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[1] To evaluate the wintertime regional brown haze in northern China, trace gases and aerosols were measured at an urban site between 9 and 20 November 2009. Ion chromatography and transmission electron microscopy (TEM) were used to investigate soluble ions in PM 2.5 and the mixing state of individual particles. The contrasts between clear and hazy days were examined in detail. Concentrations of the primary gases including NO (55.62 ppbv), NO 2 (54.86 ppbv), SO 2 (83.03 ppbv), and CO (2.07 ppmv) on hazy days were 2 to 6 times higher than those on clear days. In contrast, concentrations of O 3 remained low (5.71 ppbv) on hazy days. Mass concentrations of PM 2.5 (135.90 mg m −3 ) and BC (7.85 mg m −3 ) were 3 times higher on hazy days than on clear days. Based on the estimations from TEM analysis, fractions of both ammoniated sulfate (AS)-soot (20%) and AS-soot/organic matter/fly ash (20%) were larger on hazy days than on clear days (13% and 12%), implying that coagulation is an important mixing process in the polluted air. The SO 2 emissions from coal combustion for power plants, industrial activities, and household heating led to high concentrations. Also, high concentrations of secondary sulfates significantly formed in the haze. Therefore, high concentrations of acidic gases contributed to the increased mass and number of secondary aerosols. Our study indicates that metal-catalyzed oxidation in the aqueous phase is a major pathway of sulfate formation. The mixtures of aerosol particles, together with MODIS images, suggest that the hazes covered not only the industrial cities, but extended into the neighboring rural regions.

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Abstract. Particulate matter (PM) pollution in China is an emerging environmental issue which policy makers and the public have increasingly paid attention to. In order to investigate the characteristics, sources, and chemical processes of PM pollution in Guangzhou, field measurements were conducted from 20 November 2017 to 5 January 2018, with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) and other collocated instruments. Mass concentrations of non-refractory submicron particulate matter (NR-PM1) measured by the ToF-ACSM correlated well with those of PM2.5 or PM1.1 measured by filter-based methods. The organic mass fraction increased from 45 % to 53 % when the air switched from non-pollution periods to pollution episodes (EPs), indicating significant roles of organic aerosols (OAs) during the whole study. Based on the mass spectra measured by the ToF-ACSM, positive matrix factorization (PMF) with the multilinear engine (ME-2) algorithm was performed to deconvolve OA into four factors, including hydrocarbon-like OA (HOA, 12 %), cooking OA (COA, 18 %), semi-volatile oxygenated OA (SVOOA, 30 %), and low-volatility oxygenated OA (LVOOA, 40 %). Furthermore, we found that SVOOA and nitrate were significantly contributed from local traffic emissions while sulfate and LVOOA were mostly attributed to regional pollutants. Comparisons between this work and other previous studies in China show that secondary organic aerosol (SOA) fraction in total OA increases spatially across China from the north to the south. Two distinctly opposite trends for NR-PM1 formation were observed during non-pollution periods and pollution EPs. The ratio of secondary PM (SPM = SVOOA + LVOOA + sulfate + nitrate + ammonium) to primary PM (PPM = HOA + COA + chloride), together with peroxy radicals RO2∗ and ozone, increased with increasing NR-PM1 concentration during non-pollution periods, while an opposite trend of these three quantities was observed during pollution EPs. Furthermore, oxidation degrees of both OA and SOA were investigated using the f44∕f43 space and the results show that at least two OOA factors are needed to cover a large range of f44 and f43 in Guangzhou. Comparisons between our results and other laboratory studies imply that volatile organic compounds (VOCs) from traffic emissions, in particular from diesel combustion and aromatic compounds, are the most likely SOA precursors in Guangzhou. Peroxy radical RO2∗ was used as a tracer for SOA formed through gas-phase oxidation. For non-pollution periods, SOA concentration was reasonably correlated with RO2∗ concentration during both daytime and nighttime, suggesting that gas-phase oxidation was primarily responsible for SOA formation. However, there was no correlation between SOA and RO2∗ in pollution EPs, suggesting a dramatically changed mechanism for SOA formation. This conclusion can also be supported by different features of SOA in a van Krevelen diagram between non-pollution periods and pollution EPs. Furthermore, for pollution EPs, when NR-PM1 mass concentration was divided into six segments, in each segment except for the lowest one SOA concentration was correlated moderately with RO2∗ concentration, suggesting that gas-phase oxidation still plays important roles in SOA formation. The intercepts of the above linear regressions, which likely correspond to the extent of other mechanisms (i.e., heterogeneous and multiphase reactions), increase with increasing NR-PM1 mass concentration. Our results suggest that while gas-phase oxidation contributes predominantly to SOA formation during non-pollution periods, other mechanisms such as heterogeneous and multiphase reactions play more important roles in SOA formation during pollution EPs than gas-phase oxidation.

Isoprene, a dominant biogenic volatile organic compound that is mainly emitted by trees, has a significant impact on the atmospheric chemistry. Regional to global changes in biogenic isoprene emission associated with vegetation variations between 2000 and 2015 were estimated using the MEGAN model with satellite land cover data for inputs in this study. The satellite data estimates of land cover changes were compared to results from previous investigators that have either conducted regional studies or have used lower resolution land cover data. The analysis indicates that tree coverage increases of >5% occurred in 13% of locations including in central China and Europe. In contrast, a decrease of >5% was observed in about 5% of locations, especially in tropical regions. The trends in global tree coverage from 2000 to 2015 resulted in a global isoprene emission decrease of only 1.5%, but there were significant regional variations. Obvious decreases in tree coverage in some tropical areas (e.g., Amazon Basin, Western Africa, Southeast Asia) resulted in a ~10% reduction of regional isoprene emission due to agricultural expansion. Distinct increments of isoprene emission (5–10%) were mainly found in Northeast China and India and were associated with afforestation efforts. Deforestation and afforestation associated with managed plantations does not only affect the total forest coverage but also impacts average isoprene emission capacity, which can result in accelerated isoprene emission variations. Consequently, isoprene variation assessments are needed that not only account for changes in vegetation fractions but also consider the changes in plant species compositions of forests and other landscapes.

The North China plain is a region with megacities and huge populations. Aerosols over the highly polluted area have a significant impact on the regional and global climate. In order to investigate the physical and chemical characteristics of aerosol particles in elevated layers there, observations were carried out at the summit of Mt. Tai (1534 m a.s.l.) from 19 to 28 April, 2010, when the air masses were advected from the east (phase-I: 19–21 April), from the south (phase-II: 22–25 April), and from the northwest (phase-III: 26–28 April). Individual aerosol particles were identified with transmission electron microscopy (TEM), new particle formation (NPF) and growth events were monitored by a wide-range particle spectrometer, and ion concentrations in PM_2.5 were analyzed. During phase-I and phase-II, haze layers caused by anthropogenic pollution were observed, and a high percentage of particles were sulfur-rich (47–49%). In phase-III, the haze disappeared due to the intrusion of cold air from the northwest, and mineral dust particles from deserts were dominant (43%). NPF followed by particle growth during daytime was more pronounced on hazy than on clear days. Particle growth during daytime resulted in an increase of particle geometric mean diameter from 10–22 nm in the morning to 56–96 nm in the evening. TEM analysis suggests that sulfuric acid and secondary organic compounds should be important factors for particle nucleation and growth. However, the presence of fine anthropogenic particles (e.g., soot, metal, and fly ash) embedded within S-rich particles indicates that they could weaken NPF and enhance particle growth through condensation and coagulation. Abundant mineral particles in phase-III likely suppressed the NPF processes because they supplied sufficient area on which acidic gases or acids condensed

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