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Heterogeneous reaction of peroxyacetic acid and hydrogen peroxide on ambient aerosol particles under dry and humid conditions: kinetics, mechanism and implications
Wu, Q. Q. ; Huang, L. B. ; Liang, H. ; Zhao, Y. ; Huang, D. ; Chen, Z. M.
刊名ATMOSPHERIC CHEMISTRY AND PHYSICS
2015
关键词VOLATILE ORGANIC-COMPOUNDS ARIZONA TEST DUST PERACETIC-ACID RELATIVE-HUMIDITY CHEMICAL-CHARACTERIZATION TROPOSPHERIC DEGRADATION CATALYTIC DECOMPOSITION CALCIUM-CARBONATE PHASE OXIDATION HO2 RADICALS
DOI10.5194/acp-15-6851-2015
英文摘要Hydrogen peroxide (H2O2) and organic peroxides play important roles in the cycle of oxidants and the formation of secondary aerosols in the atmosphere. Recent field observations have suggested that the budget of peroxyacetic acid (PAA, CH3C(O)OOH) is potentially related to the aerosol phase processes, especially to secondary aerosol formation. Here, we present the first laboratory measurements of the uptake coefficient of gaseous PAA and H2O2 onto ambient fine particulate matter (PM2.5) as a function of relative humidity (RH) at 298 K. The results show that the PM2.5, which was collected in an urban area, can take up PAA and H2O2 at the uptake coefficient (gamma) of 10(-4), and both gamma(PAA) and gamma O-H2(2) increase with increasing RH. The value of gamma(PAA) at 90 % RH is 5.4 +/- 1.9 times that at 3 % RH, whereas gamma O-H2(2) at 90 % RH is 2.4 +/- 0.5 times that at 3 % RH, which suggests that PAA is more sensitive to the RH variation than H2O2 is. Considering the larger Henry's law constant of H2O2 than that of PAA, the smaller RH sensitivity of the H2O2 uptake coefficient suggests that the enhanced uptake of peroxide compounds on PM2.5 under humid conditions is dominated by chemical processes rather than dissolution. Considering that mineral dust is one of the main components of PM2.5 in Beijing, we also determined the uptake coefficients of gaseous PAA and H2O2 on authentic Asian Dust storm (ADS) and Arizona Test Dust (ATD) particles. Compared to ambient PM2.5, ADS shows a similar gamma value and RH dependence in its uptake coefficient for PAA and H2O2, while ATD gives a negative dependence on RH. The present study indicates that, in addition to the mineral dust in PM2.5, other components (e.g., soluble inorganic salts) are also important to the uptake of peroxide compounds. When the heterogeneous reaction of PAA on PM2.5 is considered, its atmospheric lifetime is estimated to be 3.0 h on haze days and 7.1 h on non-haze days, values that are in good agreement with the field observations.; National Natural Science Foundation of China [41275125, 21190053, 21477002]; State Key Laboratory of Environment Simulation and Pollution Control; SCI(E); ARTICLE; zmchen@pku.edu.cn; 12; 6851-6866; 15
语种英语
内容类型期刊论文
源URL[http://ir.pku.edu.cn/handle/20.500.11897/421159]  
专题环境科学与工程学院
推荐引用方式
GB/T 7714
Wu, Q. Q.,Huang, L. B.,Liang, H.,et al. Heterogeneous reaction of peroxyacetic acid and hydrogen peroxide on ambient aerosol particles under dry and humid conditions: kinetics, mechanism and implications[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2015.
APA Wu, Q. Q.,Huang, L. B.,Liang, H.,Zhao, Y.,Huang, D.,&Chen, Z. M..(2015).Heterogeneous reaction of peroxyacetic acid and hydrogen peroxide on ambient aerosol particles under dry and humid conditions: kinetics, mechanism and implications.ATMOSPHERIC CHEMISTRY AND PHYSICS.
MLA Wu, Q. Q.,et al."Heterogeneous reaction of peroxyacetic acid and hydrogen peroxide on ambient aerosol particles under dry and humid conditions: kinetics, mechanism and implications".ATMOSPHERIC CHEMISTRY AND PHYSICS (2015).
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