Fog composition along the Yangtze River basin: Detecting emission sources of pollutants in fog water

Xu, Xilong; Chen, Jianmin; Zhu, Chongshu; Li, Jiarong; Sui, Xiao; Liu, Lu; Sun, Jianfeng

doi:10.1016/j.jes.2017.09.018

Cited by 18 publications

(13 citation statements)

References 39 publications

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“…S2. those for the following compounds: acetosyringone, acetovanillone, azelaic acid, benzoic acid, coumaric acid, hydroxybenzoic acid, ketolimononaldehyde, nitrocatechol, o-toluic acid, phthalic acid, syringaldehyde, syringic acid, tyrosine, vanillic acid, and vanillin (Table S1) (Mazzoleni et al, 2007;Desyaterik et al, 2013;Nguyen et al, 2013;Pietrogrande et al, 2014aPietrogrande et al, , b, 2015Yu et al, 2014Yu et al, , 2016Dzepina et al, 2015). The molecular formulas for common methoxyphenols (syringol (C 8 H 10 O 3 ), methylsyringol (C 9 H 12 O 3 ), and eugenol (C 10 H 12 O 2 )) were present in all samples except BO0204N; as they are both semi-volatile and water-soluble, they are not expected to be present in aerosol with low liquid water content.…”

Section: Overview Of the Compositions Of Po Valley Ambient Fog And Aementioning

confidence: 99%

“…Biomass burning products include simple organic acids, sugars and anhydrosugars, substituted phenols, polycyclic aromatic hydrocarbons, and other compounds, depending on the type of fuel and burn conditions (Mazzoleni et al, 2007;Pietrogrande et al, 2014a, b;Gilardoni et al, 2016). These water-soluble emissions can serve as precursors for SOA once dissolved in the aqueous phase (Chang and Thompson, 2010;Yu et al, 2014Yu et al, , 2016, and upwards of 50 % of organic matter in fog and cloud droplets remains unidentified (Herckes et al, 2013). Biomass burning emissions can even facilitate droplet nucleation.…”

Section: Introductionmentioning

confidence: 99%

“…Laboratory studies focusing on simplified systems of only one or two precursor components have successfully recreated some of the complexity of ambient atmospheric samples (De Haan et al, 2011;Lee et al, 2013;Nguyen et al, 2013;Hawkins et al, 2016;Yu et al, 2016). A number of recent studies focusing on the molecular composition of cloud (Lee et al, 2012;Desyaterik et al, 2013;Pratt et al, 2013;Zhao et al, 2013;Boone et al, 2015;Cook et al, 2017) and fog (Mazzoleni et al, 2010;LeClair et al, 2012;Xu et al, 2017) chemistry have been reported. Together these studies indicate a clear importance of aqueous-phase reactions for the production of aqueous SOA, including the formation of organonitrates, organosulfates, and nitrooxy organosulfates.…”

Section: Introductionmentioning

confidence: 99%

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Molecular insights on aging and aqueous-phase processing from ambient biomass burning emissions-influenced Po Valley fog and aerosol

et al. 2018

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Abstract. To study the influence of regional biomass burning emissions and secondary processes, ambient samples of fog and aerosol were collected in the Po Valley (Italy) during the 2013 Supersito field campaign. After the extent of fresh vs. aged biomass burning influence was estimated from proton nuclear magnetic resonance (1H NMR) and high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS), two samples of fog water and two samples of PM1 aerosol were selected for ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) analysis. Molecular compositions indicated that the water-soluble organic matter was largely non-polymeric without clearly repeating units. The selected samples had an atypically large frequency of molecular formulas containing nitrogen and sulfur (not evident in the NMR composition) attributed to multifunctional organonitrates and organosulfates. Higher numbers of organonitrates were observed in aerosol, and higher numbers of organosulfates were observed in fog water. Consistent with the observation of an enhanced aromatic proton signature in the 1H-NMR analysis, the average molecular formula double-bond equivalents and carbon numbers were higher in the fresh biomass-burning-influenced samples. The average O : C and H : C values from FT-ICR MS were higher in the samples with an aged influence (O : C = 0.50–0.58, and H : C = 1.31–1.37) compared to those with fresh influence (O : C = 0.43–0.48, and H : C = 1.13–1.30). The aged fog had a large set of unique highly oxygenated CHO fragments in the HR-ToF-AMS, which reflects an enrichment of carboxylic acids and other compounds carrying acyl groups, highlighted by the NMR analysis. Fog compositions were more oxidized and SOA (secondary organic aerosol)-like than aerosols as indicated by their NMR measured acyl-to-alkoxyl ratios and the observed molecular formula similarity between the aged aerosol and fresh fog, implying that fog nuclei must be somewhat aged. Overall, functionalization with nitrate and sulfate moieties, in addition to aqueous oxidation, triggers an increase in the molecular complexity in this environment, which is apparent in the FT-ICR MS results. This study demonstrates the significance of the aqueous phase in transforming the molecular chemistry of atmospheric organic matter and contributing to secondary organic aerosol.

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Section: Overview Of the Compositions Of Po Valley Ambient Fog And Aementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Molecular insights on aging and aqueous-phase processing from ambient biomass burning emissions-influenced Po Valley fog and aerosol

et al. 2018

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“…Here we develop a chemical kinetic model using the results from our quantum chemical modeling to simulate the effects of HMS/HMSA and HMSi/HMHSi formation on the aerosols (refer to SI for the reaction scheme). In the simulations, we made the following assumptions based on the concentrations during a typical haze event: the droplet diameter = 2.5 μm, temperature = 298.15 K, the pressure = 1.0 atm, [SO 2 ] = 50 ppb, the total amount of formaldehyde and methanediol in the droplet = 5.0 × 10 −5 μM 17,18 , the uptake coefficient 19 of SO 2 adsorption = 5.0 × 10 −3 , initial pH = 5.0. The initial concentrations of all the products (i.e.…”

Section: Resultsmentioning

confidence: 99%

Theoretical investigation of a potentially important formation pathway of organosulfate in atmospheric aqueous aerosols

Chen

Zhao

2020

Sci Rep

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Organic sulfate plays important roles in modulating properties of atmospheric aerosols. Recent studies showed that organic sulfate was likably interpreted as inorganic sulfate in field measurements using advanced instruments such as Aerosol Mass Spectrometer and the major contributor to organic sulfate was thought to be hydroxymethanesulfonate (HMS). This study proposed that besides HMS, its isomer hydroxymethyl sulfite (HMSi), which has not been identified in atmospheric aerosols, can emerge as the product of aqueous reactions between sulfur dioxide and formaldehyde. Results from quantum chemical modeling showed that formation of HMS and HMSi was several orders of magnitude faster than that of their corresponding conjugate acids, HMSA and HMHSi. In addition, water involvement can largely accelerate respectively the formation rate of HMS/HMSA and HMSi, but decelerate that of HMHSi, demonstrating the non-negligible role of water in the formation process. Furthermore, our kinetic model implemented with the calculated parameters indicates that HMSi/HMHSi but not HMS/HMSA can significantly alter the pH values of atmospheric aqueous aerosols and HMHSi is the most abundant species among HMS/HMSA and HMSi/HMHSi. Therefore, the newly-discovered pathway via HMSi/HMHSi formation should be of great concern and its kinetic parameters should be implemented in future models of atmospheric chemistry.

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“…Aerosol particles (particulate matter) provide surfaces for the adsorption of gases and atmospheric species, thereby, serving as a catalyst for heterogeneous chemical reactions. Particulate matter is the main source of condensation nuclei on with other established methods for cloud water analysis such as ICP-MS, ICP-OES as well as AAS (Xu et al, 2018), sample preparation steps are few and fast.…”

Section: Introductionmentioning

confidence: 99%

Application of TXRF in monitoring trace metals in particulate matter and cloud water

Fomba¹,

Deabji²,

Barcha³

et al. 2020

Preprint

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Ambient particulate matter and cloud trace metals are considered key elements of atmospheric processes as they affect air quality, environmental ecosystems and play an important role in cloud formation. However, they are often available at trace concentrations in these media such that their analysis requires high precision and 15 sensitive techniques. In this study, different analytical methods were applied to quantify trace metals in particulate matter samples collected on quartz and polycarbonate filters as well as cloud water, using the Total reflection X-Ray Fluorescence (TXRF) technique. These methods considered the direct measurement of filter samples with and without chemical pretreatment. Direct measurements involved analysis of as collected polycarbonate and cloud water samples after they are brought onto TXRF carrier substrates. For the chemical treatment, different acid 20 digestion procedures for PM on Quartz filters were assessed including reverse aqua regia, nitric acid and a combination of nitric acid and hydrogen peroxide solution. The effect of cold-plasma treatment of samples on polycarbonate filters prior to TXRF measurements was also investigated.Digestion with the reverse aqua regia solution provided lower blanks and higher recovery in comparison to other tested procedures. The detection limits of the elements ranged from 0.3 to 44 ng/cm². Ca, K, Zn, and Fe showed 25 the highest detection limits of 44, 35, 6 and 1 ng/cm² while As and Se had the lowest of 0.3 and 0.8 ng/cm², respectively. The method showed higher recovery for most trace metals when applied to commercially available reference materials and field samples. TXRF measurements showed good agreement with results obtained from ion chromatography measurements for elements such as Ca and K. Cold plasma treatment did not significantly lead to an increase in the detected concentration and the results were element-specific. Backing of the quartz filters 30 prior to sampling showed a reduction of more than 20% of the filter blanks for elements such as V, Sr, Mn, Zn, Sb.The methods were applied successfully on ambient particulate matter and cloud water samples collected from the Atlas Mohammed V station in Morocco and the Cape Verde Atmospheric Observatory. The obtained concentrations were within the range reported using different techniques from similar remote and background 35 regions elsewhere, especially for elements of anthropogenic origins such as V, Pb, and Zn with concentrations of up to 10, 19 and 28 ng/m³, respectively. Enrichment factor analysis indicated that crustal matter dominated the abundance of most of the elements while anthropogenic activities also contributed to the abundance of elements such as Sb, Se, and Pb. The results confirm that TXRF is a useful complementary sensitive technique for trace metal analysis of particulate matter in the microgram range as well as in cloud water droplets.

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Fog composition along the Yangtze River basin: Detecting emission sources of pollutants in fog water

Cited by 18 publications

References 39 publications

Molecular insights on aging and aqueous-phase processing from ambient biomass burning emissions-influenced Po Valley fog and aerosol

Molecular insights on aging and aqueous-phase processing from ambient biomass burning emissions-influenced Po Valley fog and aerosol

Theoretical investigation of a potentially important formation pathway of organosulfate in atmospheric aqueous aerosols

Application of TXRF in monitoring trace metals in particulate matter and cloud water

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