Combustion-derived Black Carbon Research Articles

Impact of combustion-derived black carbon oxidation states on optical properties and cellular metabolomics in HeLa cells: Insights into soot organics

The 2021 WHO guidelines recommend limits for black carbon (BC) due to its role in oxidative stress and inflammation. BC is highly light-absorbing and quickly undergoes coating by secondary organic aerosols (SOA), enhancing their toxicological and optical properties. Using a miniCAST, this study produced BC at six oxidation states. HPLC-DAD-QTOF-MS and LC-MS/MS technologies were employed to characterize the organic coatings on BC and investigate the associated chromophores and metabolomics effects on Hela cells. The chemical compositions of SOA organics resembled those in ambient air. Interestingly, greater BC maturity did not correlate with increased light absorption. Intermediate maturity showed the strongest absorption, with common chromophores but higher intensities. Aliphatic and polyaromatic compounds were the primary absorbers, with C21H41O6 and C24H50N2O4 as the strongest chromophores in ESI+ mode, and C16H32O2 and C10H7NO3 in ESI- mode. Metabonomics and pathway analysis revealed down-regulation of 13 metabolites involved in lipid synthesis in cells exposed to different SOA organics. Plasmalogen, triacylglycerol, and cardiolipin pathways were significantly influenced. Plasmalogens emerged as potential therapeutic targets for neurodegenerative and cardiometabolic diseases, and cardiolipin, a crucial mitochondrial phospholipid for cellular energy production, indicating that reduced metabolites due to SOA organics disrupt cellular lipid homeostasis and alter normal cellular functions.

Source apportionment of black carbon aerosols by isotopes (14C and 13C) and Bayesian modeling from two remote islands in east Asian outflow region

We report the results of source apportionment of combustion-derived black carbon (BC), in PM2.5 aerosols collected from the East Asian continental outflow region at two islands; Okinawa and Fukue during the period from October 2009 to May 2010. The 14C contents of BC from Okinawa (Cape Hedo) and Fukue islands (Fukue) varied from 24.4 to 34.2 pMC and from 18.1 to 43.0 pMC, respectively. Source apportionment of BC was conducted by using a simple 14C mass balance model and a dual-isotope Bayesian Markov chain Monte Carlo model. Biomass combustion contributions (e.g., wood fuel and crop residues) were 23–31 % (mean 27 ± 3 %) at Cape Hedo and 15–38 % (mean 27 ± 12 %) at Fukue. Both sites were equally affected by biomass combustion, whose levels are similar to those observed in the hotspot regions (megacities) in China. Fossil fuel contributions (e.g., oil, gasoline, and diesel) were 69–77 % (mean 74 ± 3 %) with 2–69 % from coal and 3–76 % from liquid fossil at Cape Hedo, and 55–85 % (mean 73 ± 12 %) at Fukue with 3 % from coal and 53–56 % from liquid fuel for the early winter. Those variations for both sites showed significantly different source region-specific trends and this trend was also consistent with the results of the air mass trajectory analysis with a higher contribution of coal-BC from North China including Beijing, and East China including Shanghai. In spring, we found a higher contribution of liquid fossil fuel combustion (e.g., traffic) over the East China Sea, including Pacific air masses, suggesting that the possible contribution of ship emissions was relatively high. Although our results for isotopes-based source apportionment of BC are preliminary, these findings suggest that long-term monitoring of BC aerosols, even in remote sites of Asian outflows, and source-specific descriptions of BC are important to improve climate models. We also recommend further measurements for implementing regionally tailored mitigation.

Nonhomologous Black Carbon Decoupled Char and Soot Sequestration Based on Stable Carbon Isotopes in Tibetan Plateau Lake Sediment.

Combustion-derived black carbon (BC) is an important component of sedimentary carbon pool. Due to different physicochemical properties, determining the source of char and soot is crucial for BC cycling, especially for nonhomologous char and soot in the Tibetan Plateau (TP). This study analyzed the sequestration and source of BC, char, and soot in the Dagze Co (inner TP) sediment core via the content and δ13C, revealing the biomass and fossil fuel driving on nonsynchronous char and soot and their response to local anthropogenic activities and atmospheric transmission. The results showed that BC concentration increased from 1.19 ± 0.35 mg g-1 (pre-1956) to 2.03 ± 1.05 mg g-1 (after 1956). The variation of char was similar to BC, while nonhomologous growth was detected in char and soot (r = 0.29 and p > 0.05). The source apportionment showed that biomass burning for 71.52 ± 10.23% of char and promoted char sequestration. The contribution of fossil fuel combustion to soot (46.67 ± 14.07%) is much higher than char (28.48 ± 10.23%). Redundancy analysis confirmed that local anthropogenic activities significantly influenced BC burial and atmospheric transport from outside TP-regulated BC burial. The contribution of biomass and fossil fuels to nonsynchronous char and soot is conducive to understanding the anthropogenic effect on BC burial in the TP.

Evaluation of black carbon source apportionment based on one year's daily observations in Beijing

Combustion-derived black carbon (BC) is increasingly recognized as a significant pollutant that can have adverse effects on the atmospheric environment, human health, and regional climate. Fossil fuel combustion is the main source of BC, yet understanding of the relative contributions to BC from coal and liquid fuel combustion remains incomplete. Moreover, few studies have assessed the relative contributions based on long-term continuous daily field observations. This study adopted a Bayesian model of a three-dimensional array of a stable carbon isotope and the ratios of non-sea-salt K+ to BC and ΔBC/ΔCO of one year's daily observations (from September 1, 2017 to August 31, 2018) to constrain source apportionment of BC in Beijing (China). Results showed that both the BC and the carbon isotope concentrations exhibited strong seasonal variability, and that the annual BC concentration has decreased significantly in recent years. The Bayesian model results also revealed that the relative contributions from the combustion of coal, liquid fuel, and biomass were 42% ± 18%, 42% ± 18%, and 16% ± 11%, respectively, with a larger contribution from coal (liquid fuel) combustion in winter and spring (summer and autumn). The seasonal variation of source appointment was attributed to local and regional fuel combustion coupled with meteorological conditions. With increasing PM2.5 level, the BC concentration derived from biomass burning increased fastest, followed by that derived from coal combustion. But concentration of secondary inorganic ions increased faster than BC as PM2.5 increased.

Exposure to wood smoke particles leads to inflammation, disrupted proliferation and damage to cellular structures in a human first trimester trophoblast cell line

The ongoing transition to renewable fuel sources has led to increased use of wood and other biomass fuels. The physiochemical characteristics of biomass combustion derived aerosols depends on appliances, fuel and operation procedures, and particles generated during incomplete combustion are linked to toxicity. Frequent indoor wood burning is related to severe health problems such as negative effects on airways and inflammation, as well as chronic hypoxia and pathological changes in placentas, adverse pregnancy outcome, preterm delivery and increased risk of preeclampsia. The presence of combustion-derived black carbon particles at both the maternal and fetal side of placentas suggests that particles can reach the fetus. Air pollution particles have also been shown to inhibit trophoblast migration and invasion, which are vital functions for the development of the placenta during the first trimester. In this study we exposed a placental first trimester trophoblast cell line to wood smoke particles emitted under Nominal Burn rate (NB) or High Burn rate (HB). The particles were visible inside exposed cells and localized to the mitochondria, causing ultrastructural changes in mitochondria and endoplasmic reticulum. Exposed cells showed decreased secretion of the pregnancy marker human chorionic gonadotropin, increased secretion of IL-6, disrupted membrane integrity, disrupted proliferation and contained specific polycyclic aromatic hydrocarbons (PAHs) from the particles. Taken together, these results suggest that wood smoke particles can enter trophoblasts and have detrimental effects early in pregnancy by disrupting critical trophoblast functions needed for normal placenta development and function. This could contribute to the underlying mechanisms leading to pregnancy complications such as miscarriage, premature birth, preeclampsia and/or fetal growth restriction. This study support the general recommendation that more efficient combustion technologies and burning practices should be adopted to reduce some of the toxicity generated during wood burning.

Associations of black carbon and PM2.5 with daily cardiovascular mortality in Beijing, China

Due to its twofold effects on climate change and air quality, black carbon (BC) is of wide concern in the atmospheric sciences. Considerable uncertainty exists as to the health effects of atmospheric BC for the limited epidemiological and toxicological studies. As combustion-derived BC is one important component of PM2.5 (particles with aerodynamic diameters less than 2.5 μm), the question remains of whether or not BC may play an important role in PM2.5-related health risks. To quantitatively analyze the short-term health effects of BC and PM2.5, a confounder-adjusted semi-parametric generalized additive model (GAM) of a time series study was used to calculate the concentration-response relationship between BC and PM2.5 and daily cardiovascular disease (CVD) mortality from 2006 to 2011 in Beijing. During the study period, the mean daily concentrations of BC and PM2.5 were 6.8 μg/m3 and 75.9 μg/m3, respectively. The results showed that BC was significantly associated with CVD mortality, and an interquartile range (IQR) increase in BC (5.7 μg/m3) and PM2.5 (64. 5 μg/m3) were associated with 2.70% (95% CI: 2.20, 3.21) and 4.06% (95% CI: 3.47, 4.65) increase in CVD mortality. The health risk associated with BC may less than that of PM2.5. When adjusted for nitrogen dioxide (NO2) and sulfur dioxide (SO2), the effects of BC remained statistically significant. It showed the relatively difference between BC and PM2.5 when it comes to the modification effects of age, gender and educational attainment. These findings provide valuable evidence to the rare studies of the concentration-response relationship of BC with human health in developing countries.

Intra-regional transport of black carbon between the south edge of the North China Plain and central China during winter haze episodes

Abstract. Black carbon (BC), which is formed from the incomplete combustion of fuel sources (mainly fossil fuel, biofuel and open biomass burning), is a chemically inert optical absorber in the atmosphere. It has significant impacts on global climate, regional air quality and human health. During transportation, its physical and chemical characteristics as well as its sources change dramatically. To investigate the properties of BC (i.e., mass concentration, sources and optical properties) during intra-regional transport between the southern edge of the North China Plain (SE-NCP) and central China (CC), simultaneous BC observations were conducted in a megacity (Wuhan – WH) in CC, in three borderline cities (Xiangyang – XY, Suixian – SX and Hong'an – HA; from west to east) between the SE-NCP and CC, and in a city (Luohe – LH) in the SE-NCP during typical winter haze episodes. Using an Aethalometer, the highest equivalent BC (eBC) mass concentrations and the highest aerosol absorption coefficients (σabs) were found in LH in the SE-NCP, followed by the borderline cities (XY, SX and HA) and WH. The levels, sources, optical properties (i.e., σabs and absorption Ångström exponent, AAE) and geographic origins of eBC were different between clean and polluted periods. Compared with clean days, higher eBC levels (26.4 %–163 % higher) and σabs (18.2 %–236 % higher) were found during pollution episodes due to the increased combustion of fossil fuels (increased by 51.1 %–277 %), which was supported by the decreased AAE values (decreased by 7.40 %–12.7 %). The conditional bivariate probability function (CBPF) and concentration-weighted trajectory (CWT) results showed that the geographic origins of biomass burning (BCbb) and fossil fuel (BCff) combustion-derived BC were different. Air parcels from the south dominated for border sites during clean days, with contributions of 46.0 %–58.2 %, whereas trajectories from the northeast showed higher contributions (37.5 %–51.2 %) during pollution episodes. At the SE-NCP site (LH), transboundary influences from the south (CC) exhibited a more frequent impact (with air parcels from this direction comprising 47.8 % of all parcels) on the ambient eBC levels during pollution episodes. At WH, eBC was mainly from the northeast transport route throughout the observation period. Two transportation cases showed that the mass concentrations of eBC, BCff and σabs all increased, from upwind to downwind, whereas AAE decreased. This study highlights that intra-regional prevention and control for dominant sources at each specific site should be considered in order to improve the regional air quality.

Wood stove use and other determinants of personal and indoor exposures to particulate air pollution and ozone among elderly persons in a Northern Suburb.

A six‐month winter‐spring study was conducted in a suburb of the northern European city of Kuopio, Finland, to identify and quantify factors determining daily personal exposure and home indoor levels of fine particulate matter (PM2.5, diameter <2.5 µm) and its light absorption coefficient (PM2.5abs), a proxy for combustion‐derived black carbon. Moreover, determinants of home indoor ozone (O3) concentration were examined. Local central site outdoor, home indoor, and personal daily levels of pollutants were monitored in this suburb among 37 elderly residents. Outdoor concentrations of the pollutants were significant determinants of their levels in home indoor air and personal exposures. Natural ventilation in the detached and row houses increased personal exposure to PM2.5, but not to PM2.5abs, when compared with mechanical ventilation. Only cooking out of the recorded household activities increased indoor PM2.5. The use of a wood stove room heater or wood‐fired sauna stove was associated with elevated concentrations of personal PM2.5 and PM2.5abs, and indoor PM2.5abs. Candle burning increased daily indoor and personal PM2.5abs, and it was also a determinant of indoor ozone level. In conclusion, relatively short‐lasting wood and candle burning of a few hours increased residents’ daily exposure to potentially hazardous, combustion‐derived carbonaceous particulate matter.

Regionally-Varying Combustion Sources of the January 2013 Severe Haze Events over Eastern China

Thick haze plagued northeastern China in January 2013, strongly affecting both regional climate and human respiratory health. Here, we present dual carbon isotope constrained (Δ(14)C and δ(13)C) source apportionment for combustion-derived black carbon aerosol (BC) for three key hotspot regions (megacities): North China Plain (NCP, Beijing), the Yangtze River Delta (YRD, Shanghai), and the Pearl River Delta (PRD, Guangzhou) for January 2013. BC, here quantified as elemental carbon (EC), is one of the most health-detrimental components of PM2.5 and a strong climate warming agent. The results show that these severe haze events were equally affected (∼ 30%) by biomass combustion in all three regions, whereas the sources of the dominant fossil fuel component was dramatically different between north and south. In the NCP region, coal combustion accounted for 66% (46-74%, 95% C.I.) of the EC, whereas, in the YRD and PRD regions, liquid fossil fuel combustion (e.g., traffic) stood for 46% (18-66%) and 58% (38-68%), respectively. Taken together, these findings suggest the need for a regionally-specific description of BC sources in climate models and regionally-tailored mitigation to combat severe air pollution events in East Asia.

Black carbon in urban topsoils of Xuzhou (China): environmental implication and magnetic proxy

Combustion-derived black carbon has received attention as a form of refractory organic carbon that may be preferentially preserved in soils and sediments. However, little is understood about the environmental roles of black carbon in urban soils. This investigation represented the preliminary study to characterize black carbon (BC) concentrations and enrichment ratios in Xuzhou urban roadside topsoil. Data from 21 roadside topsoil samples showed that the median of BC concentrations is 21.8 mg/g, which is significantly higher than local background value that averages 3.8 mg/g. Hierarchical clustering analysis indicated that BC in Xuzhou urban roadside soils are mainly from the traffic emissions. The marked positive correlations between BC and the concentrations of heavy metals (Pb, Cu, Zn, Mo, and Sc; Pearson correlation coefficient, 0.623, 0.809, 0.846, 0.742 and 0.831, respectively) suggested that these heavy metals are likely to be strongly retained by BC present in roadside topsoil. The significant positive correlation between BC and specific magnetic susceptibility was also observed. Thus, the simple environmental magnetic method is potentially an efficient alternative technique for assessing BC concentration in roadside topsoil.

Black carbon in marine particulate organic carbon: Inputs and cycling of highly recalcitrant organic carbon in the Gulf of Maine

To increase our understanding of the roles of black carbon (BC), a highly sorptive and recalcitrant material, we measured BC concentrations and fluxes in marine particulate organic carbon (POC) out of the water column in the Gulf of Maine (GoM), a representative coastal area downwind of important BC sources of the Northeastern United States. Concentrations ranged from < 0.1 to 16 μg/L in the spring and late summer, typically contributing between 1 and 20% of the POC. Water-column export fluxes were near 10 g BC/m 2∙yr. These observations suggest that (a) up to 50% of the “molecularly uncharacterized” POC in this region's seawater is combustion-derived BC, and (b) the “bioavailabilities” of hydrophobic pollutants like polycyclic aromatic hydrocarbons (PAHs) would be influenced substantially by sorption to BC. The observed BC spatial distributions imply that a large part of the BC was carried offshore by wind and that much of it is accumulated in the coastal sediments. On a global scale, these results suggest the GoM and other coastal areas with similar BC loadings accumulate significant amounts of highly recalcitrant organic carbon that remineralizes on geological time scales in the world's oceans.

Reburial of fossil organic carbon in marine sediments.

Marine sediments act as the ultimate sink for organic carbon, sequestering otherwise rapidly cycling carbon for geologic timescales. Sedimentary organic carbon burial appears to be controlled by oxygen exposure time in situ, and much research has focused on understanding the mechanisms of preservation of organic carbon. In this context, combustion-derived black carbon has received attention as a form of refractory organic carbon that may be preferentially preserved in soils and sediments. However, little is understood about the environmental roles, transport and distribution of black carbon. Here we apply isotopic analyses to graphitic black carbon samples isolated from pre-industrial marine and terrestrial sediments. We find that this material is terrestrially derived and almost entirely depleted of radiocarbon, suggesting that it is graphite weathered from rocks, rather than a combustion product. The widespread presence of fossil graphitic black carbon in sediments has therefore probably led to significant overestimates of burial of combustion-derived black carbon in marine sediments. It could be responsible for biasing radiocarbon dating of sedimentary organic carbon, and also reveals a closed loop in the carbon cycle. Depending on its susceptibility to oxidation, this recycled carbon may be locked away from the biologically mediated carbon cycle for many geologic cycles.

Assessing the Combined Roles of Natural Organic Matter and Black Carbon as Sorbents in Sediments

We hypothesized that two mechanisms, absorption into natural organic matter and adsorption onto combustion-derived black carbon (BC), act in parallel to bind polycyclic aromatic hydrocarbons (PAHs) to Boston Harbor sediments. To focus on BC-adsorption, we removed the non-BC fraction by combusting near shore sediments at 375 degrees C for 24 h under air, leaving ca. 16% of the reduced carbon. The isotherm for pyrene sorption onto our combusted sediment was nonlinear with a Freundlich exponent of 0.62+/-0.12 and a BC-normalized distribution coefficient (microg/ kgBC)/(microg/L)n of 10(6.25)+/-0.14. Pyrene sorption to untreated sediment was reasonably estimated using Kd = f(oc) 10(4.7) + fBC 10(6.25) Cw(0.62-1) where f(oc) was the non-BC organic carbon content, 10(4.7) was the organic carbon-normalized absorption coefficient for pyrene (L/kg(oc)), fBC was the BC content, and Cw was the dissolved pyrene concentration (microg/ L). C/H/N ratios indicated that our environmental BC differed substantially from NIST diesel soot, possibly due to inclusion of larger BC particles from near source atmospheric fallout and urban runoff. The impact of BC on total PAH sorption may explain reports of nonlinear isotherms, Koc values for PAHs that exceed their respective Kow values, and discrepancies in bioavailability between planar and nonplanar sorbates.