Refractory black carbon aerosols in rainwater in the summer of 2019 in Beijing: Mass concentration, size distribution and wet scavenging ratio.

Black carbon (BC) aerosols in the atmosphere play a significant role in climate systems due to their strong ability to absorb solar radiation. The lifetime of BC depends on atmospheric transport, aging and consequently on wet scavenging processes (in-cloud and below-cloud scavenging). In this study, sequential rainwater samples in eight rainfall events collected in 2 mm interval were measured by a tandem system including a single particle soot photometer (SP2) and a nebulizer. The results showed that the volume-weighted average (VWA) mass concentrations of refractory black carbon (rBC) in each rainfall event varied, ranging from 10.8 to 78.9 µg/L. The highest rBC concentrations in the rainwater samples typically occurred in the first fraction from individual rainfall events. The geometric mean median mass-equivalent diameter (MMD) decreased under precipitation, indicating that rBC with larger sizes was relatively aged and preferentially removed by wet scavenging. A positive correlation (R2 = 0.73) between the VWA mass concentrations of rBC in rainwater and that in ambient air suggested the important contribution of scavenging process. Additionally, the contributions of in-cloud and below-cloud scavenging were distinguished and accounted for 74% and 26% to wet scavenging, respectively. The scavenging ratio of rBC particles was estimated to be 0.06 on average. This study provides helpful information for better understanding the mechanism of rBC wet scavenging and reducing the uncertainty of numerical simulations of the climate effects of rBC.

High organic aerosol in the low layer over a rural site in the North China Plain (NCP): Observations based on large tethered balloon.

High mass concentration of organic aerosol (OA) and its fraction in PM2.5 (particle matter with radius <2.5 µm) were observed in the low layer over a rural site of the North China Plain (NCP) in winter 2018. The mass fraction of OA in PM2.5 was 65.5 % at ground level (5 m above ground), and decreased to 37.1 % in layer of 200-1000 m. In addition, there was a sharp decrease of OA at around the top of planetary boundary layer (PBL), which was distinctly different from the vertical distributions of secondary inorganic aerosols (SIA, e.g., nitrate (NO3-), ammonium (NH4+), and sulfate (SO42-)). The altitude with sharp decrease of OA was very low in the morning and evening, e.g., the sharp decrease of OA occurred at a height <50 m at nighttime on Dec. 19, while was elevated in the noon with the PBL development. Furthermore, OA at ground level exhibited a distinct diurnal variation with a night-to-day ratio of 2.3, which was much larger than those of SIA and inactive CO. All the above results indicated the extremely high OA concentration at the rural site was mainly attributed to direct emission from local sources, such as the combustion of coal and biomass for heating. The extremely high OA could be expected in vest rural areas of the NCP in winter because the farmer activities are very similar to the investigated rural site, underscoring the urgency to mitigate OA emission in rural area for improving the local as well as the regional air quality.

Ground-high altitude joint detection of ozone and nitrogen oxides in urban areas of Beijing.

Based on observational data of ozone (O3) and nitrogen oxide (NO(x)) mixing ratios on the ground and at high altitude in urban areas of Beijing during a period of six days in November 2011, the temporal and spatial characteristics of mixing ratios were analyzed. The major findings include: urban O3 mixing ratios are low and NO(x) mixing ratios are always high near the road in November. Vertical variations of the gases are significantly different in and above the planetary boundary layer. The mixing ratio of O3 is negatively correlated with that of NO(x) and they are positively correlated with air temperature, which is the main factor directly causing vertical variation of O3 and NO(x) mixing ratios at 600-2100 m altitude. The NO(x) mixing ratios elevated during the heating period, while the O3 mixing ratios decreased: these phenomena are more significant at high altitudes compared to lower altitudes. During November, air masses in the urban areas of Beijing are brought by northwesterly winds, which transport O3 and NO(x) at low mixing ratios. Due to Beijing's natural geographical location, northwest air currents are beneficial to the dilution and dispersion of pollutants, which can result in lower O3 and NO(x) background values in the Beijing urban area.

Environmental impacts of three Asian dust events in the northern China and the northwestern Pacific in spring 2021.

In March 2021, China experienced three dust events (Dust-1, 2, 3), especially the first of which was reported as the strongest one in recent ten years. Their environmental impacts have received great attention, demanding comprehensive study to assess such impacts quantitatively. Multiple advanced measurement methods, including satellite, ground-based lidar, online aerosol speciation instrument, and biogeochemical Argo float, were applied to examine and compare the transport paths, optical and chemical properties, and impacts of these three dust events on urban air quality and marine ecosystem. The results showed that Dust-1 exhibited the largest impacts on urban area, increasing PM10 concentration in Beijing, Shuozhou, and Shijiazhuang up to 7525, 3819, and 2992 µg m-3, respectively. However, due to fast movement of the Mongolian low-pressure cyclone, the duration of northwest wind over the land was quite short (e.g., only 10 h in Beijing), which prevented the transport of dust plume to the northwestern Pacific, resulting in limited impact on the ocean. Dust-2 and Dust-3, though weaker in intensity, were transported directly to the sea, and led to a substantial increase in chlorophyll-a concentration (up to near 3 times) in the northwestern Pacific, comparing to climatological value. This indicates that the impacts of dust events on ocean was not necessarily and positively correlated to their impacts on land. Based on the analyses of land-ocean-space integrated observational data and synoptic systems, this study examined how marine ecosystem responded to three significant Asian dust events in spring 2021 and quantitatively assessed the overall impacts of mega dust storms both on land and ocean, which could also provide an interdisciplinary research methodology for future research on strong aerosol emission events such as wildfire and volcanic eruption.

The formation mechanism of air pollution episodes in Beijing city: Insights into the measured feedback between aerosol radiative forcing and the atmospheric boundary layer stability.

Based on the high-resolution observation of meteorological factors profiles, particulate matter concentration and aerosol radiative forcing (ARF) from 25 August to 17 November 2018 in Beijing, the feedback between ARF and the atmospheric boundary layer (ABL) stability was systematically investigated during air pollution episodes. There was the initial explosive growth in particulate matter (PM) concentration that PM2.5 sharply increased from ~8µgm-3 to ~100µgm-3, with aerosol optical depth (AOD) increasing from ~0.25 to ~0.58. This was the transport phase dominated by the southerly winds. As PM increased, the high aerosol loading scattered more solar radiation cooling the earth-atmosphere system (ARF at the top of the atmospheric column (TOA): from ~5Wm-2 to ~-52Wm-2). Meanwhile, high aerosol loading absorbed more solar radiation and heated the atmospheric layer with ARF at the interior of the atmospheric column (ATM) increasing from ~21Wm-2 to ~42Wm-2. The absorption and scattering effects of aerosol together cooled the surface (ARF at the surface of the atmospheric column (SFC): from ~-16Wm-2 to ~-90Wm-2). Thus, the ABL stability rapidly increased in the following cumulative phase and heavy pollution phase with a strong temperature inversion (inversion depth of ~300-1000m) occurring. In turn, the persistent temperature inversion caused the significant accumulation of moisture (water vapor density of ~5-10gm-3) and pollutants, and PM were prone to physicochemical reactions in the high-humidity environment, further increasing PM. It was the constant feedback effect between ARF and the ABL stability that continually reduced atmospheric environmental capacity and aggravated air pollution (PM2.5 and AOD reaching ~95-125µgm-3 and ~1.38-1.75, respectively). Finally, the feedback was broken by dry, clean and strong north winds appearing in Beijing in the dissipation phase.

Estimation of vegetative mercury emissions in China.

Vegetative mercury emissions were estimated within the framework of Biogenic Emission Inventory System (BEIS3 V3.11). In this estimation, the 19 categories of U.S. Geological Survey landcover data were incorporated to generate the vegetation-specific mercury emissions in a 81-km Lambert Conformal model grid covering the total Chinese continent. The surface temperature and cloud-corrected solar radiation from a Mesoscale Meteorological model (MM5) were retrieved and used for calculating the diurnal variation. The implemented emission factors were either evaluated from the measured mercury flux data for forest, agriculture and water, or assumed for other land fields without available flux data. Annual simulations using the MM5 data were performed to investigate the seasonal emission variation. From the sensitivity analysis using two sets of emission factors, the vegetative mercury emissions in China domain were estimated to range from a lower limit of 79 x 10(3) kg/year to an upper limit of 177 x 10(3) kg/year. The modeled vegetative emissions were mainly generated from the eastern and southern China. Using the estimated data, it is shown that mercury emissions from vegetation are comparable to that from anthropogenic sources during summer. However, the vegetative emissions decrease greatly during winter, leaving anthropogenic sources as the major sources of emission.

New positive feedback mechanism between boundary layer meteorology and secondary aerosol formation during severe haze events.

Severe haze events during which particulate matter (PM) increases quickly from tens to hundreds of microgram per cubic meter in 1-2 days frequently occur in China. Although it has been known that PM is influenced by complex interplays among emissions, meteorology, and physical and chemical processes, specific mechanisms remain elusive. Here, a new positive feedback mechanism between planetary boundary layer (PBL), relative humidity (RH), and secondary PM (SPM) formation is proposed based on a comprehensive field experiment and model simulation. The decreased PBL associated with increased PM increases RH by weakening the vertical transport of water vapor; the increased RH in turn enhances the SPM formation through heterogeneous aqueous reactions, which further enhances PM, weakens solar radiation, and decreases PBL height. This positive feedback, together with the PM-Radiation-PBL feedback, constitutes a key mechanism that links PM, radiation, PBL properties (e.g. PBL height and RH), and SPM formation, This mechanism is self-amplifying, leading to faster PM production, accumulation, and more severe haze pollution.

Development of gas chromatography-flame ionization detection system with a single column and liquid nitrogen-free for measuring atmospheric C2-C12 hydrocarbons.

A liquid nitrogen-free GC-FID system equipped with a single column has been developed for measuring atmospheric C2-C12 hydrocarbons. The system is consisted of a cooling unit, a sampling unit and a separation unit. The cooling unit is used to meet the temperature needs of the sampling unit and the separation unit. The sampling unit includes a dehydration tube and an enrichment tube. No breakthrough of the hydrocarbons was detected when the temperature of the enrichment tube was kept at -90 °C and sampling volume was 400 mL. The separation unit is a small round oven attached on the cooling column. A single capillary column (OV-1, 30 m × 0.32 mm I.D.) was used to separate the hydrocarbons. An optimal program temperature (-60 ∼ 170 °C) of the oven was achieved to efficiently separate C2-C12 hydrocarbons. There were good linear correlations (R(2)=0.993-0.999) between the signals of the hydrocarbons and the enrichment amount of hydrocarbons, and the relative standard deviation (RSD) was less than 5%, and the method detection limits (MDLs) for the hydrocarbons were in the range of 0.02-0.10 ppbv for sampling volume of 400 mL. Field measurements were also conducted and more than 50 hydrocarbons from C2 to C12 were detected in Beijing city.

Effects of meteorology and secondary particle formation on visibility during heavy haze events in Beijing, China.

The causes of haze formation in Beijing, China were analyzed based on a comprehensive measurement, including PBL (planetary boundary layer), aerosol composition and concentrations, and several important meteorological parameters such as visibility, RH (relative humidity), and wind speed/direction. The measurement was conducted in an urban location from Nov. 16, 2012 to Jan. 15, 2013. During the period, the visibility varied from >20 km to less than a kilometer, with a minimum visibility of 667 m, causing 16 haze occurrences. During the haze occurrences, the wind speeds were less than 1m/s, and the concentrations of PM2.5 (particle matter with radius less than 2.5 µm) were often exceeded 200 µg/m(3). The correlation between PM2.5 concentration and visibility under different RH values shows that visibility was exponentially decreased with the increase of PM2.5 concentrations when RH was less than 80%. However, when RH was higher than 80%, the relationship was no longer to follow the exponentially decreasing trend, and the visibility maintained in very low values, even with low PM2.5 concentrations. Under this condition, the hygroscopic growth of particles played important roles, and a large amount of water vapor acted as particle matter (PM) for the reduction of visibility. The variations of meteorological parameters (RH, PBL heights, and WS (wind speed)), chemical species in gas-phase (CO, O3, SO2, and NOx), and gas-phase to particle-phase conversions under different visibility ranges were analyzed. The results show that from high visibility (>20 km) to low visibility (<2 km), the averaged PBL decreased from 1.24 km to 0.53 km; wind speeds reduced from 1m/s to 0.5m/s; and CO increased from 0.5 ppmv to 4.0 ppmv, suggesting that weaker transport/diffusion caused the haze occurrences. This study also found that the formation of SPM (secondary particle matter) was accelerated in the haze events. The conversions between SO2 and SO4 as well as NOx to NO3(-) increased, especially under high humidity conditions. When the averaged RH was 70%, the conversions between SO2 and SO4 accounted for about 20% concentration of PM2.5, indicating that formation of secondary particle matter had important contribution for the haze occurrences in Beijing.

[Temporal and spatial distribution of ozone concentration by aircraft sounding over Beijing].

Based on the aircraft sounding volume fraction concentration data of ozone (O3), nitrogen oxides (NO, NO2) and other data in Beijing from 2007 to 2010, temporal and spatial evolution of ozone concentration from the ground surface to 3.5 km altitude were studied. Results show that: (1) Vertical profiles of monthly average O3 concentration were in good agreement, with increasing altitude, the concentrations were first increased and then decreased, and then remained almost constant, and there was a clear dividing line at 1.5 km altitude, the vertical gradient of the O3 concentration changed greatly below which, there were O3 high-value areas, which were influenced by human activities near the ground; the change of vertical gradient of O3 concentration was significantly reduced above 1.5 km altitude, this space was above the mixing layer, where the air mass movement was less affected by underlying surface, and the advection-diffusion played a crucial role in the local accumulation process of air pollutants. (2) Changes of O3 concentration showed clear seasonal characteristics, O3 concentration was lower in spring and autumn, but higher in summer. In the months studied, no significant difference in monthly average O3 concentration from July to September was detected (P > 0.05), but there was significant difference in other months (P < 0.01). (3) In summer days (daytime), the variations in the vertical profiles of hourly O3 concentration were consistent with those of the monthly O3 concentration. The O3 concentration was lower near the surface within 1.5 km in the morning (09:00-10:00), and higher in the afternoon (15:00-16:00), with the maximum discrepancy of about 60 x 10(-9) in the same altitude; there was minor difference in O3 concentration in altitude range of 1.5-3.5 km, generally fluctuating among 70 x 10(-9) -80 x 10(-9). (4) For the regional distribution of O3 concentration, higher concentration within 0-2 km appeared near the Fourth Ring Road of city center and the surrounding areas, the main reasons for this distribution might be the presence of many strong sources of pollution emissions and low sink flow near the ground; within 2-4 km, in addition to the urban area of Beijing, higher O3 concentration areas were found in the north, the south-east (Beijing-Tianjin direction), the south-west (Beijing-Baoding direction). (5) There were significant correlation between O3 and NO, NO2 and NO2/NO within 0-3.5 km, O3 was negatively related with both NO and NO2, but positively correlated with the NO2/NO ratio.