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| 1 | VOCs源强不确定性对臭氧生成及污染防治影响的模拟分析显示文摘本文基于三维区域空气质量模式WRF-Chem,通过修改模式化学模块,量化输出过程量和诊断量,提供了一种定量分析挥发性有机化合物(VOCs)源强不确定性对O_(3)生成影响的方法.为无法定量计算VOCs源强导致的臭氧生成率[P(O_(3))]偏差,以及由此对O_(3)体积分数分布和污染控制相关联的VOCs敏感区和NOx敏感区分布的误判提供了方法参考.采用标准统计参数对WRF-Chem模式的气象场与污染场模拟性能进行了评估,相关指标均优于前人结果.以INTEX-B(intercontinental chemical transport experiment-phase B)人为源、FINNv1(fire inventory from NCAR version 1)生物质燃烧源和MEGAN(model of emissions of gases and aerosols from nature)生物源作为基准源,并以卫星观测数据作为约束,对排放源进行改进,评估了源改进前后臭氧生成率[P(O_(3))]、O_(3)体积分数和O_(3)控制敏感区指标(Ln/Q)的变化情况.仅人为VOCs(AVOCs)源增加68%后,P(O_(3))模拟峰值增升比例达13%~82%,以北京观测站点为例,P(O_(3))模拟月均峰值增加42%(22.5×10^(-9) h^(-1)).对P(O_(3))形成贡献比例最大的主要化学反应是HO2+NO(占比约68%),AVOCs源增加68%后,该反应贡献比例下降至65%.在改进源下,P(O_(3))普遍增加达到2×10^(-9)~4×10^(-9) h^(-1),O_(3)各季节增幅较大的区域均主要集中在京津冀、长三角和珠三角中心城市及周边区域,与我国大型城市区基本都是VOCs敏感区的结论一致.整体而言,VOCs源强改进后,NOx敏感区O_(3)体积分数增加幅度不大,不超过4×10^(-9),而部分VOCs敏感区增幅超过20×10^(-9).VOCs源强的不确定性会影响O_(3)形成过程中NOx和VOCs敏感区的判断,特别是VOCs源强明显低估会夸大VOCs敏感区的范围,从而降低O_(3)调控对策的有效性. | 王峰 汪健伟 杨宁 翟菁 侯灿 | 2021 | 环境科学2021,42,12: | 8 |
| 2 | An overview of emissions of SO2 and NOx and the long-range transport of oxidized sulfur and nitrogen pollutants in East Asia显示文摘The long-range transport of oxidized sulfur(sulfur dioxide(SO_2) and sulfate) and oxidized nitrogen(nitrogen oxides(NO_x ) and nitrate) in East Asia is an area of increasing scientific interest and political concern. This paper reviews various published papers, including ground- and satellite-based observations and numerical simulations. The aim is to assess the status of the anthropogenic emissions of SO_2 and NO_x and the long-range transport of oxidized S and N pollutants over source and downwind region. China has dominated the emissions of SO_2 and NO_x in East Asia and urgently needs to strengthen the control of their emissions, especially NO_x emissions. Oxidized S and N pollutants emitted from China are transported to Korea and Japan, due to persistent westerly winds, in winter and spring.However, the total contributions of China to S and N pollutants across Korea and Japan were not found to be dominant over longer time scales(e.g., a year). The source–receptor relationships for oxidized S and N pollutants in East Asia varied widely among the different studies. This is because:(1) the nonlinear effects of atmospheric chemistry and deposition processes were not well considered, when calculating the source–receptor relationships;(2) different meteorological and emission data inputs and solution schemes for key physical and chemical processes were used; and(3) different temporal and spatial scales were employed. Therefore, simulations using the same input fields and similar model configurations would be of benefit, to further evaluate the source–receptor relationships of the oxidized S and N pollutants. | Yu Qu Junling An Youjiang He Jun Zheng | 2016 | Journal of Environmental Sciences2016,28,6: | 8 |
| 3 | Effect of potential HONO sources on peroxyacetyl nitrate(PAN)formation in eastern China in winter显示文摘As an important secondary photochemical pollutant,peroxyacetyl nitrate(PAN)has been studied over decades,yet its simulations usually underestimate the corresponding observations,especially in polluted areas.Recent observations in north China found unusually high concentrations of PAN during wintertime heavy haze events,but the current model still cannot reproduce the observations,and researchers speculated that nitrous acid(HONO)played a key role in PAN formation.For the first time we systematically assessed the impact of potential HONO sources on PAN formation mechanisms in eastern China using the Weather Research and Forecasting/Chemistry(WRF-Chem)model in February of 2017.The results showed that the potential HONO sources significantly improved the PAN simulations,remarkably accelerated the RO x(sum of hydroxyl,hydroperoxyl,and organic peroxy radicals)cycles,and resulted in 80%–150%enhancements of PAN near the ground in the coastal areas of eastern China and 10%–50%enhancements in the areas around 35–40°N within 3 km during a heavy haze period.The direct precursors of PAN were aldehyde and methylglyoxal,and the primary precursors of PAN were alkenes with C>3,xylenes,propene and toluene.The above results suggest that the potential HONO sources should be considered in regional and global chemical transport models when conducting PAN studies. | Jingwei Zhang Yitian Guo Yu Qu Yong Chen Ruipeng Yu Chaoyang Xue Rui Yang Qiang Zhang Xingang Liu Yujing Mu Jing Wang Can Ye Haihan Zhao Qiangqiang Sun Ziwen Wang Junling An | 2020 | Journal of Environmental Sciences2020,32,8: | 3 |
| 4 | 卫星观测资料改进活性VOCs源排放及其对臭氧模拟影响显示文摘本文以INTEX-B(Intercontinental Chemical Transport Experiment-Phase B)人为源、FINNv1(Fire Inventory from NCAR version 1)生物质燃烧源、MEGAN(Model of Emissions of Gases and Aerosols from Nature)生物源作为基准源,用2005~2007年3a的OMI观测资料作为参考,使用WRF-chem模式,建立了卫星观测数据与地面排放VOCs源数据的回归方程,通过OMI观测资料的约束,人为源在目前污染最为严重的京津冀、长三角、珠三角3个城市群区域分别增加了1.51倍、1.87倍和1.93倍,生物质燃烧源在3个区域分别增加了12.2倍、6.15倍和2.27倍,生物源在3个区域分别增加了1.66、1.31和1.21倍,增加后的浓度分布与前人研究结论有较好的一致性.使用改进后的源清单模拟结果来看,不同季节,3个区域O3浓度均有不同幅度的增加,各季节增幅较大的区域均主要集中在京津冀、长三角和珠三角中心城市及周边区域,与我国大型城市区基本都是VOCs敏感区的结论一致.整体而言,VOCs源强改进后,NOx敏感区O3浓度增加幅度不大,不超过4×10-9,而部分VOCs敏感区增幅超过20×10-9.本文所提供的方法可进一步改进后在大气污染相关研究中,特别是模式源清单研究中广泛使用. | 王峰 汪健伟 翟菁 侯灿 | 2021 | 中国环境科学2021,41,6: | 2 |
| 5 | VOCs源强不确定性对ROx平衡影响的模拟分析显示文摘本文对区域空气质量模式WRF-Chem主要化学模块进行了改进,定量输出大气关键自由基(ROx=OH+HO_(2)+RO_(2))参与反应的主要化学过程生成率、损耗率与相关收支平衡量,为无法定量分析和比较VOCs源强的不确定性对ROx平衡影响提供了一种新的定量分析方法,由此可减小污染防治中臭氧生成敏感区的误判,有助于完善开展快速城市群建设背景下大气环境效应的研究体系.人为VOCs排放源(AVOCs)增加(减少)68%后,三大城市群中OH、HO_(2)和RO_(2)生成率增幅达到4%—280%(对应减少为2%—80%),以北京、上海、广州为三大城市群代表的城市ROx初级生成率增幅达到35%—48%(对应减少为26%—39%).3个城市中,ROx生成率贡献最大的两类化学过程均为O1D+H2O和HCHO,ALD2等的光解,ROx损耗主要关联的化学过程为OH+NO_(2)(占比达71%—85%).分析表明,当AVOCs源增加68%之后,ROx白天月平均浓度在京津冀、长三角、珠三角的增幅OH为4%—48%、4%—52%与4%—44%,HO_(2)为10%—120%、10%—140%与10%—120%,RO_(2)为20%—280%、20%—240%与10%—140%,以大气边界层内ROx白天经向月均值增幅计算,OH为1%—5%,HO_(2)为4%—16%,RO_(2)为6%—26%.AVOCs源排放量增加68%后,导致ROx收支平衡发生变化,直接影响与NOx反应的ROx的损耗率(Ln)和ROx的生成率(Q)值,部分地区从VOCs敏感区转变为NOx敏感区,这意味着AVOCs排放源的低估导致VOCs敏感区的夸大,从而降低O3调控对策的有效性,从而也说明VOCs的不确定性导致的ROx的变化对局地污染防控策略制定影响重大. | 方降龙 王峰 汪健伟 司景 张慧风 孙喆 翟菁 | 2023 | 环境化学2023,42,12: | 0 |