成的贡献却不大.对特征物种的比值研究发现,上甸子站VOCs受生物质燃烧和燃煤排放的影响较大,除此之外,交通排放源也有一定的影响,完全不受工业排放源的影响.     

四川省典型行业挥发性有机物源成分谱

本研究选取了四川省汽车制造、木制家具、人造板制造、涂料生产和合成树脂生产等挥发性有机物(VOCs)排放源典型行业,通过GC-MS国标方法分析各环节有组织排放的VOCs组分,采用排放总量归一化法处理,获取了四川省汽车制造等典型行业挥发性有机物的成分谱.结果表明,汽车整车制造、木制家具和油性涂料生产企业的VOCs主要组分为芳香烃和含氧化合物,占总VOCs的70%以上,汽车零部件制造企业排放物种主要为芳香烃,其占比达90%以上.人造板制造业含氧化合物占比达97%,其中甲醛占比为75%,其次为异丙醇、丙酮等物质.合成树脂行业芳香烃、烯烃占比较高,占比之和达80%以上,其中烯烃物种主要为1,3-丁二烯和1-丁烯.不同行业排放物种虽存在一定差异,但主要以芳香烃和含氧化合物为主,因此,应加强对芳香烃和含氧化合物等浓度高、活性高、毒性大的组分进行识别和控制,采取源头、过程和末端全过程控制,达到总量减排的效果.     

阳泉市区夏季挥发性有机物污染特征、来源解析及其环境影响

采集阳泉市区夏季3个监测点的环境空气样品,利用气相色谱-质谱/氢火焰离子化检测器(GC-MSD/FID)测定了挥发性有机物(VOCs)的组成,研究了其浓度特征,运用特征比值法和正定矩阵因子分析模型(PMF)解析了VOCs来源,评估了VOCs对O_3和二次有机气溶胶(SOA)生成的影响.结果表明,阳泉市区VOCs平均总浓度为(82.1±22.7)μg·m~(-3),其中烷烃浓度占比最大(51.8%),其次是芳香烃(17.8%)和烯烃(8.0%),炔烃浓度占比最小(3.8%). VOCs呈现双峰的变化特征,分别于08:00～10:00和18:00～20:00出现峰值,在12:00～14:00出现谷值.苯/甲苯和异戊烷/正戊烷的均值分别为2.1±1.3和1.7±0.6,表明环境空气VOCs可能受燃煤排放和机动车排放的双重影响. PMF解析出VOCs来源分别为燃煤源(34.9%)、机动车排放源(18.2%)、汽油挥发源(15.2%)、工业排放源(13.6%)、植物排放源(9.2%)和溶剂使用源(9.0%). VOCs臭氧生成潜势(OFP)均值为156.6μg·m~(-3),烯烃贡献最大,二次有机气溶胶生成潜势(SOA_p)均值为68.7μg·m~(-3),芳香烃的贡献达到93.4%.总之,燃煤排放对VOCs的贡献较高,因此,控制燃煤源排放是阳泉市区VOCs管控重点,需加快矸石山治理和能源结构调整,同时机动车排放源、汽油挥发源和工业排放源的管控也不容忽视.     

北方常见绿化树种BVOCs排放特征及其与光合作用参数的相关性

为了解北方常见绿化树种植物源挥发性有机化合物(biogenic volatile organic compounds,BVOCs)的排放特征及其与光合作用参数(净光合速率P_n、气孔导度g_s、胞间CO_2浓度c_i、蒸腾速率T_r)的相关性,本实验采用动态采样装置收集14种落叶乔木BVOCs排放数据.结果表明,不同科属间异戊二烯和总BVOCs(异戊二烯、单萜和倍半萜烯之和)释放速率差异显著(P0.01).除金银木和榆树,其他绿化树种均释放异戊二烯、单萜和倍半萜烯类物质,其中杨柳科(杂交杨‘546’、速生杨‘107’、小叶杨、垂柳)和豆科植物(国槐、刺槐、龙爪槐)排放异戊二烯较多,释放速率在(30.1±4.3)～(91.8±10.0)μg·(g·h)~(-1)之间;木犀科(白蜡、丁香)、蔷薇科海棠、无患子科栾树和槭树科元宝枫主要排放单萜和倍半萜烯,其中白蜡和元宝枫单萜释放速率最高,分别为(10.6±4.8)μg·(g·h)~(-1)和(11.8±6.4)μg·(g·h)~(-1).罗勒烯和β-蒎烯是绿化树种排放的两种主要单萜物质.P_n和g_s与BVOCs释放速率之间无显著相关性,但杨柳科植物异戊二烯(r=0.681,P0.01)和总BVOCs(r=0.698,P0.01)释放速率与叶片T_r呈显著正相关,而豆科植物的总BVOCs释放速率与c_i呈显著正相关(P=0.04).本研究为城市绿化树种的筛选和配置提供科学参考,也为BVOCs释放机制的研究提供理论依据.     

海峡西岸清洁岛屿秋季VOCs特征及来源解析

挥发性有机物（VOCs）是臭氧（O₃）和二次有机气溶胶（SOA）的重要前体物.为夯实国内海岛背景点VOCs监测,研究海峡西岸清洁岛屿平潭VOCs污染特征及来源,探索化学二次生成对清洁岛屿O₃的影响,于2018年秋季,对平潭大气VOCs进行了监测研究.结果表明,平潭2018年秋季VOCs浓度为1.94~52.12 μg·m^-3,平均值为15.54 μg·m^-3,烷烃占比最高（66.02%）,乙烷为浓度的最大物种,达到6.82 μg·m^-3.平潭秋季VOCs浓度日变化呈双峰型,表现出典型的人类活动相关性.经比较甲苯/苯（T/B）可知,平潭秋季VOCs来源主要是交通排放及燃料蒸发.利用正交矩阵分解（PMF）源解析发现,汽车尾气（72.8%）、船舶排放（12.4%）、生物质燃烧（8.7%）、工业排放和溶剂使用（3.5%）和燃料蒸发（2.6%）是平潭VOCs的五大来源.平潭秋季VOCs的O₃生成潜势（OFP）差异较大,其中,烯烃（62.6%） > 烷烃（24.7%） > 芳香烃（12.7%）.当平潭O₃属于VOCs控制型时,控制大气中烯烃的浓度可一定程度上防治平潭O₃的污染.     

宝鸡市秋冬季大气VOCs浓度特征及其O3和SOA生成潜势

2017年10月、12月在宝鸡市城区开展了共29d的挥发性有机物（VOCs）浓度在线监测,共测出102种VOCs,分别采用最大增量反应活性（MIR）系数法和气溶胶生成系数（FAC）法估算了宝鸡市各VOCs组分的臭氧生成潜势（OFPs）和二次有机气溶胶生成潜势（SOAFPs）,筛选出生成O₃与SOA活性最大的VOCs成分.结果表明：宝鸡市秋季和冬季TVOC的浓度分别为（68.62±21.85）×10^-9和（42.44±16.62）×10^-9,总OFPs分别为185.49×10^-9和126.00×10^-9,总SOAFPs分别为3.26,0.65μg/m³.秋季VOCs中含量最多的2种组分为烷烃（21.83×10^-9）和芳香烃（13.37×10^-9）,分别占TVOC的31.82%和19.49%,乙烯、反-2-戊烯和甲苯是OFPs最大的3个成分,甲苯、间/对二甲苯和乙苯是SOAFPs最大的3个成分.而在冬季,烷烃（17.34×10^-9）和炔烃（8.81×10^-9）是VOCs中含量最多的2种组分,分别占TVOC的40.85%和20.75%,乙烯、丙烯、乙炔是OFPs最大的3个成分,甲苯、间/对二甲苯、乙苯是SOAFPs最大的3个成分.优先减少烯烃和芳香烃的排放是宝鸡市秋冬季抑制O₃和SOA的形成的有效途径.     

广州典型印刷企业VOCs排放特征及环境影响和健康风险评价

本文以广州市典型印刷企业为研究对象,通过对各排放环节的浓度和组分的全面统计和综合分析,深入探讨广州市该行业VOCs排放特征、环境影响及人体健康风险.结果表明,印前环节车间VOCs浓度为3.51~73.57mg/m³,印刷环节车间VOCs浓度为0.86~435.10mg/m³,印后环节车间VOCs浓度为0.05~221.93mg/m³,废气治理设施出口浓度为4.28~66.84mg/m³,处理效率为3.01%~54.90%;且VOCs物种以芳香烃类、醇醚类和酯类为主,平均臭氧生成潜势为111.09mg/m³,其中芳香烃类物质对环境影响贡献和人体健康风险较大,建议加强针对性控制.     

VOCs released from municipal solid waste at the initial decomposition stage: Emission characteristics and an odor impact assessment

The nuisance from odor caused by municipal solid waste (MSW) is resulting in a growing number of public complaints and concerns. Odor pollution occurs in the initial decomposition stage of MSW, including waste collection, transportation and early pre-treatment. Furthermore, decomposition takes place in waste facilities that are often close to living areas, which can result in odor impacts on local inhabitants. However, this aspect of odor impact from MSW has not been well studied. In the current study, lab-scale waste cells were designed to simulate MSW storage conditions in the early stage. The characteristics of VOCs emissions with different waste compositions were analyzed. The odor concentration (C_O, non-dimensional) method and odor intensity were used for the assessment of odor. Ethanol was the substance with highest emission rate. The release rate of VOCs increased with the growth easily biodegradable waste (EBW). VOCs emissions was reduced by 25% when the proportion of EBW decreased from 60% to 45%. Methyl sulfide, ethanol, dimethyl disulfide and ethyl acetate were identified as typical odorants. The EBW proportion in waste is the main factor significantly influencing odor pollution. The C_O was 244.51 for the 60% EBW condition, which was only 61.46 for 15% EBW condition. These study results provide important information for the implementation of a garbage sorting policy and the monitoring of odor pollution from waste management.     

The pollution levels, variation characteristics, sources and implications of atmospheric carbonyls in a typical rural area of North China Plain during winter

Atmospheric carbonyls were measured at a typical rural area of the North China Plain (NCP) from November 13 to December 24, 2017 to investigate the pollution characteristics, sources and environmental implications. Fifteen carbonyls were detected, and formaldehyde, acetaldehyde and acetone accounted for about 81% at most. The concentration of the total carbonyls in heavily polluted days was twice more than that in clean days. In contrast to other carbonyls, m-tolualdehyde exhibited relatively high concentrations in the clean days in comparison with the polluted days. The ratios of three principal carbonyls to CO showed similar daily variations at different pollution levels with significant daytime peaks. Multiple linear regression analysis revealed that the contributions of background, primary and secondary sources to three principal carbonyls showed similar variation trends from the clean level to the heavily polluted level. The OH formation rate of formaldehyde showed a similar variation trend to its photodegradation rate, reaching the peak value at noon, which is important to maintain relatively high OH levels to initiate the oxidation of various gas-phase pollutants for secondary pollutant formation at the rural site. OH radical consumption rate and ozone formation potential (OFP) calculations showed that formaldehyde and acetaldehyde were the dominant oxidative species among measured carbonyls. As for OH radical consumption, n-butyraldehyde and m-tolualdehyde were important contributors, while for ozone formation potential, n-butyraldehyde and propionaldehyde made significant contributions. In addition, the contribution of carbonyl compounds to secondary organic aerosol (SOA) formation was also important and needs further investigation.     

Superior CO2 uptake on nitrogen doped carbonaceous adsorbents from commercial phenolic resin

In this study, N-doped porous carbons were produced with commercial phenolic resin as the raw material, urea as the nitrogen source and KOH as the activation agent. Different from conventional carbonization-nitriding-activation three-step method, a facile two-step process was explored to produce N-incorporated porous carbons. The as-obtained adsorbents hold superior CO₂ uptake, i.e. 5.01 and 7.47 mmol/g at 25?°C and 0?°C under 1 bar, respectively. The synergistic effects of N species on the surface and narrow micropores of the adsorbents decide their CO₂ uptake under 25?°C and atmospheric pressure. These phenolic resin-derived adsorbents also possess many extremely promising CO₂ adsorption features like good recyclability, quick adsorption kinetics, modest heat of adsorption, great selectivity of CO₂ over N₂ and outstanding dynamic adsorption capacity. Cheap precursor, easy preparation strategy and excellent CO₂ adsorption properties make these phenolic resin-derived N-doped carbonaceous adsorbents highly promising in CO₂ capture.