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  • 1
    In: SOIL, Copernicus GmbH, Vol. 7, No. 2 ( 2021-09-08), p. 595-609
    Abstract: Abstract. Conservation tillage has attracted increasing attention over recent decades, mainly due to its benefits for improving soil organic matter content and reducing soil erosion. However, the effects of long-term straw mulching under a no-till system on soil physicochemical properties and bacterial communities at different soil depths are still unclear. In this 12-year experiment of straw removal (CK) and straw mulching (SM) treatments, soil samples were collected at 0–5, 5–10, 10–20, and 20–30 cm soil depths. The results showed that the contents of organic carbon (C), nitrogen (N), and phosphorus (P) fractions, and bacterial abundance significantly decreased, whereas pH significantly increased with soil depth. Compared with CK, SM significantly increased total N, inorganic N, available P, available potassium, and soil water content at 0–5 cm, total organic C content at 0–10 cm, and dissolved organic C and N contents at 0–20 cm. Regarding bacterial communities, SM increased the relative abundances of Proteobacteria, Bacteroidetes, and Acidobacteria but reduced those of Actinobacteria, Chloroflexi, and Cyanobacteria. Bacterial Shannon diversity and Shannon's evenness at 0–5 cm were reduced by SM treatment compared to CK treatment. Furthermore, SM increased the relative abundances of some C-cycling genera (such as Terracidiphilus and Acidibacter) and N-cycling genera (such as Rhodanobacter, Rhizomicrobium, Dokdonella, Reyranella, and Luteimonas) at 0–5 cm. Principal coordinate analysis showed that the largest difference in the composition of soil bacterial communities between CK and SM occurred at 0–5 cm. Soil pH and N and organic C fractions were the major drivers shaping soil bacterial communities. Overall, SM treatment is highly recommended under a no-till system because of its benefits to soil fertility and bacterial abundance.
    Type of Medium: Online Resource
    ISSN: 2199-398X
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2834892-8
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 20 ( 2016-10-27), p. 13213-13230
    Abstract: Abstract. Severe air pollution in Asia is often the consequence of a combination of large anthropogenic emissions and adverse synoptic conditions. However, limited studies on aerosols have been conducted under high emission intensity and under unique geographical and meteorological conditions. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) and other state-of-the-art instruments were utilized at a suburban site, Ziyang, in the Sichuan Basin during December 2012 to January 2013. The chemical compositions of atmospheric submicron aerosols (PM1) were determined, the sources of organic aerosols (OA) were apportioned, and the aerosol secondary formation and aging process were explored as well. Due to high humidity and static air, PM1 maintained a relatively stable level during the whole campaign, with the mean concentration of 59.7 ± 24.1 µg m−3. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. Positive matrix factorization analysis was applied to the high-resolution organic mass spectral matrix, which deconvolved OA mass spectra into four factors: low-volatility (LV-OOA) and semivolatile oxygenated OA (SV-OOA), biomass burning (BBOA) and hydrocarbon-like OA (HOA). OOA (sum of LV-OOA and SV-OOA) dominated OA as high as 71 %. In total, secondary inorganic and organic formation contributed 76 % of PM1. Secondary inorganic species correlated well (Pearson r = 0.415–0.555, p 〈 0.01) with relative humidity (RH), suggesting the humid air can favor the formation of secondary inorganic aerosols. As the photochemical age of OA increased with higher oxidation state, secondary organic aerosol formation contributed more to OA. The slope of OOA against Ox( = O3+NO2) steepened with the increase of RH, implying that, besides the photochemical transformation, the aqueous-phase oxidation was also an important pathway of the OOA formation. Primary emissions, especially biomass burning, resulted in high concentration and proportion of black carbon (BC) in PM1. During the episode obviously influenced by primary emissions, the contributions of BBOA to OA (26 %) and PM1 (11 %) were much higher than those (10–17 %, 4–7 %) in the clean and other polluted episodes, highlighting the significant influence of biomass burning.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 19 ( 2016-10-07), p. 12551-12565
    Abstract: Abstract. The North China Plain (NCP) has been experiencing severe air pollution problems with rapid economic growth and urbanisation. Many field and model studies have examined the distribution of air pollutants in the NCP, but convincing results have not been achieved, mainly due to a lack of direct measurements of pollutants over large areas. Here, we employed a mobile laboratory to observe the main air pollutants in a large part of the NCP from 11 June to 15 July 2013. High median concentrations of sulfur dioxide (SO2) (12 ppb), nitrogen oxides (NOx) (NO + NO2; 452 ppb), carbon monoxide (CO) (956 ppb), black carbon (BC; 5.5 µg m−3) and ultrafine particles (28 350 cm−3) were measured. Most of the high values, i.e. 95 percentile concentrations, were distributed near large cities, suggesting the influence of local emissions. In addition, we analysed the regional transport of SO2 and CO, relatively long-lived pollutants, based on our mobile observations together with wind field and satellite data analyses. Our results suggested that, for border areas of the NCP, wind from outside this area would have a diluting effect on pollutants, while south winds would bring in pollutants that have accumulated during transport through other parts of the NCP. For the central NCP, the concentrations of pollutants were likely to remain at high levels, partly due to the influence of regional transport by prevalent south–north winds over the NCP and partly by local emissions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
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  • 4
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    Copernicus GmbH ; 2017
    In:  Atmospheric Chemistry and Physics Vol. 17, No. 16 ( 2017-08-25), p. 9979-10000
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 16 ( 2017-08-25), p. 9979-10000
    Abstract: Abstract. A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m−3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60–80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations (r = 0.53–0.75, p 〈 0.01) between LO-OOA and odd oxygen (Ox =  O3 + NO2), and between MO-OOA and liquid water content in aerosols. BBOA was resolved in spring and autumn, influenced by agricultural biomass burning (e.g., field preparation burnings, straw burning after the harvest). CCOA was only identified in winter due to domestic heating. These results signified that the comprehensive management for biomass burning and coal combustion emissions is needed. High concentrations of chemical components in PM1 in Beijing, especially in winter or in adverse meteorological conditions, suggest that further strengthening the regional emission control of primary particulate and precursors of secondary species is expected.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 21 ( 2020-11-07), p. 13023-13040
    Abstract: Abstract. Secondary aerosols are a major component of PM2.5, yet their formation mechanisms in the ambient atmosphere are still unclear. Based on field measurements in downtown Beijing, we show that the photolysis of nitrous acid (HONO) may promote the formation of organic and nitrate aerosols in winter in Beijing, which is supported by the fact that the mass concentrations of organic and nitrate aerosols linearly increase as a function of HONO consumed from early morning to noon. The increased nitrate content also leads to the formation of ammonium particulate matter through enhancing the neutralization of nitrate and sulfate by ammonia. We further illustrate that during pollution events in winter in Beijing, over 50 % of the ambient HONO may be related to traffic-related emissions, including direct emissions and formation via the reaction between OH and vehicle-emitted NO. Overall, our results indicate that traffic-related HONO may play an important role in the oxidative capacity and in turn contribute to haze formation in winter in Beijing. The mitigation of HONO and NOx emissions from vehicles may be an effective way to reduce the formation of secondary aerosols and severe haze events in winter in Beijing.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 15 ( 2020-08-03), p. 9183-9207
    Abstract: Abstract. Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 ∘C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 ∘C to 0.7 % at −50 ∘C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at −50 ∘C compared with 25 ∘C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 17 ( 2016-09-06), p. 10985-11000
    Abstract: Abstract. Measurements of atmospheric peroxides were made during Wangdu Campaign 2014 at Wangdu, a rural site in the North China Plain (NCP) in summer 2014. The predominant peroxides were detected to be hydrogen peroxide (H2O2), methyl hydroperoxide (MHP) and peroxyacetic acid (PAA). The observed H2O2 reached up to 11.3 ppbv, which was the highest value compared with previous observations in China at summer time. A box model simulation based on the Master Chemical Mechanism and constrained by the simultaneous observations of physical parameters and chemical species was performed to explore the chemical budget of atmospheric peroxides. Photochemical oxidation of alkenes was found to be the major secondary formation pathway of atmospheric peroxides, while contributions from alkanes and aromatics were of minor importance. The comparison of modeled and measured peroxide concentrations revealed an underestimation during biomass burning events and an overestimation on haze days, which were ascribed to the direct production of peroxides from biomass burning and the heterogeneous uptake of peroxides by aerosols, respectively. The strengths of the primary emissions from biomass burning were on the same order of the known secondary production rates of atmospheric peroxides during the biomass burning events. The heterogeneous process on aerosol particles was suggested to be the predominant sink for atmospheric peroxides. The atmospheric lifetime of peroxides on haze days in summer in the NCP was about 2–3 h, which is in good agreement with the laboratory studies. Further comprehensive investigations are necessary to better understand the impact of biomass burning and heterogeneous uptake on the concentration of peroxides in the atmosphere.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
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  • 8
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 12, No. 8 ( 2019-08-21), p. 4439-4453
    Abstract: Abstract. A system based on incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) has been developed for simultaneous measurement of nitrogen dioxide (NO2), glyoxal (GLY), and methylglyoxal (MGLY). In this system, the measured light absorption at around 460 nm is spectrally resolved. The concentration of absorbers is determined from a multicomponent fit. At an integration time of 100 s, the measurement sensitivity (2σ) for NO2, GLY, and MGLY is 18, 30, and 100 ppt, respectively. The measurement uncertainty, which mainly originates from path length calibration, sampling loss, and uncertainty of absorption cross sections is estimated to be 8 % for NO2, 8 % for GLY, and 16 % for MGLY. When deploying the instrument during field observations, we found significant influence of NO2 on the spectra fitting for retrieving GLY and MGLY concentrations, which is caused by the fact that NO2 has a higher absorption cross section and higher ambient concentration. In order to minimize such an effect, a NO2 photolytic convertor (NPC), which removes sampled NO2 at an efficiency of 76 %, was integrated on the IBBCEAS system. Since sampled GLY and MGLY are mostly (≥95 %) conserved after passing through the NPC, the quality of the spectra fitting and the measurement accuracy of ambient GLY and MGLY under NO2-rich environments could be improved.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2505596-3
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 12 ( 2020-06-25), p. 7359-7372
    Abstract: Abstract. In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (〈10 nm) from sulfuric acid remain poorly measured. Therefore, the effect of stabilizing bases, the contribution of ions and the impact of attractive forces on molecular collisions are under debate. Here, we present precise growth rate measurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performed under atmospheric conditions in the CERN (European Organization for Nuclear Research) CLOUD chamber. Our results show that the evaporation of sulfuric acid particles above 2 nm is negligible, and growth proceeds kinetically even at low ammonia concentrations. The experimental growth rates exceed the hard-sphere kinetic limit for the condensation of sulfuric acid. We demonstrate that this results from van der Waals forces between the vapour molecules and particles and disentangle it from charge–dipole interactions. The magnitude of the enhancement depends on the assumed particle hydration and collision kinetics but is increasingly important at smaller sizes, resulting in a steep rise in the observed growth rates with decreasing size. Including the experimental results in a global model, we find that the enhanced growth rate of sulfuric acid particles increases the predicted particle number concentrations in the upper free troposphere by more than 50 %.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 18 ( 2021-09-27), p. 14275-14291
    Abstract: Abstract. New particle formation (NPF) is a significant source of atmospheric particles, affecting climate and air quality. Understanding the mechanisms involved in urban aerosols is important to develop effective mitigation strategies. However, NPF rates reported in the polluted boundary layer span more than 4 orders of magnitude, and the reasons behind this variability are the subject of intense scientific debate. Multiple atmospheric vapours have been postulated to participate in NPF, including sulfuric acid, ammonia, amines and organics, but their relative roles remain unclear. We investigated NPF in the CLOUD chamber using mixtures of anthropogenic vapours that simulate polluted boundary layer conditions. We demonstrate that NPF in polluted environments is largely driven by the formation of sulfuric acid–base clusters, stabilized by the presence of amines, high ammonia concentrations and lower temperatures. Aromatic oxidation products, despite their extremely low volatility, play a minor role in NPF in the chosen urban environment but can be important for particle growth and hence for the survival of newly formed particles. Our measurements quantitatively account for NPF in highly diverse urban environments and explain its large observed variability. Such quantitative information obtained under controlled laboratory conditions will help the interpretation of future ambient observations of NPF rates in polluted atmospheres.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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