Online investigations on ozonation products of pyrene and benz[a]anthracene particles with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer

Gao, Shu-Shan; Zhang, Yang; Meng, Junwang; Shu, Jinian

doi:10.1016/j.atmosenv.2009.04.021

Cited by 33 publications

(32 citation statements)

References 33 publications

(41 reference statements)

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“…This may be because the heterogeneous reaction between particulate FL and O 3 also produces oxy-and HFL products. 35,47,48 Similar with that in Figure 2A, the similar NFL isomer distributions (2-> > 3-> 8-> 7-> 1-NFL) in the presence of O 3 under different RH were observed ( Figure 5B). The decreasing amount of NFL and the increasing ratio of 2-NFL/3-NFL with the decreasing RH were also observed in the presence of O 3 , which was similar to that exposure to N 2 O 5 / NO 3 /NO 2 only (shown in Figure 2A).…”

Section: ■ Experimental Methodssupporting

confidence: 84%

Effects of Humidity and [NO₃]/[N₂O₅] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N₂O₅/NO₃/NO₂

Zhang

Sun

et al. 2014

Environ. Sci. Technol.

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Atmospheric 2-nitrofluoranthene (2-NFL) and 2-nitropyrene (2-NPY) were two important nitro-polycyclic aromatic hydrocarbons (NPAHs). Especially, 2-NFL was recognized to be the most abundant particle-associated NPAH . In previous studies, these two products were observed in the gas-phase reaction between N 2 O 5 /NO 3 /NO 2 and their parent polycyclic aromatic hydrocarbons (PAHs), while the heterogeneous reaction generated other nitro-PAH isomers (1, 3, 7, 8-NFL and 1-NPY) (Atkinson et al. 1990). To clarify the possible reasons for this difference, the heterogeneous reactions of suspended fluoranthene (FL) and pyrene (PY) particles under different relative humidity (RH; 0.5%−43%) and [NO 3 + (aq)] in the particle surface has an influence on the product distribution of FL and PY in the atmosphere. The experimental results provide evidence for the heterogeneous formations of particle-bound 2-NFL and 2-NPY. However, relative to the gas-phase formation, they will be negligible in the real atmosphere. 2-NFL and 2-NPY observed in the ambient particles should mainly derive from deposition of gas-phase reactions. Additionally, this study also clarifies the reason for different nitro-PAHs isomers observed between gas and particulate reactions. ■ INTRODUCTIONThe atmospheric chemistry between polycyclic aromatic hydrocarbons (PAHs) and gas-phase oxidants (O 3 , OH, NO 3 , and NO 2 ) is the most important source of toxic and mutagenic PAH derivatives (nitro-PAHs and oxy-PAHs) in the atmosphere. 1−6 Nitro-PAHs (NPAHs) have mutagenic potencies up to 100 000 times greater than PAHs 7−10 and constitute 10% of the total mutagenicity of inhalable particles in the ambient atmosphere. 11,12 Additionally, these nitrated species especially have strong narrow band adsorption bands in the UV−visible range, which may enhance the radiative forcing in the atmosphere and therefore contribute to significant climate effects. 13,14 Both 2-nitrofluoranthene (2-NFL) and 2-nitropyrene (2-NPY) are two ubiquitous nitro-PAH pollutants and ambient 2-NFL/2-NPY ratio is generally used to assess the contribution of the NO 3 radical chemistry for NPAHs formation. 15−18 Considering that neither 2-NFL nor 2-NPY have been directly observed from combustion emissions, 19−21 most research has focused on the contribution of the atmospheric reactions of FL and PY with gas-phase oxidants (OH or NO 3 radicals in the presence of NO 2 ). Some studies have suggested that these two nitro-PAHs were formed exclusively via atmospheric gas-phase reactions of FL and PY. 22,23 The production of 2-NFL involves the gas-phase reaction between FL and either OH or NO 3 radicals in the presence of NO 2 , whereas the production of 2-NPY mainly involves the gas-phase reaction of PY initiated by OH radical. 24−27 The formation of both 2-NFL and 2-NPY in the gas phase is a multistep addition−elimination reaction initiated by OH or NO 3 radical species. This radical-initiated reaction is postulated to proceed by an initiated-addition of OH radical (present during the day...

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Section: ■ Experimental Methodssupporting

confidence: 84%

Effects of Humidity and [NO₃]/[N₂O₅] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N₂O₅/NO₃/NO₂

Zhang

Sun

et al. 2014

Environ. Sci. Technol.

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“…The experimental setup has been described in detail elsewhere (Gao et al, 2009;Meng et al, 2009). Briefly, the aerosol reaction chamber consists of a thin-walled open head stainless steel drum (50 cm (outer diameter) Â 60 cm (height)) and a thin Tedlar polyvinyl fluoride (PVF) film bag (50 cm (diameter) Â 50 cm (length)).…”

Section: Methodsmentioning

confidence: 99%

“…However, the mass spectra of complex organic aerosols obtained with aerosol mass spectrometer equipped with an electron-impact ionizer are usually too complicate to identify organics. Utilizing a VUV photoionization source, the VUV-ATOFMS is capable of acquiring mass spectra of organic particles with less fragments or even fragment free, which are easier to assign than the ones obtained with an electron-impact source (Shu et al, 2008;Gao et al, 2009). The real-time analysis of the solid-state products is conducted and reaction products are speculated based on the mass spectra obtained.…”

Section: Introductionmentioning

confidence: 99%

Heterogeneous ozonation of suspended malathion and chlorpyrifos particles

et al. 2010

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a b s t r a c tThe heterogeneous ozonation of suspended malathion and chlorpyrifos particles are studied in real-time with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS). The pesticide particles with the diameter of hundreds of nanometers are generated by the homogeneous nucleation method using azelaic acid as nucleus. The reactions are carried out in an aerosol reaction chamber under ambient pressure (1 atm) and room temperature (298 K), respectively. The time-of-flight mass spectra of the solid-state ozonation products of malathion and chlorpyrifos are obtained. The assignments of the mass spectra reveal that the major ozonation products of malathion particles are s-(1,2-diethoxycarbonyl)ethyl-O,O-dimethylphosphorothioate (malaoxon), 2-mercapto-succinic acid diethylester, 1,2-dicarbethoxyethyl-dimethoxyphosphinyldisulfide and bis(1,2-bis-ethoxycarbonylethyl)disulfide. The experimental results reveal that water vapor can enhance the formation of malaoxon, 2-mercapto-succinic acid diethylester and bis(1,2-bis-ethoxycarbonyl-ethyl)disulfide. In the case of chlorpyrifos, the sole ozonation product observed is 3,5,6-trichloro-2-pyridyl-diethylphosphate (chlorpyrifos oxon). The pathways of heterogeneous ozonation of malathion and chlorpyrifos particles are proposed. The atmospheric lifetimes of malathion and chlorpyrifos particles towards ozone reaction are estimated based on the time-dependent mass spectrometric signals obtained.

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“…The diagram of the experimental setup is shown elsewhere (19), which is mainly composed of three parts: an aerosol generator, a reaction chamber, and monitoring instruments.…”

Section: Experimental Equipmentmentioning

confidence: 99%

Heterogeneous Reactivity of Suspended Pirimiphos-Methyl Particles with Ozone

Yang

Zhang

Meng

et al. 2010

Environ. Sci. Technol.

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Pirimiphos-methyl (PMM) is a widely used pesticide that can be released into the atmosphere in the gas phase and the condensed phase. The reaction of suspended PMM particles with ozone is investigated using an online vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer (VUV-ATOFMS) and a scanning mobility particle sizer (SMPS). . Additionally, ozonation of PMM vapor is conducted, and the rapid formation of secondary organic aerosol (SOA) is observed in the homogeneous ozonation of gas-phase PMM. The experimental results indicate that ozone is an important atmospheric oxidant for the transformation of PMM in the atmosphere.

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Online investigations on ozonation products of pyrene and benz[a]anthracene particles with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer

Cited by 33 publications

References 33 publications

Effects of Humidity and [NO₃]/[N₂O₅] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N₂O₅/NO₃/NO₂

Effects of Humidity and [NO₃]/[N₂O₅] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N₂O₅/NO₃/NO₂

Heterogeneous ozonation of suspended malathion and chlorpyrifos particles

Heterogeneous Reactivity of Suspended Pirimiphos-Methyl Particles with Ozone

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Online investigations on ozonation products of pyrene and benz[a]anthracene particles with a vacuum ultraviolet photoionization aerosol time-of-flight mass spectrometer

Cited by 33 publications

References 33 publications

Effects of Humidity and [NO3]/[N2O5] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N2O5/NO3/NO2

Effects of Humidity and [NO3]/[N2O5] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N2O5/NO3/NO2

Heterogeneous ozonation of suspended malathion and chlorpyrifos particles

Heterogeneous Reactivity of Suspended Pirimiphos-Methyl Particles with Ozone

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Effects of Humidity and [NO₃]/[N₂O₅] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N₂O₅/NO₃/NO₂

Effects of Humidity and [NO₃]/[N₂O₅] Ratio on the Heterogeneous Reaction of Fluoranthene and Pyrene with N₂O₅/NO₃/NO₂