Russia has a particularly important role regarding black carbon (BC) emissions given the extent of its territory above the Arctic Circle, where BC emissions have a particularly pronounced effect on ...the climate. This study presents a comprehensive review of BC estimates from a range of studies. We assess underlying methodologies and data sources for each major emissions source based on their level of detail, accuracy and extent to which they represent current conditions. We then present reference values for each major emissions source. In the case of flaring, the study presents new estimates drawing on data on Russian associated petroleum gas and the most recent satellite data on flaring. We also present estimates of organic carbon (OC) for each source, either based on the reference studies or from our own calculations. In addition, the study provides uncertainty estimates for each source. Total BC emissions are estimated at 689 Gg in 2014, with an uncertainty range between (407-1,416), while OC emissions are 9,228 Gg (with uncertainty between 5,595 and 14,728). Wildfires dominated and contributed about 83% of the total BC emissions, however the effect on radiative forcing is mitigated by OC emissions. We also present an adjusted estimate of Arctic forcing from Russian OC and BC emissions. In recent years, Russia has pursued policies to reduce flaring and limit particulate emissions from on-road transport, both of which appear to significantly contribute to the lower emissions and forcing values found in this study.
Black carbon (BC) and carbon monoxide (CO) at different model levels from the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis were comprehensively evaluated against observations performed ...simultaneously on both surface and mountain sites in winter and summer in the North China Plain for the first time. CAMS could capture the seasonal difference in BC and CO emission on both sites but showed significant and persistent biases. Biases were high on the surface site and low on the mountain site for both seasons, implying the uncertainties in emission inventories used in the CAMS reanalysis which may have more influence near source. Biases were reduced and the correlation coefficient of CAMS BC with observed BC increased when two datasets were compared on a daily basis, which suggests daily or longer time averaged CAMS BC could be more suitable for trend analysis. Although CAMS could generally reproduce the distinct diurnal variation of BC and CO on both sites, the inaccurate representation of the daily evolution of planetary boundary layer (PBL) in model may bring more uncertainties to the concentration biases on surface from midnight to early morning. BC hydrophilic ratio from CAMS displayed large biases compared to observations with no seasonal difference on both sites, which was probably resulted from the initial emission state of BC hygroscopicity for all source types in model. Uncertainties in the removal processes and the simplified aging processes in model could further induce uncertainty in modelling BC hydrophilic ratio in the CAMS. These results could not only be referenced for the improvement on CAMS reanalysis but also facilitate model or trend analysis of BC and CO pollution by utilizing the CAMS reanalysis product from both short- and long-term perspectives, which will be beneficial to both the mitigation and policy-making on primary emissions in China.
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•BC and CO from CAMS were evaluated for the first time in the NCP.•CAMS can capture the seasonal and diurnal variations of pollutants.•BC hydrophilic ratio from CAMS displayed large biases compared to observations.
Biochar application has multiple benefits for soil fertility improvement and climate change mitigation. Biochar can act as a source of nutrients and sequester carbon (C) in the soil. The nutrient ...release capacity of biochar once applied to the soil varies with the composition of the biochar, which is a function of the feedstock type and pyrolysis condition used for biochar production. Biochar has a crucial influence on soil C mineralization, including its positive or negative priming of microorganisms involved in soil C cycling. However, in various cases, biochar application to the soil may cause negative effects in the soil and the wider environment. For instance, biochar may suppress soil nutrient availability and crop productivity due to the reduction in plant nutrient uptake or reduction in soil C mineralization. Biochar application may also negatively affect environmental quality and human health because of harmful compounds such as polycyclic aromatic hydrocarbons (PAHs), polychlorinated dibenzodioxins, and dibenzofurans (PCDD/DF). In this review, we discuss the linkage between biochar composition and function, evaluate the role biochar plays in soil fertility improvement and C sequestration, and discuss regulations and concerns regarding biochar's negative environmental impact. We also summarize advancements in biochar production technologies and discuss future challenges and priorities in biochar research.
•Nutrient contents in biochar highly dependent on the feedstock type.•Pyrolysis temperature alters the proportion of aromatic and aliphatic C fractions.•Chemical and physical properties of biochar affect the nutrient release from biochar.•Application of unsuitable biochar can negatively affect environmental quality and human health.•Biochar can be a potential source of polycyclic aromatic hydrocarbons and polychlorinated dibenzodioxins.
•UV–Vis, EEM and FT-ICR-MS to characterize the transformation of DBC in various UV-AOPs.•After UV-AOP treatment, a significant increase in the oxygen content of DBC, indicating substantial ...oxygenation processes.•Mass difference analysis based on 11 types of typical reactions elucidated detailed oxygenation processes.
Dissolved black carbon (DBC) released from biochar, is an essential group in the dissolved organic matter (DOM) pool and is widely distributed in aquatic environments. In various advanced oxidation processes (AOPs), DBC exhibits enhanced free radical scavenging compared to typical DOM, attributed to its smaller molecular weight and more compacted aromatic structure; however, the molecular-level transformations of DBC in different AOPs, such as UV/H2O2, UV/PDS, and UV/Chlorine, remain unclear. This study employed a DBC derived from wheat biochar for experimentation. Characterization involved ultraviolet-visible (UV–Vis) spectroscopy and fluorescence excitation-emission-matrix (EEM) spectroscopy, revealing the transformation of DBC through diminished SUVA254 values and reduced intensity of three-dimensional fluorescence peaks. Further insights into the transformation were gained through Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). After each UV-AOP treatment, a conspicuous augmentation in the oxygen content of DBC was observed. The detailed oxygenation processes were elucidated through mass difference analysis, based on 23 types of typical reactions. Results indicated that oxygenation reactions were most frequently detected in all three UV-AOP treatments. Specifically, the hydroxylation (+O) predominated in UV/H2O2, while the di-hydroxylation (+2O) prevailed in UV/PDS. UV/Chlorine treatments commonly exhibited tri-hydroxylation (+3O), with the identification of 1194 Cl-BPs of unknown structures. This study contributes to a comprehensive understanding of the molecular transformations of DBC induced by various free radicals in different UV-AOP processes, leading to a better understanding of the different fates of DBC in UV-AOP processes. In addition, the identification of DBC as a precursor of by-products will also contribute to the understanding of how to inhibit the generation of by-products.
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Dissolved black carbon (DBC) is the more photoactive component of dissolved organic matter (DOM) pool, which plays a dual role in the photoconversion of aquatic contaminants, acting as both a ...photosensitizer and an inhibitor. However, little is known about the more systematic mechanism by which DBC exhibits a dual effect, which is closely related to the structure composition of DBC. In this study, the differences in characteristics of DBC obtained from 300 °C and 500 °C were compared via UV–vis absorption spectrum, Fluorescence excitation emission matrix spectra (3D-EEM), Fourier transform infrared (FT-IR), and X-ray photoelectron spectroscopy (XPS), and evaluated the promoting and inhibiting effects of DBC on ofloxacin (OFL) photodegradation. It was found that higher pyrolysis temperature reduced the UV absorbance, molecular weight, aromaticity, and phenolics of DBC while increasing the content of quinone/aromatic ketone and humic substances. Photochemical data showed that 3DBC*, 1O2 and ·OH were all participated in the DBC-mediated OFL photodegradation. Wherein, DBC300 (DBCT, where T = pyrolysis temperature) had strong light screening and dynamic quenching effect, but the formation ability of 3DBC*, 1O2 and ·OH was poor, which significantly retarded the photodegradation of OFL. While DBC500 exhibited a slight promotion effect due to its higher formation ability of reactive species and weak light screening effect. Moreover, DBC500 had higher steady-state concentration and (kOFL,3DBC⁎) than DBC300, which might be due to the higher contents of quinone/aromatic ketone and the lower contents of phenol in DBC500, thus enhancing the reactivity of 3DBC* and OFL. Our research systematically revealed the trade-off mechanism of DBC on the photodegradation of fluoroquinolones, and provided an important theoretical guidance for the photodegradation of fluoroquinolones under the evolution of DBC composition.
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•Higher temperature reduced UV absorbance, aromaticity, MW and phenolics.•DBC300 retarded the OFL photodegradation by light screening and dynamic quenching.•DBC500 promoted the photodegradation OFL through the light screening effect.•DBC500 has higher contents of quinone/aromatic ketone and lower contents of phenol.•The generation of RS and the reactivity of 3DBC* and OFL in DBC500 were greater.
The 31st FISU Summer World University Games (SWUG) was held in Chengdu, southwestern China, from July 22 to August 8, 2023. A series of control measures were carried out to ensure good air quality ...during the SWUG, providing an opportunity to investigate the atmospheric behaviors of light-absorbing aerosols under such a substantial disturbance caused by the control measures. To assess the impacts of emission controls on primary pollutants, a field campaign was conducted at a rural site in Chengdu to investigate the characterization of equivalent black carbon (eBC). The changes of eBC concentrations before, during, and after the SWUG were characterized. The sources of eBC were resolved, and the impacts of atmospheric processes on the absorption capacity were also investigated. During the SWUG, the eBC concentration decreased by 12.1 % and 25.3 % compared with those before and after the SWUG. A fossil fuel combustion (eBCff) and a biomass burning (eBCbb) originated eBC were resolved using the aethalometer model. Both eBCff and eBCbb decreased during the SWUG, indicating the effectiveness of control measures. After the SWUG, the influence of biomass burning emissions became more and more significant, and the contribution of brown carbon (BrC) to light absorption at 370–660 nm increased by 52, 19, 7, 6, and 17 % compared to those during the SWUG. As the biomass burning emitted aerosols aged, the absorption Ångström exponent and babs(BrC370nm) decreased gradually, which was mainly due to the photobleaching of the chromophores during the daytime. eBCff was mainly affected by strong wind, while high eBCbb concentration was mainly attributed to the gradual accumulation of biomass-burning emissions near the observation site. The results show the significant reduction of eBC with the implementation of the air pollution mitigation campaign, and provide insights on the impacts of atmospheric processes on BC optical properties during summertime.
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•Black carbon reduced significantly during the Summer World University Games.•Fossil fuel combustion and biomass burning were main sources of black carbon.•Higher absorption Ångström exponent was attributed to biomass-burning emissions.•Brown carbon absorption coefficient reduced as biomass-burning organic aerosol aged.
Heteroaggregation between polystyrene nanoplastics (PSNPs) and soot nanoparticles (STNPs) in aquatic environments may affect their fate and transport. This study investigated the effects of particle ...concentration ratio, electrolytes, pH, and humic acid on their heteroaggregation kinetics. The critical coagulation concentration (CCC) ranked CCCPSNPs > CCCPSNPs-STNPs > CCCSTNPs, indicating that heteroaggregation rates fell between homoaggregation rates. In NaCl solution, as the PSNPs/STNPs ratio decreased from 9/1 to 3/7, heteroaggregation rate decreased and CCCPSNPs-STNPs increased from 200 to 220 mM due to enhanced electrostatic repulsion. Outlier was observed at PSNPs/STNPs= 1/9, where CCCPSNPs-STNPs= 170 mM and homoaggregation of STNPs dominated. However, in CaCl2 solution where calcium bridged with STNPs, heteroaggregation rate increased and CCCPSNPs-STNPs decreased from 26 to 5 mM as the PSNPs/STNPs ratio decreasing from 9/1 to 1/9. In composite water samples, heteroaggregation occurred only at estuarine and marine salinities. Acidic condition promoted heteroaggregation via charge screening. Humic acid retarded or promoted heteroaggregation in NaCl or CaCl2 solutions by steric hindrance or calcium bridging, respectively. Other than van der Waals attraction and electrostatic repulsion, heteroaggregation was affected by steric hindrance, hydrophobic interactions, π − π interactions, and calcium bridging. The results highlight the role of black carbon on colloidal stability of PSNPs in aquatic environments.
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•Stability of homo- and heteroaggregation ranked CCCPSNPs > CCCPSNPs-STNPs > CCCSTNPs.•Decreasing PSNPs/STNPs ratio generally retarded heteroaggregation in NaCl solution.•Reducing PSNPs/STNPs ratio promoted heteroaggregation in CaCl2 solution via bridging.•PSNPs and STNPs underwent heteroaggregation at salinity levels of estuary and ocean.•Heteroaggregation was promoted in HA-CaCl2 solution but retarded in HA-NaCl solution.
We implement a set of new parameterizations into the widely used Snow, Ice, and Aerosol Radiative (SNICAR) model to account for effects of snow grain shape (spherical vs. nonspherical) and black ...carbon (BC)–snow mixing state (external vs. internal). We find that nonspherical snow grains lead to higher pure albedo but weaker BC-induced albedo reductions relative to spherical snow grains, while BC–snow internal mixing significantly enhances albedo reductions relative to external mixing. The combination of snow nonsphericity and internal mixing suggests an important interactive effect on BC-induced albedo reduction. Comparisons with observations of clean and BC-contaminated snow albedo show that model simulations accounting for both snow nonsphericity and BC–snow internal mixing perform better than those using the common assumption of spherical snow grains and external mixing. We further apply the updated SNICAR model with comprehensive in situ measurements of BC concentrations in the Tibetan Plateau snowpack to quantify the present-day (2000–2015) BC-induced snow albedo effects from a regional and seasonal perspective. The BC concentrations show distinct and substantial sub-regional and seasonal variations, with higher values in the non-monsoon season and low altitudes. As a result, the BC-induced regional mean snow albedo reductions and surface radiative effects vary by up to an order of magnitude across different sub-regions and seasons, with values of 0.7–30.7 and 1.4–58.4 W m−2 for BC externally mixed with fresh and aged snow spheres, respectively. The BC radiative effects are further complicated by uncertainty in snow grain shape and BC–snow mixing state. BC–snow internal mixing enhances the mean albedo effects over the plateau by 30–60 % relative to external mixing, while nonspherical snow grains decrease the mean albedo effects by up to 31 % relative to spherical grains. Based on this study, extensive measurements and improved model characterization of snow grain shape and aerosol–snow mixing state are urgently needed in order to precisely evaluate BC–snow albedo effects.
Brown carbon aerosol consists of light‐absorbing organic particulate matter with wavelength‐dependent absorption. Aerosol optical extinction, absorption, size distributions, and chemical composition ...were measured in rural Alabama during summer 2013. The field site was well located to examine sources of brown carbon aerosol, with influence by high biogenic organic aerosol concentrations, pollution from two nearby cities, and biomass burning aerosol. We report the optical closure between measured dry aerosol extinction at 365 nm and calculated extinction from composition and size distribution, showing agreement within experiment uncertainties. We find that aerosol optical extinction is dominated by scattering, with single‐scattering albedo values of 0.94 ± 0.02. Black carbon aerosol accounts for 91 ± 9% of the total carbonaceous aerosol absorption at 365 nm, while organic aerosol accounts for 9 ± 9%. The majority of brown carbon aerosol mass is associated with biomass burning, with smaller contributions from biogenically derived secondary organic aerosol.
Key Points
Aerosol optical extinction in the southeastern U.S. is dominated by scattering
Black carbon is a more significant absorber than organic carbon at 365 nm
Biomass burning makes the largest contribution to organic aerosol absorption
Black carbon (BC) and brown carbon (BrC) are aerosols that absorb light and thereby contribute to climate change. In this study, the light absorption properties and spatiotemporal distributions of ...equivalent BC (eBC) and BrC aerosols were determined based on continuous measurements of aerosol light absorption from January to August 2017, using a seven-channel aethalometer at 49 sampling sites in China. The source apportionments of BC and BrC were identified using the BC/PM2.5, absorption Ångström exponent, the concentration-weighted trajectory method, and the random forest model. Based on the results, BC was the dominant light absorber, whereas BrC was responsible for a higher proportion of the light absorption in northern compared to southern China. The light absorption of BrC was highest in winter (34.3 Mm−1), followed by spring (19.0 Mm−1) and summer (3.6 Mm−1). The combustion of liquid fuels accounted for over 50 % of the light absorption coefficient of BC in most cities and the importance of carbon monoxide (CO) and nitrogen dioxide (NO2) was over 10 % for BC emitted by liquid fuel combustion, based on the random forest model. The contribution of solid fuel combustion to BC in the north was larger than that in the southern regions as coal combustion and crop residue burning are important emission sources of BC in most northern cities. The contribution of primary BrC to light absorption was high in some northern cities, whereas that of secondary BrC was prevalent in some southern cities. The diurnal variations in secondary BrC were affected by changes in odd oxygen and relative humidity, which promoted the photobleaching of the chromophores and aqueous-phase reactions of secondary BrC.
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•High BC concentrations were observed in northern China, and the liquid fuels dominated the light absorption of BC.•Combustion of coal and crop residue were major sources for BC and BrC in northern China during winter.•Temperature, CO, and NO2 were significant contributors to the formation of primary and secondary BrC.•Secondary BrC was affected by photo-oxidation processes and liquid phase reaction.
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