Total Black Carbon Deposition Research Articles

Sources, size-resolved deposition in the human respiratory tract and health risks of submicron black carbon in urban atmosphere in Pearl River Delta, China

Black carbon (BC) has a significantly negative impact on air quality, climate and human health. Here we investigated the sources and health effects of BC in urban area of the Pearl River Delta (PRD) based on online data measured by Aerodyne soot particle high-resolution time of flight aerosol mass spectrometer (SP-AMS). In urban PRD, BC particles mainly came from vehicle emissions especially heavy-duty vehicle exhausts (contributing 42.9 % of total BC mass concentration), long-range transport (27.6 %), and aged biomass combustion emissions (22.3 %). Indicated by source analysis using simultaneous aethalometer data, BC associated with local secondary oxidation and transport may also be originated from fossil fuel combustion, especially traffic sources in urban and surrounding areas. Size-resolved BC mass concentrations provided by SP-AMS, for the first time to our best knowledge, were used to calculate BC deposition in the human respiratory tract (HRT) of different populations (children, adults, and the elderly) by the Multiple-Path Particle Dosimetry (MPPD) model. We found that submicron BC was deposited more in the pulmonary (P) region (49.0–53.2 % of the total BC deposition dose), while less in the tracheobronchial (TB, 35.6–37.2 %) and head (HA, 11.2–13.8 %) regions. Adults suffered the highest BC deposition (1.19 μg day−1) than the elderly (1.09 μg day−1) and children (0.25 μg day−1). BC deposition rate was greater at night (especially 18:00–24:00) than during the daytime. The maximum deposition in the HRT was found for BC particles around 100 nm, mainly in deeper respiratory regions (TB and P), which may cause more serious health effects. Adults and the elderly group are confronted with the notable carcinogenic risk of BC in the urban PRD, up to 29 times higher than the threshold. Our study emphasizes the need to control BC pollution in the urban area, especially nighttime vehicle emissions.

Deposition of Organic and Black Carbon: Direct Measurements at Three Remote Stations in the Himalayas and Tibetan Plateau

AbstractCarbonaceous matter in the atmosphere has an important influence on climate change. Currently, the deposition of carbonaceous matter is one of the largest uncertainties in the climate system. This phenomenon is common in remote regions, such as the Himalayas and Tibetan Plateau. In this study, for the first time, we reported in situ measurements of wet and dry deposition rates of carbonaceous matter at three remote stations: Nam Co, Lulang, and Everest. The results showed that the annual wet deposition rates of water‐insoluble organic carbon (WIOC) and black carbon (BC) were 60.2 and 5.8 mg·m−2·year−1, 330 and 34.6 mg·m−2·year−1, and 47.0 and 2.6 mg·m−2·year−1 at the Nam Co, Lulang, and Everest stations, respectively. Seasonal variations in the wet deposition rates of WIOC and BC were controlled by precipitation amount and their atmospheric concentrations. In addition, the wet scavenging ratios of WIOC and BC at Nam Co Station were close to those observed in other remote areas. The total BC deposition at Nam Co Station (15.3 mg·m−2·year−1) was higher than that from chemical transport models, implying a dominant role of dry deposition of BC in the total deposition at this station and an urgent need to improve the aerosol deposition in models for the Himalayas and Tibetan Plateau. It was found that the deposition rates of carbonaceous matter in the Himalayas and Tibetan Plateau had large spatial variation; thus, high‐resolution models need to be applied in the future.

Sources of Black Carbon Deposition to the Himalayan Glaciers in Current and Future Climates.

WRF-Chem and a modified version of the ECLIPSE 5a emission inventory were used to investigate the sources impacting black carbon (BC) deposition to the Himalaya, Karakoram, and Hindu Kush (HKHK) region. This work extends previous studies by simulating deposition to the HKHK region not only under current conditions, but also in the 2040–2050 period under two realistic emission scenarios and in three different phases of the El Niño-Southern Oscillation (ENSO). Under current conditions, sources from outside our South Asian modelling domain have a similar impact on total BC deposition to the HKHK region (35–87%, varying with month) as South Asian anthropogenic sources (13–62%). Industry (primarily brick kilns) and residential solid fuel burning combined account for 45–66% of the in-domain anthropogenic BC deposition to the HKHK region. Under a no further control emission scenario for 2040–2050, the relative contributions to BC deposition in the HKHK region are more skewed toward in-domain anthropogenic sources (45–65%) relative to sources outside the domain (26–52%). The in-domain anthropogenic BC deposition has significant contributions from industry (32–42%), solid fuel burning (17–28%), and diesel fuel burning (17–27%). Under a scenario in which emissions in South Asia are mitigated, the relative cotribution from South Asian anthropogenic sources is significantly reduced to 11–34%. The changes due to phase of ENSO do not seem to follow consistent patterns with ENSO. Future work will use the high-resolution deposition maps developed here to determine the impact of different sources of BC on glacier melt and water availability in the region.

Seasonal Progression of the Deposition of Black Carbon by Snowfall at Ny‐Ålesund, Spitsbergen

AbstractDeposition of black carbon (BC) aerosol in the Arctic lowers snow albedo, thus contributing to warming in the region. However, the processes and impacts associated with BC deposition are poorly understood because of the scarcity and uncertainties of measurements of BC in snow with adequate spatiotemporal resolution. We sampled snowpack at two sites (11 m and 300 m above sea level) at Ny‐Ålesund, Spitsbergen, in April 2013. We also collected falling snow near the surface with a windsock from September 2012 to April 2013. The size distribution of BC in snowpack and falling snow was measured using a single‐particle soot photometer combined with a characterized nebulizer. The BC size distributions did not show significant variations with depth in the snowpack, suggesting stable size distributions in falling snow. The BC number and mass concentrations (CNBC and CMBC) at the two sites agreed to within 19% and 10%, respectively, despite the sites' different snow water equivalent (SWE) loadings. This indicates the small influence of the amount of SWE (or precipitation) on these quantities. Average CNBC and CMBC in snowpack and falling snow at nearly the same locations agreed to within 5% and 16%, after small corrections for artifacts associated with the sampling of the falling snow. This comparison shows that the dry deposition was a small contributor to the total BC deposition. CMBC were highest (2.4 ± 3.0 μg L−1) in December–February and lowest (1.2 ± 1.2 μg L−1) in September–November.

Tagged tracer simulations of black carbon in the Arctic: transport, source contributions, and budget

Abstract. We implemented a tagged tracer method of black carbon (BC) into a global chemistry transport model, GEOS-Chem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and examined the sensitivity of an aging parameterization and wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62 % to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Sea of Okhotsk and eastern Siberia during winter and spring. We identified an important window area, which allowed a strong incoming of East Asian BC to the Arctic (130–180° E and 3–8 km of altitude at 66° N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km of altitude due to uplifting during long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was lower than that from other large source regions such as Europe, Russia, and North America. However, the East Asian contribution was the most important for BC in the middle troposphere (41 %) and the BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska, and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12–15 %, which became the maximum during summer.

Light‐absorbing impurities enhance glacier albedo reduction in the southeastern Tibetan plateau

AbstractLight‐absorbing impurities (LAIs) in snow of the southeastern Tibetan Plateau (TP) and their climatic impacts are of interest not only because this region borders areas affected by the South Asian atmospheric brown clouds but also because the seasonal snow and glacier melt from this region form important headwaters of large rivers. In this study, we collected surface snow and snowpit samples from four glaciers in the southeastern TP in June 2015 to investigate the comprehensive observational data set of LAIs. Results showed that the LAI concentrations were much higher in the aged snow and granular ice than in the fresh snow and snowpits due to postdepositional processes. Impurity concentrations fluctuated across snowpits, with maximum LAI concentrations frequently occurring toward the bottom of snowpits. Based on the SNow ICe Aerosol Radiative model, the albedo simulation indicated that black carbon and dust account for approximately 20% of the albedo reduction relative to clean snow. The radiative forcing caused by black carbon and dust deposition on the glaciers were between 1.0–141 W m−2 and 1.5–120 W m−2, respectively. Black carbon (BC) played a larger role in albedo reduction and radiative forcing than dust in the study area, enhancing approximately 15% of glacier melt. Analysis based on the Fire INventory from NCAR indicated that nonbiomass‐burning sources of BC played an important role in the total BC deposition, especially during the monsoon season. This study suggests that eliminating anthropogenic BC could mitigate glacier melt in the future of the southeastern TP.

Effects of the Wegener–Bergeron–Findeisen process on global black carbon distribution

Abstract. We systematically investigate the effects of Wegener–Bergeron–Findeisen process (hereafter WBF) on black carbon (BC) scavenging efficiency, surface BCair, deposition flux, concentration in snow (BCsnow, ng g−1), and washout ratio using a global 3-D chemical transport model (GEOS-Chem). We differentiate riming- versus WBF-dominated in-cloud scavenging based on liquid water content (LWC) and temperature. Specifically, we implement an implied WBF parameterization using either temperature or ice mass fraction (IMF) in mixed-phase clouds based on field measurements. We find that at Jungfraujoch, Switzerland, and Abisko, Sweden, where WBF dominates in-cloud scavenging, including the WBF effect strongly reduces the discrepancies of simulated BC scavenging efficiency and washout ratio against observations (from a factor of 3 to 10 % and from a factor of 4–5 to a factor of 2). However, at Zeppelin, Norway, where riming dominates, simulation of BC scavenging efficiency, BCair, and washout ratio become worse (relative to observations) when WBF is included. There is thus an urgent need for extensive observations to distinguish and characterize riming- versus WBF-dominated aerosol scavenging in mixed-phase clouds and the associated BC scavenging efficiency. Our model results show that including the WBF effect lowers global BC scavenging efficiency, with a higher reduction at higher latitudes (8 % in the tropics and up to 76 % in the Arctic). The resulting annual mean BCair increases by up to 156 % at high altitudes and at northern high latitudes because of lower temperature and higher IMF. Overall, WBF halves the model–observation discrepancy (from −65 to −30 %) of BCair across North America, Europe, China and the Arctic. Globally WBF increases BC burden from 0.22 to 0.29–0.35 mg m−2 yr−1, which partially explains the gap between observed and previous model-simulated BC burdens over land. In addition, WBF significantly increases BC lifetime from 5.7 to ∼ 8 days. Additionally, WBF results in a significant redistribution of BC deposition in source and remote regions. Specifically, it lowers BC wet deposition (by 37–63 % at northern mid-latitudes and by 21–29 % in the Arctic), while it increases dry deposition (by 3–16 % at mid-latitudes and by 81–159 % in the Arctic). The resulting total BC deposition is lower at mid-latitudes (by 12–34 %) but higher in the Arctic (by 2–29 %). We find that WBF decreases BCsnow at mid-latitudes (by ∼ 15 %) but increases it in the Arctic (by 26 %) while improving model comparisons with observations. In addition, WBF dramatically reduces the model–observation discrepancy of washout ratios in winter (from a factor of 16 to 4). The remaining discrepancies in BCair, BCsnow and BC washout ratios suggest that in-cloud removal in mixed-phased clouds is likely still excessive over land.

Factors controlling black carbon distribution in the Arctic

Abstract. We investigate the sensitivity of black carbon (BC) in the Arctic, including BC concentration in snow (BCsnow, ng g−1) and surface air (BCair, ng m−3), as well as emissions, dry deposition, and wet scavenging using the global three-dimensional (3-D) chemical transport model (CTM) GEOS-Chem. We find that the model underestimates BCsnow in the Arctic by 40 % on average (median = 11.8 ng g−1). Natural gas flaring substantially increases total BC emissions in the Arctic (by ∼ 70 %). The flaring emissions lead to up to 49 % increases (0.1–8.5 ng g−1) in Arctic BCsnow, dramatically improving model comparison with observations (50 % reduction in discrepancy) near flaring source regions (the western side of the extreme north of Russia). Ample observations suggest that BC dry deposition velocities over snow and ice in current CTMs (0.03 cm s−1 in the GEOS-Chem) are too small. We apply the resistance-in-series method to compute a dry deposition velocity (vd) that varies with local meteorological and surface conditions. The resulting velocity is significantly larger and varies by a factor of 8 in the Arctic (0.03–0.24 cm s−1), which increases the fraction of dry to total BC deposition (16 to 25 %) yet leaves the total BC deposition and BCsnow in the Arctic unchanged. This is largely explained by the offsetting higher dry and lower wet deposition fluxes. Additionally, we account for the effect of the Wegener–Bergeron–Findeisen (WBF) process in mixed-phase clouds, which releases BC particles from condensed phases (water drops and ice crystals) back to the interstitial air and thereby substantially reduces the scavenging efficiency of clouds for BC (by 43–76 % in the Arctic). The resulting BCsnow is up to 80 % higher, BC loading is considerably larger (from 0.25 to 0.43 mg m−2), and BC lifetime is markedly prolonged (from 9 to 16 days) in the Arctic. Overall, flaring emissions increase BCair in the Arctic (by ∼ 20 ng m−3), the updated vd more than halves BCair (by ∼ 20 ng m−3), and the WBF effect increases BCair by 25–70 % during winter and early spring. The resulting model simulation of BCsnow is substantially improved (within 10 % of the observations) and the discrepancies of BCair are much smaller during the snow season at Barrow, Alert, and Summit (from −67–−47 % to −46–3 %). Our results point toward an urgent need for better characterization of flaring emissions of BC (e.g., the emission factors, temporal, and spatial distribution), extensive measurements of both the dry deposition of BC over snow and ice, and the scavenging efficiency of BC in mixed-phase clouds. In addition, we find that the poorly constrained precipitation in the Arctic may introduce large uncertainties in estimating BCsnow. Doubling precipitation introduces a positive bias approximately as large as the overall effects of flaring emissions and the WBF effect; halving precipitation produces a similarly large negative bias.

Impact of future Arctic shipping on high‐latitude black carbon deposition

The retreat of Arctic sea ice has led to renewed calls to exploit Arctic shipping routes. The diversion of ship traffic through the Arctic will shorten shipping routes and possibly reduce global shipping emissions. However, deposition of black carbon (BC) aerosol emitted by additional Arctic ships could cause a reduction in the albedo of snow and ice, accelerating snowmelt and sea ice loss. Here we use recently compiled Arctic shipping emission inventories for 2004 and 2050 together with a global aerosol model to quantify the contribution of future Arctic shipping to high‐latitude BC deposition. Our results show that Arctic shipping in 2050 will contribute less than 1% to the total BC deposition north of 60°N due to the much greater relative contribution of BC transported from non‐shipping sources at lower latitudes. We suggest that regulation of the Arctic shipping industry will be an insufficient control on high‐latitude BC deposition.

Estimated impact of black carbon deposition during pre-monsoon season from Nepal Climate Observatory – Pyramid data and snow albedo changes over Himalayan glaciers

Abstract. The possible minimal range of reduction in snow surface albedo due to dry deposition of black carbon (BC) in the pre-monsoon period (March–May) was estimated as a lower bound together with the estimation of its accuracy, based on atmospheric observations at the Nepal Climate Observatory – Pyramid (NCO-P) sited at 5079 m a.s.l. in the Himalayan region. A total BC deposition rate was estimated as 2.89 μg m−2 day−1 providing a total deposition of 266 μg m−2 for March–May at the site, based on a calculation with a minimal deposition velocity of 1.0×10−4 m s−1 with atmospheric data of equivalent BC concentration. Main BC size at NCO-P site was determined as 103.1–669.8 nm by correlation analyses between equivalent BC concentration and particulate size distributions in the atmosphere. The BC deposition from the size distribution data was also estimated. It was found that 8.7% of the estimated dry deposition corresponds to the estimated BC deposition from equivalent BC concentration data. If all the BC is deposited uniformly on the top 2-cm pure snow, the corresponding BC concentration is 26.0–68.2 μg kg−1, assuming snow density variations of 195–512 kg m−3 of Yala Glacier close to NCO-P site. Such a concentration of BC in snow could result in 2.0–5.2% albedo reductions. By assuming these albedo reductions continue throughout the year, and then applying simple numerical experiments with a glacier mass balance model, we estimated reductions would lead to runoff increases of 70–204 mm of water. This runoff is the equivalent of 11.6–33.9% of the annual discharge of a typical Tibetan glacier. Our estimates of BC concentration in snow surface for pre-monsoon season is comparable to those at similar altitudes in the Himalayan region, where glaciers and perpetual snow regions begin, in the vicinity of NCO-P. Our estimates from only BC are likely to represent a lower bound for snow albedo reductions, because we used a fixed slower deposition velocity. In addition, we excluded the effects of atmospheric wind and turbulence, snow aging, dust deposition, and snow albedo feedbacks. This preliminary study represents the first investigation of BC deposition and related albedo on snow, using atmospheric aerosol data observed at the southern slope in the Himalayas.

A multi-model assessment of pollution transport to the Arctic

Abstract. We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe, East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosols and CO, European emissions dominate at the Arctic surface but East Asian emissions become progressively more important with altitude, and are dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute ~40% of total BC deposition to Greenland, with ~20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by European emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physical and chemical processing (including removal). Comparison of modeled aerosol concentrations with observations indicates problems in the models, and perhaps, interpretation of the measurements. For gas phase pollutants such as CO and O3, which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region and altitude examined. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions, and oxidation are comparable for European and North American sources. At higher levels, model-to-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity, though transport also contributes substantially in the mid-troposphere.