Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-18-2547-2018 |
Understanding in situ ozone production in the summertime through radical observations and modelling studies during the Clean air for London project (ClearfLo) | |
Whalley, Lisa K.1,2; Stone, Daniel1; Dunmore, Rachel3; Hamilton, Jacqueline3; Hopkins, James R.3,4; Lee, James D.3,4; Lewis, Alastair C.3,4; Williams, Paul5,6; Kleffmann, Joerg7; Laufs, Sebastian7; Woodward-Massey, Robert1; Heard, Dwayne E.1,2 | |
2018-02-21 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
![]() |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:4页码:2547-2571 |
文章类型 | Article |
语种 | 英语 |
国家 | England; Germany |
英文摘要 | Measurements of OH, HO2, RO(2)i (alkene and aromatic-related RO2) and total RO2 radicals taken during the ClearfLo campaign in central London in the summer of 2012 are presented. A photostationary steady-state calculation of OH which considered measured OH reactivity as the OH sink term and the measured OH sources (of which HO2+ NO reaction and HONO photolysis dominated) compared well with the observed levels of OH. Comparison with calculations from a detailed box model utilising the Master Chemical Mechanism v3.2, however, highlighted a substantial discrepancy between radical observations under lower NOx conditions ([NO] < 1 ppbv), typically experienced during the afternoon hours, and indicated that the model was missing a significant peroxy radical sink; the model overpredicted HO2 by up to a factor of 10 at these times. Known radical termination steps, such as HO2 uptake on aerosols, were not sufficient to reconcile the model-measurement discrepancies alone, suggesting other missing termination processes. This missing sink was most evident when the air reaching the site had previously passed over central London to the east and when elevated temperatures were experienced and, hence, contained higher concentrations of VOCs. Uncertainties in the degradation mechanism at low NOx of complex biogenic and diesel related VOC species, which were particularly elevated and dominated OH reactivity under these easterly flows, may account for some of the model-measurement disagreement. Under higher [NO] (> 3 ppbv) the box model increasingly underpredicted total [RO2]. The modelled and observed HO2 were in agreement, however, under elevated NO concentrations ranging from 7 to 15 ppbv. The model uncertainty under low NO conditions leads to more ozone production predicted using modelled peroxy radical concentrations (similar to 3 ppbv h(-1)) versus ozone production from peroxy radicals measured (similar to 1 ppbv h(-1)). Conversely, ozone production derived from the predicted peroxy radicals is up to an order of magnitude lower than from the observed peroxy radicals as [NO] increases beyond 7 ppbv due to the model underprediction of RO2 under these conditions. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000425788700001 |
WOS关键词 | LASER-INDUCED FLUORESCENCE ; URBAN ATMOSPHERIC CHEMISTRY ; NITROUS-ACID HONO ; MISSING OH SOURCE ; HO2 CONCENTRATIONS ; RO2 RADICALS ; BOUNDARY-LAYER ; NONMETHANE HYDROCARBONS ; ORGANIC-COMPOUNDS ; BUDGET ANALYSIS |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/24971 |
专题 | 地球科学 |
作者单位 | 1.Univ Leeds, Sch Chem, Leeds LS2 9JT, W Yorkshire, England; 2.Univ Leeds, Natl Ctr Atmospher Sci, Leeds LS2 9JT, W Yorkshire, England; 3.Univ York, Dept Chem, York YO10 5DD, N Yorkshire, England; 4.Univ York, Natl Ctr Atmospher Sci, York YO10 5DD, N Yorkshire, England; 5.Univ Manchester, Ctr Atmospher Sci, Sch Earth Atmospher & Environm Sci, Manchester M13 9PL, Lancs, England; 6.Univ Manchester, Natl Ctr Atmospher Sci, Manchester M13 9PL, Lancs, England; 7.BUW, Inst Atmospher & Environm Res, Gaussstr 20, D-42119 Wuppertal, Germany |
推荐引用方式 GB/T 7714 | Whalley, Lisa K.,Stone, Daniel,Dunmore, Rachel,et al. Understanding in situ ozone production in the summertime through radical observations and modelling studies during the Clean air for London project (ClearfLo)[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(4):2547-2571. |
APA | Whalley, Lisa K..,Stone, Daniel.,Dunmore, Rachel.,Hamilton, Jacqueline.,Hopkins, James R..,...&Heard, Dwayne E..(2018).Understanding in situ ozone production in the summertime through radical observations and modelling studies during the Clean air for London project (ClearfLo).ATMOSPHERIC CHEMISTRY AND PHYSICS,18(4),2547-2571. |
MLA | Whalley, Lisa K.,et al."Understanding in situ ozone production in the summertime through radical observations and modelling studies during the Clean air for London project (ClearfLo)".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.4(2018):2547-2571. |
条目包含的文件 | 条目无相关文件。 |
除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。
修改评论