{"title":"远程输送过程中影响电厂羽流气相化学的主要因素ⅱ。进入“城市”环境大气的释放时间和扩散速率","authors":"Alan T. Cocks, Ian S. Fletcher","doi":"10.1016/0004-6981(89)90561-1","DOIUrl":null,"url":null,"abstract":"<div><p>A gas-phase chemical kinetic scheme combined with a simple dispersion model has been used to examine the influence of season, time of release, and dispersion rate on the chemical behaviour of a power-plant plume emitted into an ambient atmosphere defined by urban emissions. Simulations were carried out over 24 h for a plume trajectory primarily over the sea at a typical Northern European latitude.</p><p>The temporal behaviour of in-plume OH radical concentrations is a complex function of the parameters studied. For daytime releases, mean OH concentrations over 24 h are predicted to be lower than the ambient values. For evening and night releases, mean OH concentrations are calculated to be greater than the corresponding ambient values for rapidly dispersing plumes.</p><p>Mean effective first-order rate constants for the gas-phase oxidation of plume SO<sub>2</sub> are estimated to be <em>ca</em> 0.4% h<sup>−1</sup>, 0.2% h<sup>−1</sup> and 0.02% h<sup>−1</sup>, for summer, autumn/spring, and winter, respectively, and are lower than the mean values calculated for the ambient troposphere.</p><p>Ozone, H<sub>2</sub>O<sub>2</sub> and PAN concentrations in power plant plumes are normally predicted to be less than the corresponding ambient values over most of the simulation period. A significant ozone excess in plumes is only expected for slowly dispersing plumes under summer conditions after 24 h.</p><p>Most of the plume and ambient NO<sub>x</sub> is predicted to be converted to HNO<sub>3</sub> in summer and autumn/spring within 24 h and concentrations of HNO<sub>3</sub> are predicted to greatly exceed those of H<sub>2</sub>SO<sub>4</sub>.</p><p>These results are compared with those obtained previously for simulations of dispersion into a ‘rural’ ambient atmosphere.</p></div>","PeriodicalId":100138,"journal":{"name":"Atmospheric Environment (1967)","volume":"23 12","pages":"Pages 2801-2812"},"PeriodicalIF":0.0000,"publicationDate":"1989-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/0004-6981(89)90561-1","citationCount":"0","resultStr":"{\"title\":\"Major factors influencing gas-phase chemistry in power plant plumes during long range transport—II. Release time and dispersion rate for dispersion into an ‘urban’ ambient atmosphere\",\"authors\":\"Alan T. Cocks, Ian S. Fletcher\",\"doi\":\"10.1016/0004-6981(89)90561-1\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A gas-phase chemical kinetic scheme combined with a simple dispersion model has been used to examine the influence of season, time of release, and dispersion rate on the chemical behaviour of a power-plant plume emitted into an ambient atmosphere defined by urban emissions. Simulations were carried out over 24 h for a plume trajectory primarily over the sea at a typical Northern European latitude.</p><p>The temporal behaviour of in-plume OH radical concentrations is a complex function of the parameters studied. For daytime releases, mean OH concentrations over 24 h are predicted to be lower than the ambient values. For evening and night releases, mean OH concentrations are calculated to be greater than the corresponding ambient values for rapidly dispersing plumes.</p><p>Mean effective first-order rate constants for the gas-phase oxidation of plume SO<sub>2</sub> are estimated to be <em>ca</em> 0.4% h<sup>−1</sup>, 0.2% h<sup>−1</sup> and 0.02% h<sup>−1</sup>, for summer, autumn/spring, and winter, respectively, and are lower than the mean values calculated for the ambient troposphere.</p><p>Ozone, H<sub>2</sub>O<sub>2</sub> and PAN concentrations in power plant plumes are normally predicted to be less than the corresponding ambient values over most of the simulation period. A significant ozone excess in plumes is only expected for slowly dispersing plumes under summer conditions after 24 h.</p><p>Most of the plume and ambient NO<sub>x</sub> is predicted to be converted to HNO<sub>3</sub> in summer and autumn/spring within 24 h and concentrations of HNO<sub>3</sub> are predicted to greatly exceed those of H<sub>2</sub>SO<sub>4</sub>.</p><p>These results are compared with those obtained previously for simulations of dispersion into a ‘rural’ ambient atmosphere.</p></div>\",\"PeriodicalId\":100138,\"journal\":{\"name\":\"Atmospheric Environment (1967)\",\"volume\":\"23 12\",\"pages\":\"Pages 2801-2812\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"1989-01-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/0004-6981(89)90561-1\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Atmospheric Environment (1967)\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/0004698189905611\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Atmospheric Environment (1967)","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/0004698189905611","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
摘要
采用气相化学动力学方案结合简单扩散模型,研究了季节、释放时间和扩散速率对电厂排放到城市排放界定的环境大气中的羽流化学行为的影响。在典型的北欧纬度,对主要在海上上空的羽流轨迹进行了24小时的模拟。羽流中OH自由基浓度的时间行为是所研究参数的复杂函数。对于白天释放,预计24小时的平均OH浓度低于环境值。对于傍晚和夜间释放,计算出的平均OH浓度大于快速扩散羽状物的相应环境值。估计在夏季、秋季/春季和冬季,羽流SO2气相氧化的平均有效一阶速率常数分别约为0.4% h - 1、0.2% h - 1和0.02% h - 1,低于对流层环境计算的平均值。在大部分模拟期间,电厂烟尘中的臭氧、H2O2和PAN浓度通常预测低于相应的环境值。在24 h后,只有在夏季条件下缓慢分散的羽流中才会出现明显的臭氧过剩。预计在夏季和秋季/春季,大部分羽流和周围的NOx将在24 h内转化为HNO3, HNO3的浓度将大大超过H2SO4的浓度。将这些结果与先前模拟扩散到“农村”环境大气中所获得的结果进行比较。
Major factors influencing gas-phase chemistry in power plant plumes during long range transport—II. Release time and dispersion rate for dispersion into an ‘urban’ ambient atmosphere
A gas-phase chemical kinetic scheme combined with a simple dispersion model has been used to examine the influence of season, time of release, and dispersion rate on the chemical behaviour of a power-plant plume emitted into an ambient atmosphere defined by urban emissions. Simulations were carried out over 24 h for a plume trajectory primarily over the sea at a typical Northern European latitude.
The temporal behaviour of in-plume OH radical concentrations is a complex function of the parameters studied. For daytime releases, mean OH concentrations over 24 h are predicted to be lower than the ambient values. For evening and night releases, mean OH concentrations are calculated to be greater than the corresponding ambient values for rapidly dispersing plumes.
Mean effective first-order rate constants for the gas-phase oxidation of plume SO2 are estimated to be ca 0.4% h−1, 0.2% h−1 and 0.02% h−1, for summer, autumn/spring, and winter, respectively, and are lower than the mean values calculated for the ambient troposphere.
Ozone, H2O2 and PAN concentrations in power plant plumes are normally predicted to be less than the corresponding ambient values over most of the simulation period. A significant ozone excess in plumes is only expected for slowly dispersing plumes under summer conditions after 24 h.
Most of the plume and ambient NOx is predicted to be converted to HNO3 in summer and autumn/spring within 24 h and concentrations of HNO3 are predicted to greatly exceed those of H2SO4.
These results are compared with those obtained previously for simulations of dispersion into a ‘rural’ ambient atmosphere.