面向区域二次污染风险控制的臭氧及其前体物卫星遥感监测

日益突出的臭氧(O_3)污染已成为继PM2. 5之后我国大气污染防治的又一艰巨任务。由于氮氧化物(NO_x)、挥发性有机物(VOCs)这2种前体物的减排难度较大,且与O_3浓度存在复杂的非线性关系,准确获取O_3及NO_x、VOCs的时空分布对制定有效的防控措施至关重要。基于卫星遥感可定量反演O_3及2种前体物的代表性物种——二氧化氮(NO_2)、甲醛(HCHO)及乙二醛(C_2H_2O_2)的时空分布信息。面向区域O_3污染分析和防控应用,综述了卫星遥感对O_3及NO_2、HCHO、C_2H_2O_2的探测能力,以及利用遥感手段分析区域O_3及其前体物的传输。进而从O_3与NO_x、VOCs关系的角度,分析了利用卫星反演的前体物表征O_3生成风险的可行性。最后对卫星在区域O_3及其前体物监测方面的前景趋势提出了思考。     

江苏省2014-2016年臭氧污染区域特征分析

分析2014—2016年江苏省O₃污染状况，以及苏北、苏中和苏南3个典型区域O₃年度、季度、日变化和频度占比等分布特征。结果表明，江苏省的O₃空间分布呈现北低南高，2014—2016年的O₃超标占比由18.4%上升至34.9%；2016年苏北、苏中和苏南地区O₃-8h第90百分位数与2014年相比，上升2.7%，21.8%和3.3%；3个区域夏季O₃-8h均值最高，春、秋2季次之，冬季最低；O₃-1h日变化呈单峰状态，最低值出现在06:00—07:00，最高值出现在15:00—16:00；2016年3个地区的O₃频度占比均呈正态分布，主要集中在40~80 μg/m³，所占比例均>15%；苏中和苏南区域2016和2014年相比O₃频率占比的变化幅度较大，苏北地区变化幅度不大。指出，江苏省的O₃污染程度在逐年提高，污染范围从苏南逐渐往中部和北部城市扩大。     

Precursors and potential sources of ground-level ozone in suburban Shanghai

• Air masses from Zhejiang Province is the major source of O₃ in suburban Shanghai. • O₃ formation was in VOC-sensitive regime in rural Shanghai. • O₃ formation was most sensitive to propylene in rural Shanghai. A high level of ozone (O₃) is frequently observed in the suburbs of Shanghai, the reason for this high level remains unclear. To obtain a detailed insight on the high level of O₃ during summer in Shanghai, O₃ and its precursors were measured at a suburban site in Shanghai from July 1, 2016 to July 31, 2016. Using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model and concentration weighted trajectories (CWT), we found that Zhejiang province was the main potential source of O₃ in suburban Shanghai. When the sampling site was controlled by south-western winds exceeding 2 m/s, the O₃-rich air masses from upwind regions (such as Zhejiang province) could be transported to the suburban Shanghai. The propylene-equivalent concentration (PEC) and ozone formation potential (OFP) were further calculated for each VOC species, and the results suggested that propylene, (m+p)-xylene, and toluene played dominant roles in O₃ formation. The Ozone Isopleth Plotting Research (OZIPR) model was used to reveal the impact of O₃ precursors on O₃ formation, and 4 base-cases were selected to adjust the model simulation. An average disparity of 18.20% was achieved between the simulated and observed O₃ concentrations. The O₃ isopleth diagram illustrated that O₃ formation in July 2016 was in VOC-sensitive regime, although the VOC/NO_x ratio was greater than 20. By introducing sensitivity (S), a sensitivity analysis was performed for O₃ formation. We found that O₃ formation was sensitive to propylene, (m+p)-xylene, o-xylene and toluene. The results provide theoretical support for O₃ pollution treatment in Shanghai.     

大连星海地区环境空气中挥发性有机物的臭氧生成潜势研究

以该实验的观测资料为基础,通过数据分析表明,对大连星海地区OH自由基消耗的主要环境VOCs组分是烯烃类物质,对O3生成潜势贡献最高的环境VOCs组分是芳香烃类物质;综合LiOH及OFP值评价,识别影响大连星海地区O3生成的关键环境VOCs反应活性物种为丙烯、甲苯、间对二甲苯等物质。     

Heterogeneous oxidation of SO2 by O3-aged black carbon and its dithiothreitol oxidative potential

Ozone (O₃) is an important atmospheric oxidant. Black carbon (BC) particles released into the atmosphere undergo an aging process via O₃ oxidation. O₃-aged BC particles may change their uptake ability toward trace reducing gases such as SO₂ in the atmosphere, leading to different environmental and health effects. In this paper, the heterogeneous reaction process between O₃-aged BC and SO₂ was explored via in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Combined with ion chromatography (IC), DRIFTS was used to qualitatively and quantitatively analyze the sulfate product. The results showed that O₃-aged BC had stronger SO₂ oxidation ability than fresh BC, and the reactive species/sites generated on the surface had an important role in the oxidation of SO₂. Relative humidity or 254 nm UV (ultraviolet) light illumination enhanced the oxidation uptake of SO₂ on O₃-aged BC. The oxidation potentials of the BC particles were detected via dithiothreitol (DTT) assay. The DTT activity over BC was decreased in the process of SO₂ reduction, with the consumption of oxidative active sites.     

Ozone concentrations, flux and potential effect on yield during wheat growth in the Northwest-Shandong Plain of China

Ozone (O₃) concentration and flux (F_o) were measured using the eddy covariance technique over a wheat field in the Northwest-Shandong Plain of China. The O₃-induced wheat yield loss was estimated by utilizing O₃ exposure-response models. The results showed that: (1) During the growing season (7 March to 7 June, 2012), the minimum (16.1 ppbV) and maximum (53.3 ppbV) mean O₃ concentrations occurred at approximately 6:30 and 16:00, respectively. The mean and maximum of all measured O₃ concentrations were 31.3 and 128.4 ppbV, respectively. The variation of O₃ concentration was mainly affected by solar radiation and temperature. (2) The mean diurnal variation of deposition velocity (V_d) can be divided into four phases, and the maximum occurred at noon (12:00). Averaged V_d during daytime (6:00–18:00) and nighttime (18:00–6:00) were 0.42 and 0.14 cm/sec, respectively. The maximum of measured V_d was about 1.5 cm/sec. The magnitude of V_d was influenced by the wheat growing stage, and its variation was significantly correlated with both global radiation and friction velocity. (3) The maximum mean F_o appeared at 14:00, and the maximum measured F_o was − 33.5 nmol/(m²·sec). Averaged F_o during daytime and nighttime were − 6.9 and − 1.5 nmol/(m²·sec), respectively. (4) Using O₃ exposure-response functions obtained from the USA, Europe, and China, the O₃-induced wheat yield reduction in the district was estimated as 12.9% on average (5.5%–23.3%). Large uncertainties were related to the statistical methods and environmental conditions involved in deriving the exposure-response functions.     

Prediction of future disposal of end-of-life refrigerators containing CFC-11

The objective of this study was to predict the number of refrigerators containing CFC-11 blown isolation foam and the amount of CFC-11 banked in these refrigerators. By using a Weibull-based survival function, the number of CFC-11 containing and still-functioning refrigerators was estimated to be approximately 1.6 million in 2013 in Turkey. In order to determine the amount of CFC-11 in the isolation foam of these refrigerators, polyurethane (PU) foam samples were taken from a refrigerator manufactured in 1993 and the quantity of CFC-11 was analyzed by a GC-MS. It was determined that 113–195 mg CFC-11/g PU remains in the PU foam depending on the location such as door, sides, top and bottom. Knowing that a mid-sized refrigerator contains 4 kg PU on average, the total amount of PU foam to be disposed of is 6344 tons when the CFC-11 containing refrigerators in Turkey become obsolete in the near future. Furthermore, 717–1237 tons of CFC-11 are expected to be banked in the PU foam of these refrigerators which will exert an equivalent amount of ozone depleting potential (ODP). In addition, the global warming potential will vary between 3.4 and 5.9 million tons of CO₂.     

许昌市臭氧污染趋势及时空分布特征研究

为研究许昌市的臭氧(O3)污染情况及时空分布特征,对2014年-2016年许昌市3个国家环境空气监测点位的监测数据进行了统计分析.结果表明:2014年-2016年,许昌市O3污染状况整体呈加重趋势,2016年污染最为严重;O3浓度和超标天数均具有明显的季节变化特征,春末和夏季的O3污染最为严重;不同季节的O3、NO2、NO和NOx浓度日变化也不尽相同,同时O3具有明显的日变化特征,呈单峰型分布,峰值出现在14:00~15:00;并且O3与NO2具有较好的相关性.     

Combining sap flow and eddy covariance approaches to derive stomatal and non-stomatal O3 fluxes in a forest stand

Stomatal O₃ fluxes to a mixed beech/spruce stand (Fagus sylvatica/Picea abies) in Central Europe were determined using two different approaches. The sap flow technique yielded the tree-level transpiration, whereas the eddy covariance method provided the stand-level evapotranspiration. Both data were then converted into stomatal ozone fluxes, exemplifying this novel concept for July 2007. Sap flow-based stomatal O₃ flux was 33% of the total O₃ flux, whereas derivation from evapotranspiration rates in combination with the Penman-Monteith algorithm amounted to 47%. In addition to this proportional difference, the sap flow-based assessment yielded lower levels of stomatal O₃ flux and reflected stomatal regulation rather than O₃ exposure, paralleling the daily courses of canopy conductance for water vapor and eddy covariance-based total stand-level O₃ flux. The demonstrated combination of sap flow and eddy covariance approaches supports the development of O₃ risk assessment in forests from O₃ exposure towards flux-based concepts.     

Effect of ambient-level gas-phase peroxides on foliar injury, growth, and net photosynthesis in Japanese radish (Raphanus sativus)

To investigate the effects of ambient-level gas-phase peroxides concurrent with O₃ on foliar injury, photosynthesis, and biomass in herbaceous plants, we exposed Japanese radish (Raphanus sativus) to clean air, 50 ppb O₃, 100 ppb O₃, and 2-3 ppb peroxides + 50 ppb O₃ in outdoor chambers. Compared with exposure to 100 ppb O₃, exposure to 2-3 ppb peroxides + 50 ppb O₃ induced greater damage in foliar injury, net photosynthetic rates and biomass; the pattern of foliar injury and the cause of net photosynthetic rate reduction also differed from those occurring with O₃ exposure alone. These results indicate for the first time that sub-ppb peroxides + 50 ppb O₃ can cause more severe damage to plants than 100 ppb O₃, and that not only O₃, but also peroxides, could be contributing to the herbaceous plant damage and forest decline observed in Japan's air-polluted urban and remote mountains areas.