Long-term spatial distribution and implication of black and brown carbon in the Tibetan Plateau.

Black carbon (BC) and brown carbon (BrC) over the high-altitude Tibetan Plateau (TP) can significantly influence regional and global climate change as well as glacial melting. However, obtaining plateau-scale in situ observations is challenging due to its high altitude. By integrating reanalysis data with on-site measurements, the spatial distribution of BC and BrC can be accurately estimated using the random forest algorithm (RF). In our study, the on-site observations of BC and BrC were successively conducted at four sites from 2018 to 2021. Ground-level BC and BrC concentrations were then obtained at a spatial resolution of 0.25° × 0.25° for three periods (including Periods-1980, 2000, and 2020) using RF and multi-source data. The highest annual concentrations of BC (1363.9 ± 338.7 ng/m3) and BrC (372.1 ± 96.2 ng/m3) were observed during Period-2000. BC contributed a dominant proportion of carbonaceous aerosol, with concentrations 3-4 times higher than those of BrC across the three periods. The ratios of BrC to BC decreased from Period-1980 to Period-2020, indicating the increasing importance of BC over the TP. Spatial distributions of plateau-scale BC and BrC concentrations showed heightened levels in the southeastern TP, particularly during Period-2000. These findings significantly enhance our understanding of the spatio-temporal distribution of light-absorbing carbonaceous aerosol over the TP.

[Case Analysis of Heavy Air Pollution Process in Xi'an Using Multi-source Data].

Air pollution continues to be a serious problem in Xi'an. A heavy pollution process and formation mechanism were investigated in Xi'an in January 2019 using multi-source methods (such as material balance and sulfur/nitrogen oxidation rate (SOR/NOR)). The multi-source data included the concentrations of PM2.5, PM10, SO2, NO2, CO, and O3; the chemical components of PM2.5; the meteorological records of ground and vertical observations; the atmospheric reanalysis data. Three phases were obtained including the accumulation phase (P1), maintenance phase (P2), and dispersion phase (P3) during the pollution period. The pollution event was primarily attributed to the superposition of adverse weather conditions and feedback effects. During the periods of P1 and P2, the area of Xi'an was affected by blocking and zonal westerly airflow at 500 hPa (with flat westerly airflow) and uniform-distribution pressure at sea level with a limited pressure gradient and stable weather conditions, and the easterly wind was dominant at 925 hPa; not all of these factors were conducive to the pollutant diffusion. An interaction feedback mechanism between meteorological conditions and heavy pollution could be studied using the ground-based microwave radiometer. The correlations between PM2.5 and inversions of water vapor density, relative humidity, air temperature, and temperature inversion were significant with coefficients of 0.86, 0.62, 0.53, and 0.38, respectively. The feedback mechanism was primarily manifested as follows:with the pollutant accumulation, the radiative cooling effect could lead to or strengthen the occurrence and intensity of temperature inversion, decrease the mixed layer height, and cause moisture accumulation. High humidity could further maintain the pollution by accelerating the secondary formation and promoting the hygroscopic growth of aerosol particles. Therefore, the dominant chemical components to PM2.5were secondary inorganic ions (SO42-+NO3-+NH4+, SNA) and "other" components during the period of P2, with contributions of 43.2% and 23.1%, respectively. In addition, the peak values of PM2.5, SOR, NOR, and the light extinction coefficients all occurred on the same days (January 3 and 6), indicating that the effect of secondary formation was important for both heavy pollution events and visibility. The total contribution of NH4NO3, organic matter (OM), (NH4)2SO4, and EC to the light extinction coefficient was more than 85%. Limited variations in the proportion for components were observed in three phases. During the period of P3, the strong cold air in the mid-lower atmosphere was conducive to the dry and clean air sinking and the pressure gradient at sea level increasing. These were beneficial to the diffusion of air pollutants and water vapor.

Comparison of black carbon, primary and secondary brown carbon light absorption and direct solar absorption at the foothill and summit of Mt. Hua, China.

Atmospheric black carbon (BC), primary and secondary brown carbon (BrCpri and BrCsec) are the light-absorbing carbonaceous aerosol components. The vertical changes in the BC and BrC distributions are not generally known. Here, we presented a study of the spectral light absorption properties, direct solar absorption, and potential source areas of BC and BrC at the foothill (375 m a.s.l.) and summit (2060 m a.s.l.) of Mt. Hua, China. More than tripled BC and BrC light absorption coefficient were observed at the foothill compared to the summit. The dominant carbonaceous light-absorbing was attributed to BC with the percentages of 77 % (foothill) and 79 % (summit), respectively. The light absorption coefficient and direct solar absorption of BrCpri were much higher than those of BrCsec at foothill, especially in winter. The enhancing contributions of BrCsec light absorption coefficient and direct solar absorption were observed with high RH and visibility at the summit. The light absorption properties of BC, BrCpri, and BrCsec may be attributed to the emissions, meteorological conditions, and photochemical oxidation. The inferred potential source spatial distributions of BC and BrCpri showed different patterns at the foothill and summit. The results underlined the primary emission effects (including BC and BrCpri) at the foothill and the importance of BrCsec at the summit, respectively.

Contributions of local pollution emissions to particle bioreactivity in downwind cities in China during Asian dust periods.

This study investigated the effects of pollution emissions on the bioreactivity of PM2.5 during Asian dust periods. PM2.5 during the sampling period were 104.2 and 85.7 µg m-3 in Xi'an and Beijing, respectively, whereas PM2.5 which originated from the Tengger Desert was collected (dust background). Pollution conditions were classified as non-dust days, pollution episode (PE), dust storm (DS)-1, and DS-2 periods. We observed a significant decrease in cell viability and an increase in LDH that occurred in A549 cells after exposure to PM2.5 during a PE and DS-1 in Xi'an and Beijing compared to Tengger Desert PM2.5. Positive matrix factorization was used to identify pollution emission sources. PM2.5 from biomass and industrial sources contributed to alterations in cell viability and LDH in Xi'an, whereas vehicle emissions contributed to LDH in Beijing. OC, EC, Cl-, K+, Mg2+, Ca, Ti, Mn, Fe, Zn, and Pb were correlated with cell viability and LDH for industrial emissions in Xi'an during DS. OC, EC, SO42-, S, Ti, Mn, and Fe were correlated with LDH for vehicle emissions in Beijing during DS. In conclusion, the dust may carry pollutants on its surface to downwind areas, leading to increased risks of particle toxicity.

Light absorption properties of brown carbon over the southeastern Tibetan Plateau.

We present a study of the light-absorbing properties of water-soluble brown carbon (WS-BrC) and methanol-soluble brown carbon (MeS-BrC) at a remote site (Lulang, 3326m above sea level) in the southeastern Tibetan Plateau during the period 2015-2016. The light absorption coefficients at 365nm (babs365) of WS-BrC and MeS-BrC were the highest during winter and the lowest during monsoon season. MeS-BrC absorbs about 1.5 times higher at 365nm compared to WS-BrC. The absorption at 550nm appears lower compared to that of 365nm for WS-BrC and MeS-BrC, respectively. Higher average value of the absorption Ångström exponent (AAE, 365-550nm) was obtained for MeS-BrC (8.2) than that for WS-BrC (6.9). The values of the mass absorption cross section at 365nm (MAC365) indicated that BrC in winter absorbs UV-visible light more efficiently than in monsoon. The results confirm the importance of BrC in contributing to light-absorbing aerosols in this region. The understanding of the light absorption properties of BrC is of great importance, especially in modeling studies for the climate effects and transport of BrC in the Tibetan Plateau.

Spectral dependence of aerosol light absorption at an urban and a remote site over the Tibetan Plateau.

We present a study of aerosol light absorption by using a 7-wavelength Aethalometer model AE33 at an urban site (Lhasa) and a remote site (Lulang) in the Tibetan Plateau. Approximately 5 times greater aerosol absorption values were observed at Lhasa (53±46Mm-1 at 370nm and 20±18Mm-1 at 950nm, respectively) in comparison to Lulang (15±19Mm-1 at 370nm and 4±5Mm-1 at 950nm, respectively). Black carbon (BC) was the dominant light absorbing aerosol component at all wavelengths. The brown carbon (BrC) absorption at 370nm is 32±15% of the total aerosol absorption at Lulang, whereas it is 8±6% at Lhasa. Higher value of absorption Ångström exponent (AAE, 370-950nm) was obtained for Lulang (1.18) than that for Lhasa (1.04) due to the presence of BrC. The AAEs (370-950nm) of BrC were directly extracted at Lulang (3.8) and Lhasa (3.3). The loading compensation parameters (k) increased with wavelengths for both sites, and lower values were obtained at Lulang than those observed at Lhasa for all wavelengths. This study underlines the relatively high percentage of BrC absorption contribution in remote area compared to urban site over the Tibetan Plateau.

The rural carbonaceous aerosols in coarse, fine, and ultrafine particles during haze pollution in northwestern China.

The carbonaceous aerosol concentrations in coarse particle (PM10: Dp ≤ 10 µm, particulate matter with an aerodynamic diameter less than 10 µm), fine particle (PM2.5: Dp ≤ 2.5 µm), and ultrafine particle (PM0.133: Dp ≤ 0.133 µm) carbon fractions in a rural area were investigated during haze events in northwestern China. The results indicated that PM2.5 contributed a large fraction in PM10. OC (organic carbon) accounted for 33, 41, and 62 % of PM10, PM2.5, and PM0.133, and those were 2, 2.4, and 0.4 % for EC (elemental carbon) in a rural area, respectively. OC3 was more abundant than other organic carbon fractions in three PMs, and char dominated EC in PM10 and PM2.5 while soot dominated EC in PM0.133. The present study inferred that K(+), OP, and OC3 are good biomass burning tracers for rural PM10 and PM2.5, but not for PM0.133 during haze pollution. Our results suggest that biomass burning is likely to be an important contributor to rural PMs in northwestern China. It is necessary to establish biomass burning control policies for the mitigation of severe haze pollution in a rural area.

Spatial and seasonal variations of PM2.5 mass and species during 2010 in Xi'an, China.

PM2.5 mass and selected chemical species are measured in 24-h integrated PM2.5 samples collected simultaneously at the urban and rural regions of Xi'an (six sites in total), China in the four seasons of 2010. The analytes include organic carbon and elemental carbon (OC+EC = total carbon, TC), seven water-soluble inorganic ions (NH4(+), K(+), Mg(2+), Ca(2+), Cl(-), SO4(2-), NO3(-)) and six trace elements (Ti, Mn, Fe, Zn, As, Pb). The average PM2.5 mass for the entire measurement period is 142.6 ± 102.7 µg m(-3), which is more than four times that of the Chinese national ambient air quality standard. Spatial variations in PM2.5 mass are not pronounced. The PM2.5 mass and those species measured show a similar seasonal pattern in all six measurement sites, i.e., in the order of winter > autumn > spring > summer. The dominant PM2.5 composition is OC in winter, soil dust in spring, and sulfate, nitrate, and ammonium in summer and autumn. Seasonal variations of TC/PM2.5 and OC/EC ratios follow the PM2.5 changes. Seasonal distributions of (SO4(2-)+NO3(-)+NH4(+))/PM2.5 showed increase in autumn and decrease in winter, while NO3(-)/SO4(2-) ratios increased in autumn and decreased in summer. Eight main PM2.5 sources are identified based on the positive matrix factorization (PMF) analysis and emissions from fossil fuel combustion (traffic and coal burning) are founded to be the main source responsible for the fine particle pollution in Xi'an. In addition, a decreasing trend in OC/PM2.5 is observed in comparison with previous studies in Xi'an.

Comparison and implications of PM2.5 carbon fractions in different environments.

The concentrations of PM2.5 carbon fractions in rural, urban, tunnel and remote environments were measured using the IMPROVE thermal optical reflectance (TOR) method. The highest OC1 and EC1 concentrations were found for tunnel samples, while the highest OC2, OC3, and OC4 concentrations were observed for urban winter samples, respectively. The lowest levels of most carbon fractions were found for remote samples. The percentage contributions of carbon fractions to total carbon (TC) were characterized by one peak (at rural and remote sites) and two peaks (at urban and tunnel sites) with different carbon fractions, respectively. The abundance of char in tunnel and urban environments was observed, which might partly be due to traffic-related tire-wear. Various percentages of optically scattering OC and absorbing EC fractions to TC were found in the four different environments. In addition, the contribution of heating carbon fractions (char and soot) indicated various warming effects per unit mass of TC. The ratios of OC/EC and char/soot at the sites were shown to be source indicators. The investigation of carbon fractions at different sites may provide some information for improving model parameters in estimating their radiative effects.

[Day-night variation of carbonaceous aerosols in PM10 during winter and spring over Xi'an].

The purpose of this study was to investigate the day-night variation of carbonaceous aerosols in PM10 during spring and winter over Xi'an. PM10 samples were collected during 19 Dec 2006 to 21 Jan 2007 (Winter) and 1 Apr 2007 to 30 Apr 2007 (Spring). Organic carbon (OC) and elemental carbon (EC) concentrations were measured using thermal-optical method. PM10, OC, and EC concentrations in winter were 455.0, 62.4, and 7.5 microg/m3 during daytime, and 448.7, 66.1, and 6.9 microg/m3 for nighttime, respectively, while in spring were 397.9, 26.7, and 6.9 microg/m3 for daytime, and 362.1, 31.9, and 8.6 microg/m3 for nighttime. The correlation coefficient of OC and EC during daytime in winter was 0.44, while a strong relationship between OC and EC was observed in spring daytime, indicating that the emission sources of carbonaceous aerosol in winter were more complicated than those in spring. Due to high OC levels and the weaker dispersal ability of atmosphere, the mean concentrations of SOC during winter (8.9 and 10.2 microg/m3 at daytime and nighttime) were much higher than those in spring (2.8 and 3.4 microg/m3). Factor analysis on the eight carbon fraction indicated that coal combustion and biomass burning were the major sources for carbonaceous aerosol in winter, while vehicle exhaust played an important role in spring.