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  • Copernicus GmbH  (11)
  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 7 ( 2020-04-16), p. 4399-4414
    Abstract: Abstract. A regional fully coupled meteorology–chemistry model, Weather Research and Forecasting model with Chemistry (WRF-Chem), was employed to study the seasonality of ozone (O3) pollution and its sources in both China and India. Observations and model results suggest that O3 in the North China Plain (NCP), Yangtze River Delta (YRD), Pearl River Delta (PRD), and India exhibit distinctive seasonal features, which are linked to the influence of summer monsoons. Through a factor separation approach, we examined the sensitivity of O3 to individual anthropogenic, biogenic, and biomass burning emissions. We found that summer O3 formation in China is more sensitive to industrial and biogenic sources than to other source sectors, while the transportation and biogenic sources are more important in all seasons for India. Tagged simulations suggest that local sources play an important role in the formation of the summer O3 peak in the NCP, but sources from Northwest China should not be neglected to control summer O3 in the NCP. For the YRD region, prevailing winds and cleaner air from the ocean in summer lead to reduced transport from polluted regions, and the major source region in addition to local sources is Southeast China. For the PRD region, the upwind region is replaced by contributions from polluted PRD as autumn approaches, leading to an autumn peak. The major upwind regions in autumn for the PRD are YRD (11 %) and Southeast China (10 %). For India, sources in North India are more important than sources in the south. These analyses emphasize the relative importance of source sectors and regions as they change with seasons, providing important implications for O3 control strategies.
    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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  • 2
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    Copernicus GmbH ; 2022
    In:  Atmospheric Chemistry and Physics Vol. 22, No. 6 ( 2022-03-24), p. 3861-3873
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 6 ( 2022-03-24), p. 3861-3873
    Abstract: Abstract. The peripheral circulation of typhoon forms sustained ozone episodes. However, how it impacts the day-to-day ozone pollution levels during the episodes has not been clearly studied, which is crucial for better prediction of the daily ozone variation. In this study, the analysis of ground observation, wind profile data, and model simulation is integrated. By analysing the wind profile radar observations, we found a weak wind deepening (WWD; vertical depth of the weak winds increased), more correlated with the ground-level ozone variation than surface weak wind. Long-term statistical analyses showed that the WWD is a common weather phenomenon in the peripheral subsidence region of typhoons and is generally accompanied by ozone pollution episodes. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) with process analysis simulation showed that the peripheral subsidence chemical formation (CHEM) and vertical mixing (VMIX) effects are two major contributors to the enhancement of ozone levels to form the episode, while the advection (ADV) showed negative values. However, the day-to-day variation of the daytime ozone levels during the episode is not determined by the daily variation of daytime CHEM and VMIX but is dominated by the ADV terms. Therefore, the ozone and its precursors accumulation, including the enhancement during the night-time, contribute to the daytime ozone increase in the following day. A detail day-to-day process analysis showed that in additional to decrease of negative ADV values (e.g. the weakened advection outflow or dispersion) on the ground, the integrated effect of the daily variation of the accumulative CHEM and ADV above the ground throughout the planetary boundary layer (PBL) together determined the overall day-to-day daytime ozone variation on the ground through the VMIX process. The results indicate that the peripheral characteristics of approaching typhoon not only form the ozone episode by the enhanced photochemical reactions, but also could increase the day-to-day daytime ozone levels via pollution accumulation throughout the PBL due to the WWD up to 3–5 km. These results illustrate the important role of the WWD in the lower troposphere for the formation of sustained ozone episodes due to the peripheral circulation of the typhoon, which helps to better predict the daily changes of daytime ozone levels.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
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  • 3
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    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 10 ( 2018-05-23), p. 7081-7094
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 10 ( 2018-05-23), p. 7081-7094
    Abstract: Abstract. As an important solar radiation absorbing aerosol, the effect of black carbon (BC) on surface ozone, via reducing photolysis rate, has been widely discussed by “offline” model studies. However, BC–boundary layer (BL) interactions also influence surface ozone. Using the “online” model simulations and process analysis, we demonstrate the significant impact of BC–BL interaction on surface ozone in Nanjing. The absorbing effect of BC heats the air above the BL and suppresses and delays the development of the BL, which eventually leads to a change in surface ozone via a change in the contributions from chemical and physical processes (photochemistry, vertical mixing and advection). For chemical processes, the suppression of the BL leads to large amounts of ozone precursors being confined below the BL which has an increased effect on ozone chemical production and offsets the decrease caused by the reduction of the photolysis rate, thus enhancing ozone chemical formation from 10:00 to 12:00 LT. Furthermore, changes in physical processes, especially the vertical mixing process, show a more significant influence on surface ozone. The weakened turbulence, caused by the suppressed BL, entrains much less ozone aloft down to the surface. Finally, summing-up the changes in the processes, surface ozone reduces before noon and the maximum reduction reaches 16.4 ppb at 12:00 LT. In the afternoon, the changes in chemical process are small which inconspicuously influence surface ozone. However, change in the vertical mixing process still influences surface ozone significantly. Due to the delayed development of the BL, there are obvious ozone gradients around the top of BL. Therefore, high concentrations of ozone aloft can still be entrained down to the surface which offsets the reduction of surface ozone. Comparing the changes in the processes, the change in vertical mixing plays the most important role in impacting surface ozone. Our results highlight the great impacts BC–BL interactions have on surface ozone by influencing the ozone contribution from physical process. This suggests that more attention should be paid to the mechanism of aerosol–BL interactions when controlling ozone pollution.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 4
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 14, No. 2 ( 2021-02-03), p. 703-718
    Abstract: Abstract. The development of chemical transport models with advanced physics and chemical schemes could improve air-quality forecasts. In this study, the China Meteorological Administration Unified Atmospheric Chemistry Environment (CUACE) model, a comprehensive chemistry module incorporating gaseous chemistry and a size-segregated multicomponent aerosol algorithm, was coupled to the Weather Research and Forecasting (WRF) framework with chemistry (WRF-Chem) using an interface procedure to build the WRF/CUACE v1.0 model. The latest version of CUACE includes an updated aerosol dry deposition scheme and the introduction of heterogeneous chemical reactions on aerosol surfaces. We evaluated the WRF/CUACE v1.0 model by simulating PM2.5, O3, NO2, and SO2 concentrations for January, April, July, and October (representing winter, spring, summer and autumn, respectively) in 2013, 2015, and 2017 and comparing them with ground-based observations. Secondary inorganic aerosol simulations for the North China Plain (NCP), Yangtze River Delta (YRD), and Sichuan Basin (SCB) were also evaluated. The model captured well the variations of PM2.5, O3, and NO2 concentrations in all seasons in eastern China. However, it is difficult to accurately reproduce the variations of air pollutants over SCB, due to its deep basin terrain. The simulations of SO2 were generally reasonable in the NCP and YRD with the bias at −15.5 % and 24.55 %, respectively, while they were poor in the Pearl River Delta (PRD) and SCB. The sulfate and nitrate simulations were substantially improved by introducing heterogeneous chemical reactions into the CUACE model (e.g., change in bias from −95.0 % to 4.1 % for sulfate and from 124.1 % to 96.0 % for nitrate in the NCP). Additionally, The WRF/CUACE v1.0 model was revealed with better performance in simulating chemical species relative to the coupled Fifth-Generation Penn State/NCAR Mesoscale Model (MM5) and CUACE model. The development of the WRF/CUACE v1.0 model represents an important step towards improving air-quality modeling and forecasts in China.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2456725-5
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  • 5
    Online Resource
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    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 2 ( 2019-01-22), p. 847-860
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 2 ( 2019-01-22), p. 847-860
    Abstract: Abstract. The continent-to-ocean supply of phosphorus (P) in the soluble state, recognized as bioavailable P, via the atmosphere is hypothesized to be crucial to the biological cycle in offshore surface seawater. To investigate the solubility of P in aerosol particles moving towards the northwestern Pacific from the Asian continent, we measured the total P (TP), total dissolved P (TDP) and dissolved inorganic P (DIP) in aerosols at Qingdao (36∘06′ N, 120∘33′ E), a coastal city in eastern China. The samples were collected in December 2012 and January 2013 (winter) and in March and April 2013 (spring), when the middle-latitude westerly wind was prevailing. On average, P solubility, i.e., the ratio of TDP to TP, was 32.9±16.7 % in winter and 21.3±9.8 % in spring, and the TP concentrations in the two seasons were similar. This seasonal solubility difference is attributed to the aerosol sources containing the P. Particles in winter were predominantly anthropogenic particles from local and regional areas, and particles in spring were significantly influenced by natural dust from the arid and semiarid areas in the inland part of the continent. Moreover, acidification processes associated with the formation of sulfate and nitrate in the winter samples enhanced P solubility, suggesting that the P in anthropogenic particles was more susceptible to the production of acidic species than that in natural dust particles. There was a strong positive correlation between P solubility and relative humidity (RH). P solubility was usually less than 30 % when RH was below 60 %, even when the content of acidic species and/or anthropogenic particles in the aerosols was high, suggesting humidity had a critical role in the production of TDP. In addition, the proportion of DIP in TDP was high when the particles were predominantly anthropogenic, and the proportion of dissolved organic P (DOP; quantified as TDP minus DIP) in TDP was high when the particles were dominated by natural dust. These results indicate that, as the contents of bioavailable P in Asian continent outflows are closely dependent on the aerosol particle origins, atmospheric acidic processes could convert P into a bioavailable state under certain meteorological conditions. Therefore, the recent severe air pollution over East Asia might have enhanced the input of bioavailable P to downwind marine areas.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
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  • 6
    Online Resource
    Online Resource
    Copernicus GmbH ; 2023
    In:  Atmospheric Chemistry and Physics Vol. 23, No. 9 ( 2023-05-05), p. 5177-5190
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 9 ( 2023-05-05), p. 5177-5190
    Abstract: Abstract. Tropospheric ozone, an important secondary pollutant, is greatly impacted by aerosols within boundary layer (BL). Previous studies have mainly attributed ozone variation to either aerosol–BL or aerosol–photolysis interactions at the near-surface level. In this study, we analyze the sensitivities of ozone response to aerosol mixing states (e.g., mixing behavior hypothesis of scattering and absorbing components) in the vertical direction and address the effects of aerosol–BL and aerosol–photolysis interactions on ozone profiles in autumn by Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) simulations. The aerosol internal mixing state experiment reasonably reproduces the vertical distribution and time variation in meteorological elements and ozone. Sensitivity experiments show that aerosols lead to turbulent suppression, precursor accumulation, lower-level photolysis reduction, and upper-level photolysis enhancement. Consequently, ozone basically decreases within entire the BL during daytime (08:00–17:00 LT), and the decrease is the least in the external mixing state (2.0 %) when compared with internal (10.5 %) and core shell mixing states (8.6 %). The photolysis enhancement is the most significant in the external mixing state due to its strong scattering ability. By process analysis, lower-level ozone chemical loss is enhanced due to photolysis reduction and NOx accumulation under a volatile organic compound (VOC)-limited regime. Upper-level ozone chemical production is accelerated due to a higher photolysis rate resulting from aerosol backscattering. Therefore, the increased ozone entrainment from BL aloft to the surface induced by the boosted ozone vertical gradient outweighs the decreased ozone entrainment induced by turbulent suppression after 11:00 LT. Additional simulations support the finding that the aerosol effect on precursors, photolysis, and ozone is consistent under different underlying surface and pollution conditions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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  • 7
    Online Resource
    Online Resource
    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 20 ( 2021-10-18), p. 15555-15567
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 20 ( 2021-10-18), p. 15555-15567
    Abstract: Abstract. Observations suggest that the vertical distributions of air pollutants, such as black carbon (BC), present as various types depending on the emission sources and meteorological diffusion conditions. However, the formation process and source appointment of some special BC profiles are not fully understood. In this paper, by using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) with a BC-tagging technique, we investigate the formation mechanism and regional sources of a BC peak in the free troposphere observed by an aircraft flight in Beijing (BJ) on 5 May 2018. The results show that the contribution rate of the Beijing–Tianjin–Hebei (BTH) region to the surface BC of BJ exceeded 80 % in this case. Local sources dominated BC in BJ from the surface to approximately 700 m (78.5 %), while the BC peak in the free troposphere (∼4000 m) was almost entirely imported from external sources (99.8 %). Combining BC tracking and process analysis, we find that horizontal advection (HADV) and vertical advection (VADV) processes played an important role in the convergent and upward movement and the transport of BC. The BC originating from the surface in central provinces, including Shanxi (SX), Henan (HN), and Hebei (HB), had been uplifted through a cyclone system 16 h previously, was transported to a height of approximately 3000 m above BJ, and was then lifted by the VADV process to approximately 4000 m. At the surface, BJ and its surroundings were under the control of a weak pressure gradient, leading to the accumulation of BC within the boundary layer. Our results indicate that cyclone systems can quickly lift air pollutants, such as BC, up to the free troposphere, as well as extend their lifetimes and further affect the regional atmospheric environment and climate.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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  • 8
    In: Biogeosciences, Copernicus GmbH, Vol. 15, No. 3 ( 2018-02-07), p. 749-765
    Abstract: Abstract. In this study, five on-board microcosm experiments were performed in the subtropical gyre, the Kuroshio Extension region of the northwest Pacific Ocean (NWPO), and the Yellow Sea (YS) in order to investigate phytoplankton growth following the addition of artificially modified mineral dust (AM dust) and various nutrients (nitrogen (N), phosphorus (P), iron (Fe), N + P, and N + P + Fe). The two experiments carried out with AM-dust addition in the subtropical gyre showed a maximum chlorophyll a (Chl a) concentration increase of 1.7- and 2.8-fold, while the cell abundance of large-sized phytoplankton ( 〉  5 µm) showed a 1.8- and 3.9-fold increase, respectively, relative to the controls. However, in the Kuroshio Extension region and the YS, the increases in maximum Chl a and cell abundance of large-sized phytoplankton following AM-dust addition were at most 1.3-fold and 1.7-fold larger than those in the controls, respectively. A net conversion efficiency index (NCEI) newly proposed in this study, size-fractionated Chl a, and the abundance of large-sized phytoplankton were analysed to determine which nutrients contribute to supporting phytoplankton growth. Our results demonstrate that a combination of nutrients, N–P or N + P + Fe, is responsible for phytoplankton growth in the subtropical gyre following AM-dust addition. Single nutrient addition, i.e., N in the Kuroshio Extension region and P or N in the YS, controls the phytoplankton growth following AM-dust addition. In the AM-dust-addition experiments, in which the increased N–P or P was identified to determine phytoplankton growth, the dissolved inorganic P from AM dust (8.6 nmol L−1) was much lower than the theoretically estimated minimum P demand (∼ 20 nmol L−1) for phytoplankton growth. These observations suggest that additional supply augments the bioavailable P stock in incubated seawater with AM-dust addition, most likely due to an enhanced solubility of P from AM dust or the remineralization of the dissolved organic P.
    Type of Medium: Online Resource
    ISSN: 1726-4189
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2158181-2
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  • 9
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 6 ( 2019-03-21), p. 3673-3685
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 6 ( 2019-03-21), p. 3673-3685
    Abstract: Abstract. Cold frontal passages usually promote quick removal of atmospheric pollutants over North China (e.g. the Beijing–Tianjin–Hebei region). However, in the Yangtze River Delta (YRD), cold fronts may bring air pollutants from the polluted North China Plain (NCP), thereby deteriorating the air quality in the YRD. In this study, a cold frontal passage and a subsequent stable weather event over YRD during 21–26 January 2015 was investigated with in situ observations and Weather Research and Forecasting – Community Multiscale Air Quality Modeling System simulations. Observations showed a burst of PM2.5 pollution and an obvious southward motion of PM2.5 peaks on the afternoon of 21 January, suggesting a strong inflow of highly polluted air masses to YRD by a cold frontal passage. Model simulations revealed an existing warm and polluted air mass over YRD ahead of the frontal zone, which climbed to the free troposphere along the frontal surface as the cold front passed, increasing the PM2.5 concentration at high altitudes. Strong north-westerly frontal airflow transported particles from the highly polluted NCP to the YRD. As the frontal zone moved downstream of YRD, high pressure took control over the YRD, which resulted in a synoptic subsidence that trapped PM2.5 in the boundary layer. After the cold frontal episode, a uniform pressure field took control over the YRD. Locally emitted PM2.5 started to accumulate under the weak winds and stable atmosphere. Tagging of PM2.5 by geophysical regions showed that the PM2.5 contribution from the YRD itself was 35 % and the contribution from the NCP was 29 % during the cold frontal passage. However, under the subsequent stable weather conditions, the PM2.5 contribution from the YRD increased to 61.5 % and the contribution from the NCP decreased to 14.5 %. The results of this study indicate that cold fronts are potential carriers of atmospheric pollutants when there are strong air pollutant sources in upstream areas, which may deteriorate air quality in downstream regions.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 10
    Online Resource
    Online Resource
    Copernicus GmbH ; 2020
    In:  Atmospheric Chemistry and Physics Vol. 20, No. 18 ( 2020-09-15), p. 10831-10844
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 18 ( 2020-09-15), p. 10831-10844
    Abstract: Abstract. Previous studies have emphasized that the decrease in photolysis rate at the surface induced by the light extinction of aerosols could weaken ozone photochemistry and then reduce surface ozone. However, quantitative studies have shown that weakened photochemistry leads to a much greater reduction in the net chemical production of ozone, which does not match the reduction in surface ozone. This suggests that in addition to photochemistry, some other physical processes related to the variation of ozone should also be considered. In this study, the Weather Research and Forecasting with Chemistry (WRF-Chem) model coupled with the ozone source apportionment method was applied to determine the mechanism of ozone reduction induced by aerosols over central East China (CEC). Our results showed that weakened ozone photochemistry led to a significant reduction in ozone net chemical production, which occurred not only at the surface but also within the lowest several hundred meters in the planetary boundary layer (PBL). Meanwhile, a larger ozone gradient was formed in the vertical direction, which led to the high concentrations of ozone aloft being entrained by turbulence from the top of the PBL to the surface and partly counteracting the reduction in surface ozone. In addition, contribution from dry deposition was weakened due to the decrease in surface ozone concentration. The reduction in the ozone's sink also slowed down the rate of the decrease in surface ozone. Ozone in the upper layer of the PBL was also reduced, which was induced by much ozone aloft being entrained downward. Therefore, by affecting the photolysis rate, the impact of aerosols was a reduction in ozone not only at the surface but also throughout the entire PBL during the daytime over CEC in this study. The ozone source apportionment results showed that 41.4 %–66.3 % of the reduction in surface ozone came from local and adjacent source regions, which suggested that the impact of aerosols on ozone from local and adjacent regions was more significant than that from long-distance regions. The results also suggested that while controlling the concentration of aerosols, simultaneously controlling ozone precursors from local and adjacent source regions is an effective way to suppress the increase in surface ozone over CEC at present.
    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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