Sulfur dioxide in rain clouds: Gas-liquid scavenging efficiencies and wet deposition rates in the presence of formaldehyde

Warneck, Peter

doi:10.1007/bf00053717

Cited by 25 publications

(6 citation statements)

References 53 publications

(62 reference statements)

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“…It should be pointed out that although the half-times are not a strong function of ionic strength, the composition of trace anions can be quite important. The levels of S(IV) in acidic fog and cloud waters [Munger et al, 1984;Warneck, 1989] have been shown to reach concentrations as high as 3000/aM, while the values in marine aerosol are normally less than 1 /aM. These calculations indicate that the higher levels of Fe(II) found in water droplets [Behra and $igg, 1990] compared to marine aerosols [Zhu et al, 1992] may be due to the reduction of Fe(III) by S(IV).…”

Section: Chemicalsmentioning

confidence: 97%

Reduction of Fe(III) with sulfite in natural waters

Millero¹,

González‐Dávila²,

Santana‐Casiano³

1995

J. Geophys. Res.

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The Fe(III) in marine aerosols and rainwaters can be reduced to Fe(II) by photochemical processes and by reactions with sulfite. In this paper, measurements of the rates of reduction of nanomolar levels of Fe(III) with sulfite (without 02) have been determined in NaC1 and seawater solutions as a function of temperature (0 ø to 40øC) + 2+ ' pH (2 to 6.8), ionic strength (I = 0.1 to 6 M), and composition (Na , Mg , Ca 2+, F-, CI-, Br-, HCO•-, SO4:-). The overall rate constant (k, M -1 min -1) for the reaction, Fe(III) + S(IV)-• products, is given by d[Fe(III)]/dt = -k[Fe(III)] [S(IV)]. The reaction was found to be first order with respect to Fe(III) and S(IV). The rate constants as a function of p H increased from a p H = 2 to 4 and decreased at higher p H. The effect of temperature and ionic strength on the rates could be represented by log k -log k ø + AIø'5/(1 + Iø'•), where A = -1.1 in NaC1 and -2.2 in seawater and 10g k ø -25.39 -6,323/T. The energy of activation was found by 121 __+ 6 kJ mol -• . The measured rates in seawater as a function of salinity were lower than the rates in NaC1 at the same ionic strength. Measurements in NaC1 solutions with added sea-salt ions (Mg 2+ , C_a •+, F-, Br-, and SO4:-) at pH = 3.5 indicate that the formation of inert FeF 2+ may be responsible for the lower rates. The effect of changes in the composition on the rates was interpreted by examining the speciation of Fe(III) and S(IV). Thi_s analysis indicates that the rate-determining steps from a p H of 2.5 to 4.0 are FeOH 2+ + HSO•-< • HOFeSO3H + and HOFeSO3H + • FeOH + + HSO3' and at pH of 4 to 6, the reactions Fe(OH)• + HSO•-< • (HO):FeSO3 H and (HO):FeSO3H •Fe(OH): + HSO3' become important. The changes in the concentration of FeOH 2+ and HSO•-as a function of pH and composition can account for most of the changes in the rates. These kinetic studies indicate that the rates of reduction of Fe(III) with S(IV) in acidic water droplets at natural levels of S(IV) may be an important source of Fe(II).1Also at

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Section: Chemicalsmentioning

confidence: 97%

Reduction of Fe(III) with sulfite in natural waters

Millero¹,

González‐Dávila²,

Santana‐Casiano³

1995

J. Geophys. Res.

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“…HMS is an important S(IV) species near combustion sources in the presence of high levels of SO 2 and HCHO or in a polluted and humid urban atmosphere . The formation of HMS has a potential impact on the enhancement of gas–liquid scavenging efficiencies of SO 2 in cloud droplets . It is therefore of high interest to understand the role of HMS in atmospheric sulfur chemistry.…”

Section: Introductionmentioning

confidence: 99%

“…10 The formation of HMS has a potential impact on the enhancement of gas−liquid scavenging efficiencies of SO 2 in cloud droplets. 11 It is therefore of high interest to understand the role of HMS in atmospheric sulfur chemistry.…”

Section: ■ Introductionmentioning

confidence: 99%

Quantitative Determination of Hydroxymethanesulfonate (HMS) Using Ion Chromatography and UHPLC-LTQ-Orbitrap Mass Spectrometry: A Missing Source of Sulfur during Haze Episodes in Beijing

Wei

Chen

et al. 2020

Environ. Sci. Technol. Lett.

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Hydroxymethanesulfonate (HMS), the product of HSO 3 − and SO 3 2− reacting with dissolved formaldehyde in fog, cloud, and aerosol liquid water, has been suggested to be an important source of particulate sulfur during haze events. However, there have been limited studies of high concentrations of HMS in atmospheric aerosol. We report here two feasible analytical methods for the identification of HMS using ion chromatography and UHPLC-LTQ-Orbitrap mass spectrometry. The concentrations of HMS in fine particles in wintertime Beijing ranged from below the detection limit to 7.3 μg m −3 (with an average at 2.0 ± 2.1 μg m −3 ). Increased concentrations of HMS and sulfate were associated with the occurrence of fog. The results reveal that HMS may be a potential S(IV) reservoir and an effective tracer of aqueous-phase chemistry. The atmospheric aqueous-phase chemistry promoted the rapid conversion of S(IV) under haze−fog conditions. The kinetic modeling results suggest that the aqueous pH should be taken into account when exploring the mechanism of HMS formation in atmospheric sulfur chemistry.

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“…In contrast to HSO 3 – and SO 3 2– , HMS is stable against oxidation by hydrogen peroxide, a primary oxidant in aqueous aerosols . It has been suggested that the formation of aldehyde–sulfite adducts in cloudwater and fogwater particles could account for up to a 2-fold increase in wet deposition of SO 2 , and that such particles may act as a vehicle for long-range transport of S(IV) species in the atmosphere, reducing the rates of S(VI) formation. ,,− …”

Section: Introductionmentioning

confidence: 99%

Uptake of SO₂ to Aqueous Formaldehyde Surfaces

Ota

Richmond

2012

J. Am. Chem. Soc.

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Aqueous surfaces act as a gateway to absorption and aqueous-phase reaction of gases in the atmosphere. The composition of aerosols varies greatly and is expected to influence the structure of the interface. For example, aldehydes comprise a significant fraction of atmospheric organics and are likely to accumulate at aqueous surfaces. But it is difficult to anticipate their effect on the migration of gaseous species through the interfacial region. Surface organics may act as a barrier to absorption, or they may facilitate uptake via cooperative interactions with absorbing compounds. The surface spectroscopic studies presented here examine the nature of the vapor/water interface during uptake of SO(2) to aqueous formaldehyde solutions, elucidating the role of surface species in a multicomponent interfacial system. The results show that the product of the reaction between SO(2) and formaldehyde, hydroxymethanesulfonate, shows a surface affinity that is enhanced in the presence of SO(2).

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Sulfur dioxide in rain clouds: Gas-liquid scavenging efficiencies and wet deposition rates in the presence of formaldehyde

Cited by 25 publications

References 53 publications

Reduction of Fe(III) with sulfite in natural waters

Reduction of Fe(III) with sulfite in natural waters

Quantitative Determination of Hydroxymethanesulfonate (HMS) Using Ion Chromatography and UHPLC-LTQ-Orbitrap Mass Spectrometry: A Missing Source of Sulfur during Haze Episodes in Beijing

Uptake of SO₂ to Aqueous Formaldehyde Surfaces

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Sulfur dioxide in rain clouds: Gas-liquid scavenging efficiencies and wet deposition rates in the presence of formaldehyde

Cited by 25 publications

References 53 publications

Reduction of Fe(III) with sulfite in natural waters

Reduction of Fe(III) with sulfite in natural waters

Quantitative Determination of Hydroxymethanesulfonate (HMS) Using Ion Chromatography and UHPLC-LTQ-Orbitrap Mass Spectrometry: A Missing Source of Sulfur during Haze Episodes in Beijing

Uptake of SO2 to Aqueous Formaldehyde Surfaces

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Uptake of SO₂ to Aqueous Formaldehyde Surfaces