CORC  > 北京大学  > 环境科学与工程学院
On the formation of sulphuric acid - amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation
Paasonen, P. ; Olenius, T. ; Kupiainen, O. ; Kurten, T. ; Petaja, T. ; Birmili, W. ; Hamed, A. ; Hu, M. ; Huey, L. G. ; Plass-Duelmer, C. ; Smith, J. N. ; Wiedensohler, A. ; Loukonen, V. ; McGrath, M. J. ; Ortega, I. K. ; Laaksonen, A. ; Vehkamaki, H. ; Kerminen, V.M. ; Kulmala, M.
刊名atmospheric chemistry and physics
2012
关键词AEROSOL NUCLEATION CCN CONCENTRATIONS SIZE DISTRIBUTION GLOBAL SCALES GROWTH-RATES H2SO4 AMMONIA MODEL MECHANISMS CLIMATE
DOI10.5194/acp-12-9113-2012
英文摘要Sulphuric acid is a key component in atmospheric new particle formation. However, sulphuric acid alone does not form stable enough clusters to initiate particle formation in atmospheric conditions. Strong bases, such as amines, have been suggested to stabilize sulphuric acid clusters and thus participate in particle formation. We modelled the formation rate of clusters with two sulphuric acid and two amine molecules (J(A2B2)) at varying atmospherically relevant conditions with respect to concentrations of sulphuric acid ([H2SO4]), dimethylamine ([DMA]) and trimethylamine ([TMA]), temperature and relative humidity (RH). We also tested how the model results change if we assume that the clusters with two sulphuric acid and two amine molecules would act as seeds for heterogeneous nucleation of organic vapours (other than amines) with higher atmospheric concentrations than sulphuric acid. The modelled formation rates J(A2B2) were functions of sulphuric acid concentration with close to quadratic dependence, which is in good agreement with atmospheric observations of the connection between the particle formation rate and sulphuric acid concentration. The coefficients K-A2B2 connecting the cluster formation rate and sulphuric acid concentrations as J(A2B2) = K-A2B2[H2SO4](2) turned out to depend also on amine concentrations, temperature and relative humidity. We compared the modelled coefficients K-A2B2 with the corresponding coefficients calculated from the atmospheric observations (K-obs) from environments with varying temperatures and levels of anthropogenic influence. By taking into account the modelled behaviour of J(A2B2) as a function of [H2SO4], temperature and RH, the atmospheric particle formation rate was reproduced more closely than with the traditional semi-empirical formulae based on sulphuric acid concentration only. The formation rates of clusters with two sulphuric acid and two amine molecules with different amine compositions (DMA or TMA or one of both) had different responses to varying meteorological conditions and concentrations of vapours participating in particle formation. The observed inverse proportionality of the coefficient K-obs with RH and temperature agreed best with the modelled coefficient K-A2B2 related to formation of a cluster with two H2SO4 and one or two TMA molecules, assuming that these clusters can grow in collisions with abundant organic vapour molecules. In case this assumption is valid, our results suggest that the formation rate of clusters with at least two of both sulphuric acid and amine molecules might be the rate-limiting step for atmospheric particle formation. More generally, our analysis elucidates the sensitivity of the atmospheric particle formation rate to meteorological variables and concentrations of vapours participating in particle formation (also other than H2SO4).; Meteorology & Atmospheric Sciences; SCI(E); 32; ARTICLE; 19; 9113-9133; 12
语种英语
内容类型期刊论文
源URL[http://ir.pku.edu.cn/handle/20.500.11897/393869]  
专题环境科学与工程学院
推荐引用方式
GB/T 7714
Paasonen, P.,Olenius, T.,Kupiainen, O.,et al. On the formation of sulphuric acid - amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation[J]. atmospheric chemistry and physics,2012.
APA Paasonen, P..,Olenius, T..,Kupiainen, O..,Kurten, T..,Petaja, T..,...&Kulmala, M..(2012).On the formation of sulphuric acid - amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation.atmospheric chemistry and physics.
MLA Paasonen, P.,et al."On the formation of sulphuric acid - amine clusters in varying atmospheric conditions and its influence on atmospheric new particle formation".atmospheric chemistry and physics (2012).
个性服务
查看访问统计
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

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。


©版权所有 ©2017 CSpace - Powered by CSpace