Kinetics of Heterogeneous Reaction of Sulfur Dioxide on Authentic Mineral Dust: Effects of Relative Humidity and Hydrogen Peroxide

2015 ◽  
Vol 49 (18) ◽  
pp. 10797-10805 ◽  
Author(s):  
Liubin Huang ◽  
Yue Zhao ◽  
Huan Li ◽  
Zhongming Chen
2009 ◽  
Vol 11 (36) ◽  
pp. 7921 ◽  
Author(s):  
A. Vlasenko ◽  
T. Huthwelker ◽  
H. W. Gäggeler ◽  
M. Ammann

2018 ◽  
Vol 5 (8) ◽  
pp. 1821-1833 ◽  
Author(s):  
Tao Wang ◽  
Yangyang Liu ◽  
Yue Deng ◽  
Hongbo Fu ◽  
Liwu Zhang ◽  
...  

Synergistic effects of the heterogeneous reaction of sulfur dioxide on mineral dust nanoparticle mixtures.


1994 ◽  
Vol 59 (11) ◽  
pp. 2357-2374 ◽  
Author(s):  
Erich Lippert ◽  
Karel Mocek ◽  
Emerich Erdös

Results are presented of an experimental kinetic study of the heterogeneous reaction between gaseous sulfur dioxide and solid anhydrous potassium carbonate. The measurements were carried out in an all glass kinetic flow apparatus with nitrogen as the carrier gas and a fixed bed of the solid working in the differential regime at atmospheric pressure and a temperature of 423 K (150 °C). The reaction course was studied in dependence on the partial pressures of sulfur dioxide (pSO2) and water vapour (pH2O) in concentration ranges pSO2 = 13 - 430 Pa and pH2O = 0 - 2 100 Pa. In the reaction, water vapour acts as a gaseous catalyst. Based on the experimental data, the corresponding kinetic equation was found together with the numerical values of the relevant rate and equilibrium adsorption constants.


2015 ◽  
Vol 15 (4) ◽  
pp. 5713-5750
Author(s):  
Q. Q. Wu ◽  
L. B. Huang ◽  
H. Liang ◽  
Y. Zhao ◽  
D. Huang ◽  
...  

Abstract. 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 suggest that peroxyacetic acid (PAA, CH3C(O)OOH) is one of the most important organic peroxides in the atmosphere, whose budget is potentially related to the aerosols. Here we present the first laboratory measurements of the uptake coefficient of gaseous PAA and H2O2 onto the 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 (γ) of 10−4, and both γPAA and γH2O2 increase with increasing RH. However, γPAA is more sensitive to the RH variation than is γH2O2, which indicates 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, 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 γ 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., inorganic soluble 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 3.3 h on haze days and 7.6 h on non-haze days, values which agree well with the field observed result.


2004 ◽  
Vol 4 (5) ◽  
pp. 1381-1388 ◽  
Author(s):  
D. J. Stewart ◽  
P. T. Griffiths ◽  
R. A. Cox

Abstract. The kinetics of uptake of gaseous N2O5 on submicron aerosols containing NaCl and natural sea salt have been investigated in a flow reactor as a function of relative humidity (RH) in the range 30-80% at 295±2K and a total pressure of 1bar. The measured uptake coefficients, γ, were larger on the aerosols containing sea salt compared to those of pure NaCl, and in both cases increased with increasing RH. These observations are explained in terms of the variation in the size of the salt droplets, which leads to a limitation in the uptake rate into small particles. After correction for this effect the uptake coefficients are independent of relative humidity, and agree with those measured previously on larger droplets. A value of γ=0.025 is recommended for the reactive uptake coefficient for N2O5 on deliquesced sea salt droplets at 298K and RH>40%.


2004 ◽  
Vol 4 (1) ◽  
pp. 569-590 ◽  
Author(s):  
D. J. Stewart ◽  
R. A. Cox

Abstract. The kinetics of uptake of gaseous N2O5 on submicron aerosols containing NaCl and natural sea salt has been investigated in a flow reactor as a function of relative humidity (RH) in the range 30-80% at 295+/-2 K and a total pressure of 1 bar. The measured uptake coefficients, γ, were larger on the aerosols containing sea salt compared to those of pure NaCl, and in both cases increased with increasing RH. These observations are explained in terms of the variation in water content and hence size of the salt droplets, which leads to a limitation in the uptake rate into small particles. After correction for this effect the uptake coefficients are independent of relative humidity, and agree with those measured previously on larger droplets. A value of γ=0.025 is recommended for the reactive uptake coefficient for N2O5 on deliquesced sea salt droplets at 298 K and RH>40%.


2015 ◽  
Vol 15 (12) ◽  
pp. 6851-6866 ◽  
Author(s):  
Q. Q. Wu ◽  
L. B. Huang ◽  
H. Liang ◽  
Y. Zhao ◽  
D. Huang ◽  
...  

Abstract. 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 (γ) of 10−4, and both γPAA and γH2O2 increase with increasing RH. The value of γPAA at 90 % RH is 5.4 ± 1.9 times that at 3 % RH, whereas γH2O2 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 γ 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.


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