Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO
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Harris, Eliza; Sinha, B.; Pinxteren, Dominik van; Tilgner, Andreas; Fomba, Khanneh Wadinga; Schneider, Johannes; Roth, Anja; Gnauk, T.; Fahlbusch, B.; Mertes, Stephan; Lee, Taehyoung; Collett, Jeffrey L.; Foley, Stephen F.; Borrmann, Stephan; Hoppe, P.; Herrmann, Hartmut

doi:10.1126/science.1230911

Cited by 314 publications

(330 citation statements)

References 83 publications

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“…The model's underestimation during the severe winter haze episodes is consistent with previous studies (Liu et al, 2010;Zhou et al, 2014). Possible reasons for this underestimation are (1) the bias in simulating meteorological conditions during haze episodes; (2) un- certainties in emissions; (3) missing SOA in the MOSAIC mechanism, which will be addressed below; and (4) the lack of formation mechanisms of secondary inorganic aerosols, like heterogeneous oxidation of SO 2 on the surface of particulate matter (Harris et al, 2013). By adjusting SO 2 and NO x emissions according to surface observations and parameterizing the heterogeneous oxidation of SO 2 on deliquesced aerosols in the GEOS-Chem model, Y. X. reported improvements of simulated PM 2.5 spatial distribution and an increase of 120 % in sulfate fraction in PM 2.5 .…”

Section: Pm 25supporting

confidence: 77%

Simulating aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe haze conditionsin winter

2015

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Abstract. The aerosol-radiation-cloud feedbacks on meteorology and air quality over eastern China under severe winter haze conditions in January 2013 are simulated using the fully coupled online Weather Research and Forecasting/Chemistry (WRF-Chem) model. Three simulation scenarios including different aerosol configurations are undertaken to distinguish the aerosol's radiative (direct and semi-direct) and indirect effects. Simulated spatial and temporal variations of PM 2.5 are generally consistent with surface observations, with a mean bias of −18.9 µg m −3 (−15.0 %) averaged over 71 big cities in China. Comparisons between different scenarios reveal that aerosol radiative effects (direct effect and semidirect effects) result in reductions of downward shortwave flux at the surface, 2 m temperature, 10 m wind speed and planetary boundary layer (PBL) height by up to 84.0 W m −2 , 3.2 • C, 0.8 m s −1 , and 268 m, respectively. The simulated impact of the aerosol indirect effects is comparatively smaller. Through reducing the PBL height and stabilizing lower atmosphere, the aerosol effects lead to increases in surface concentrations of primary pollutants (CO and SO 2 ). Surface O 3 mixing ratio is reduced by up to 6.9 ppb (parts per billion) due to reduced incoming solar radiation and lower temperature, while the aerosol feedbacks on PM 2.5 mass concentrations show some spatial variations. Comparisons of model results with observations show that inclusion of aerosol feedbacks in the model significantly improves model performance in simulating meteorological variables and improves simulations of PM 2.5 temporal distributions over the North China Plain, the Yangtze River delta, the Pearl River delta, and central China. Although the aerosol-radiationcloud feedbacks on aerosol mass concentrations are subject to uncertainties, this work demonstrates the significance of aerosol-radiation-cloud feedbacks for real-time air quality forecasting under haze conditions.

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Section: Pm 25supporting

confidence: 77%

Simulating aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe haze conditionsin winter

2015

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“…were found to be the most important sources for in-cloud addition of sulfate to mixed particles (the most common particle type during HCCT-2010), while in-cloud aqueous oxidation of SO 2 primarily catalysed by transition metal ions (Harris et al, 2013b) was most important for coarse mineral dust. The isotopic analyses showed that the sulfate content of particles increased following cloud processing during HCCT-2010 by > 10-40 % depending on particle type (cf.…”

Section: Chemical In-cloud Processing Of the Particlesmentioning

confidence: 99%

Influence of cloud processing on CCN activation behaviour in the Thuringian Forest, Germany during HCCT-2010

et al. 2014

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Abstract. Within the framework of the "Hill Cap Cloud Thuringia 2010" (HCCT-2010) international cloud experiment, the influence of cloud processing on the activation properties of ambient aerosol particles was investigated. Particles were probed upwind and downwind of an orographic cap cloud on Mt Schmücke, which is part of a large mountain ridge in Thuringia, Germany. The activation properties of the particles were investigated by means of size-segregated cloud condensation nuclei (CCN) measurements at 3 to 4 different supersaturations. The observed CCN spectra together with the total particle spectra were used to calculate the hygroscopicity parameter κ for the upwind and downwind stations. The upwind and downwind critical diameters and κ values were then compared for defined cloud events (FCE) and noncloud events (NCE). Cloud processing was found to increase the hygroscopicity of the aerosol particles significantly, with an average increase in κ of 50 %. Mass spectrometry analysis and isotopic analysis of the particles suggest that the observed increase in the hygroscopicity of the cloud-processed particles is due to an enrichment of sulfate and possibly also nitrate in the particle phase.

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“…The contribution of anthropogenic and natural Fe-containing particle sources (Moteki et al, 2017) to observed Fe-containing residues is expected. The presence of Fe in the cloud droplets plays an important role in aqueous-phase SO 2 catalytic oxidation in cloud processing (Harris et al, 2013), thus accelerating the sulfate content of Fe-containing particles in cloud processing.…”

Section: The Chemical Characterization Of Cloud Droplet Residuesmentioning

confidence: 99%

In situ chemical composition measurement of individual cloud residue particles at a mountain site, southern China

et al. 2017

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Abstract. To investigate how atmospheric aerosol particles interact with chemical composition of cloud droplets, a ground-based counterflow virtual impactor (GCVI) coupled with a real-time single-particle aerosol mass spectrometer (SPAMS) was used to assess the chemical composition and mixing state of individual cloud residue particles in the Nanling Mountains (1690 m a.s.l.), southern China, in January 2016. The cloud residues were classified into nine particle types: aged elemental carbon (EC), potassium-rich (K-rich), amine, dust, Pb, Fe, organic carbon (OC), sodiumrich (Na-rich) and "Other". The largest fraction of the total cloud residues was the aged EC type (49.3 %), followed by the K-rich type (33.9 %). Abundant aged EC cloud residues that mixed internally with inorganic salts were found in air masses from northerly polluted areas. The number fraction (NF) of the K-rich cloud residues increased within southwesterly air masses from fire activities in Southeast Asia. When air masses changed from northerly polluted areas to southwesterly ocean and livestock areas, the amine particles increased from 0.2 to 15.1 % of the total cloud residues. The dust, Fe, Pb, Na-rich and OC particle types had a low contribution (0.5-4.1 %) to the total cloud residues. Higher fraction of nitrate (88-89 %) was found in the dust and Na-rich cloud residues relative to sulfate (41-42 %) and ammonium (15-23 %). Higher intensity of nitrate was found in the cloud residues relative to the ambient particles. Compared with nonactivated particles, nitrate intensity decreased in all cloud residues except for dust type. To our knowledge, this study is the first report on in situ observation of the chemical composition and mixing state of individual cloud residue particles in China.

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Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO ₂

Cited by 314 publications

References 83 publications

Simulating aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe haze conditionsin winter

Simulating aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe haze conditionsin winter

Influence of cloud processing on CCN activation behaviour in the Thuringian Forest, Germany during HCCT-2010

In situ chemical composition measurement of individual cloud residue particles at a mountain site, southern China

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Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO 2

Cited by 314 publications

References 83 publications

Simulating aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe haze conditionsin winter

Simulating aerosol–radiation–cloud feedbacks on meteorology and air quality over eastern China under severe haze conditionsin winter

Influence of cloud processing on CCN activation behaviour in the Thuringian Forest, Germany during HCCT-2010

In situ chemical composition measurement of individual cloud residue particles at a mountain site, southern China

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Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO ₂