Brown Carbon Emission Research Articles

Brownness of organics in anthropogenic biomass burning aerosols over South Asia

Abstract. In South Asia, biomass is burned for energy and waste disposal, producing brown carbon (BrC) aerosols whose climatic impacts are highly uncertain. To assess these impacts, a real-world understanding of BrC's physio-optical properties is essential. For this region, the order-of-magnitude variability in BrC's spectral refractive index as a function of particle volatility distribution is poorly understood. This leads to oversimplified model parameterization and subsequent uncertainty in regional radiative forcing. Here we used the field-collected aerosol samples from major anthropogenic biomass activities to examine the methanol-soluble BrC optical properties. We show a strong relation between the absorption strength, wavelength dependence, and thermo-optical fractions of carbonaceous aerosols. Our observations show strongly absorbing BrC near the Himalayan foothills that may accelerate glacier melt, further highlighting the limitations of climate models where variable BrC properties are not considered. These findings provide crucial inputs for refining climate models and developing effective regional strategies to mitigate BrC emissions.

Brown Carbon Emissions from Biomass Burning under Simulated Wildfire and Prescribed-Fire Conditions.

We investigated the light-absorption properties of brown carbon (BrC) as part of the Georgia Wildland-Fire Simulation Experiment. We constructed fuel beds representative of three ecoregions in the Southeastern U.S. and varied the fuel-bed moisture content to simulate either prescribed fires or drought-induced wildfires. Based on decreasing fire radiative energy normalized by fuel-bed mass loading (FREnorm), the combustion conditions were grouped into wildfire (Wild), prescribed fire (Rx), and wildfire involving duff ignition (WildDuff). The emitted BrC ranged from weakly absorbing (WildDuff) to moderately absorbing (Rx and Wild) with the imaginary part of the refractive index (k) values that were well-correlated with FREnorm. We apportioned the BrC into water-soluble (WSBrC) and water-insoluble (WIBrC). Approximately half of the WSBrC molecules detected using electrospray-ionization mass spectrometry were potential chromophores. Nevertheless, k of WSBrC was an order of magnitude smaller than k of WIBrC. Furthermore, k of WIBrC was well-correlated with FREnorm while k of WSBrC was not, suggesting different formation pathways between WIBrC and WSBrC. Overall, the results signify the importance of combustion conditions in determining BrC light-absorption properties and indicate that variables in wildland fires, such as moisture content and fuel-bed composition, impact BrC light-absorption properties to the extent that they influence combustion conditions.

Predicted Concentrations and Optical Properties of Brown Carbon from Biomass Burning over Europe.

Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosol components that can contribute to radiative forcing and thus affect the climate. In this study, we focus on the modification of aerosol optical properties associated with BrC emissions from biomass burning. BrC is simulated with the introduction of three new species in the three-dimensional chemical transport model PMCAMx-SR, two primary-absorbing (inert and reactive BrC) species, and one "photobleached" BrC species. 10% of the emitted BrC is assumed to be inert, and the rest to be reactive and able to undergo photobleaching. The scattering and absorption coefficients of the aerosol for different wavelengths are estimated by using Mie theory. BrC causes a 5-15% increase of the aerosol optical depth at 550 nm in regions affected by fires and can increase light absorption by up to 12% compared to when there is no BrC. During major biomass burning events, the absorption of BrC can reach up to 13% of that of BC at 550 nm and 25% at 440 nm. The ability of the model to reproduce measured absorption is improved when BrC is added to the light-absorbing components.

Pollutant emissions from biomass burning: A review on emission characteristics, environmental impacts, and research perspectives

Biomass is one most abundant resource on the earth providing important energies in support of socioeconomic development in many areas. Burning of biomass fuels comprises to nearly 10% of the total energy from anthropogenic combustion processes; however, as the burning is usually incomplete, this process yields products of incomplete combustion posing consequently significant impacts on air quality, human health, and climate change. Here, we analyzed spatiotemporal characteristics in intentional and unintentional biomass burning from different sectors, discussed impacts of biomass burning emissions on indoor and outdoor air quality, and consequent influences on human health. The global total consumption amount of biomass including both natural and anthropogenic sources was approximately 7900 Tg in 2019, with significantly large regional and sectorial discrepancies among regions. Globally, anthropogenic biomass burning amounts increased gradually, but notably in some developing countries like China residential consumption of biomass fuels, as one large sector of biomass use, decreased over time. Uncommercial biomass consumption needs to be accurately quantified. There are relatively rich datasets of pollutant emission factors from biomass burning, including laboratory and field tests, but still large variations exit and contribute substantially to the uncertainty in emission inventory. Global primary PM2.5, black carbon and organic carbon emissions from biomass burning were about 51, 4.6, and 29 Tg, respectively, contributing to nearly 70%, 55%, and 90% of the total emission from all sources, and emissions from the residential sector and open fires are major sources. Brown carbon emissions from biomass burning attracts growing interests but available studies adopted different methodologies challenging the comparability of those results. Biomass burning emissions polluted not only ambient air but more severely indoor air quality, adversely affecting human health. Future studies that should be emphasized and promoted are suggested.

Effects of Bio-Coal Briquette for Residential Combustion on Brown Carbon Emission Reduction

Biomass burning is an important source of brown carbon (BrC) which poses high-risk threats to human health and the environment. In this study, bio-coal briquette (coal mixed with biomass), a promising solid fuel for residential combustion, is proven to be a clean fuel which can effectively reduce BrC emission. First of all, an orthogonal experiment with three factors and three levels on the physical property of bio-briquette was carried out to identify the optimal preparation conditions including the ratio of biomass to anthracite, particle size and molding pressure. Then a combustion experiment of the bio-coal briquetted was implemented in a simulated residential combustion system. BrC emission factors (EFs) were calculated based on the detected black carbon (BC) concentration by an aethalometer, and other optical characteristics for organic components of extract samplers, such as mass absorption efficiency (MAE) and absorption angstrom index (AAE), were also explored. Lastly, composition analysis of BrC by a gas chromatography (GC) tandem mass spectrometer (MS) and direct visible images by scanning electron microscopy (SEM) were investigated to provide more detail information on BrC EFs and property change. It was shown that bio-coal briquette had such low BrC EFs that 70–81% BrC was reduced in comparison with an interpolation value of 100% biomass and 100% coal. Furthermore, the composition of BrC from bio-coal briquette burning was different, which consisted of more substances with strong wavelength dependence. Consequently, although MAE declined by 60% at a 540 nm wavelength, the AAE value of bio-coal briquette only decreased slightly compared with interpolation values. To be more specific, tar balls, the main existing form of BrC, were distributed much more sparsely in the SEM image of bio-coal briquette. To sum up, a positive reduction effect on BrC was discovered in bio-coal briquette. It is evident that bio-coal briquette can serve as an alternative solid fuel for residential combustion, which is beneficial for both human health and the atmosphere.

Emission and optical characteristics of brown carbon in size-segregated particles from three types of Chinese ships

Brown carbon (BrC) is one of the important light absorption substances that have high light absorption ability under short wavelength light. However, limit studies have focused on the BrC emission from ships. In this study, size-segregated particulate matters (PM) were collected from three different types of ships, light absorption characteristics and size distribution of methanol-soluble BrC and water-soluble BrC in PM from ship exhausts were investigated. Results showed that four-stroke low-power diesel fishing boat (4-LDF) had the highest mass concentrations of methanol-soluble organic carbon (MSOC) and water-soluble organic carbon (WSOC), followed by 2-stroke high-power heavy-fuel-oil vessel (2-HHV), and four-stroke high-power marine-diesel vessel (4-HMV). While 2-HHV had obviously higher light absorption coefficients of methanol-soluble BrC (Abs365,M) and water-soluble BrC (Abs365,W) in unit weight of PM than the other two types of ships. The tested ships presented comparable or higher absorption efficiency of BrC in water extracts (MAE365,W) compared with other BrC emission sources. Majority of BrC was concentrated in fine particles, and the particle size distributions of both Abs365,M and Abs365,W showed bimodal patterns, peaking at 0.43–0.65 µm and 4.7–5.8 µm, respectively. However, different particle size distributions were found for MAE365,M between diesel and heavy fuel oil ships. Besides, different wavelength dependence in particles with different size were also detected. Ship exhaust could be confirmed as a non-ignorable BrC emission source, and complex influencing factor could affect the light absorption characteristics of ship emissions. Particle size should also be considered when light absorption ability of BrC was evaluated.

Broadband spectrum characteristics and radiative effects of primary brown carbon from wood pyrolysis

Brown carbon (BrC), known as light-absorbing organic aerosol in the near-ultraviolet (UV) and short visible region, plays a significant role in the global and regional climate change. A detailed understanding of the spectral optical properties of BrC is beneficial for reducing the uncertainty in radiative forcing calculation. In this work, the spectral properties of primary BrC were investigated by using a four-wavelength broadband cavity-enhanced albedometer with central wavelengths at 365, 405, 532 and 660 nm. The BrC samples were generated by the pyrolysis of three types of wood. During the pyrolysis process, the measured average single scattering albedo (SSA) at 365 nm was about 0.66 to 0.86, where the average absorption Ångström exponent (AAE) was between 5.8 and 7.8, and the average extinction Ångström exponent (EAE) was within 2.1 to 3.5. The full spectral measurement of SSA (300–700 nm) was realized by an optical retrieval method and the retrieved SSA spectrum was directly applied to evaluate aerosol direct radiative forcing (DRF) efficiency. The DRF efficiency over ground of various primary BrC emissions increased from 5.3 % to 68 % as compared to the non-absorbing organic aerosol assumption. A decrease of about 35 % in SSA would cause the DRF efficiency over ground to change from cooling effect to warming effect (from −0.33 W/m2 to +0.15 W/m2) in the near-UV band (365–405 nm). The DRF efficiency over ground of strongly absorptive primary BrC (lower SSA) contributed 66 % more than weakly absorptive primary BrC (higher SSA). These findings proved the importance of broadband spectral properties of BrC, which are substantial for radiative forcing evaluation of BrC and should be considered in global climate models.

Optical properties of vehicular brown carbon emissions: Road tunnel and chassis dynamometer tests

Brown carbon (BrC), as an important light-absorbing aerosol, significantly impacts regional and global climate. Vehicle emission is a nonnegligible source of BrC, but the optical properties of BrC emitted from vehicles remain poorly understood. This study evaluates the absorption Ångström exponent (AAE) of traffic-related light-absorbing aerosols (i.e., AAETr) and the absorption emission factor (EFabs) of vehicular BrC via chassis dynamometer tests and a road tunnel measurement in Tianjin, China. AAETr are estimated as 0.98–1.33 and 1.11 ± 0.001 for tested vehicles and on-road vehicle fleet, respectively. The AAE of vehicular BrC (AAEBrC) is 3.83 ± 0.092 for on-road vehicle fleet. The vehicle technology updates effectively reduce the EFabs of vehicular BrC. Among the four tested China 5 and China 6 gasoline vehicles in the chassis dynamometer tests, BrC EFabs of China 5 gasoline direct injection vehicle is the highest, while China 6 mixing fuel injection vehicle exhibits the lowest EFabs. The BrC EFabs of on-road vehicle fleet at 370 nm wavelength are 0.081 ± 0.0058 m2 kg−1 for mixed fleet, 0.074 ± 0.018 m2 kg−1 for gasoline vehicles (GVs), and 1.66 ± 0.71 m2 kg−1 for diesel vehicles (DVs) in the tunnel measurement. EFabs of GV fleet in the road tunnel is higher than China 5 and China 6 vehicles, as China 1–4 vehicles accounted for 26.8% of the total vehicle fleet in the tunnel. EFabs of vehicular BrC are lower than those from biomass burning and coal combustion emissions. The light absorption of BrC from GVs and DVs accounts for 7.2 ± 2.1% and 1.5 ± 0.77% of total traffic-related absorption at 370 nm, respectively. Our study provides optical features of BrC from vehicle source and could contribute to estimating the impacts of vehicular aerosol emissions on global and regional climate change.

Assessment of carbonaceous aerosols at Mukteshwar: A high-altitude (~2200 m amsl) background site in the foothills of the Central Himalayas

The present study examined the equivalent black carbon (eBC) mass concentrations measured over 10.5 years (September 2005–March 2016) using a 7-wavelength Aethalometer (AE-31) at Mukteshwar, a high-altitude and regional background site in the foothills of Indian central Himalayas. The total spectral absorption coefficient (babs) was divided into three categories: black carbon (BC) and brown carbon (BrC); fossil fuels (FF) and wood/biomass burning (WB/BB); and primary and secondary sources. At the wavelength of 370 nm, a significant BrC contribution (25 %) to the total babs is identified, characterized by a pronounced seasonal variation with winter (December–January-February) maxima (31 %) and post-monsoon (October and November) minima (20 %); whereas, at 660 nm, the contribution of BrC is dramatically less (9 %). Climatologically, the estimated BCFF at 880 nm ranges from 0.25 ± 0.19 μg m−3 in July to 1.17 ± 0.80 μg m−3 in May with the annual average of 0.67 ± 0.63 μg m−3, accounting for 79 % of the BC mass. The maximum BCFF/BC fraction reaches its peak value during the monsoon (July and August, 85 %), indicating the dominance of local traffic emissions due to tourism activities. Further, the highest BCWB concentration observed during pre-monsoon (March–May) suggests the influence of local forest fires along with long-range transported aerosols from the low-altitude plains. The increased contribution of BrC (26 % at 370 nm) and WB absorption (61 % at 370 nm) to the total absorption at the shorter wavelengths suggests that wood burning is one of the major sources of BrC emissions. Secondary BrC absorption accounts for 24 % [91 %] of the total absorption [BrC absorption] at 370 nm, implying the dominance of secondary sources in BrC formation. A trend analysis for the measured BC concentration shows a statistically significant increasing trend with a slope of 0.02 μgm−3/year with a total increase of about 22 % over the study period. A back trajectory-based receptor model, potential source contribution function (PSCF), was used to identify the potential regional source region of BC. The main source regions of BC are the northwest states of India in the IGP region and the northeast Pakistan region.

Brown carbon absorption and radiative effects under intense residential wood burning conditions in Southeastern Europe: New insights into the abundance and absorptivity of methanol-soluble organic aerosols

Biomass burning is a major source of Brown Carbon (BrC), strongly contributing to radiative forcing. In urban areas of the climate-sensitive Southeastern European region, where strong emissions from residential wood burning (RWB) are reported, radiative impacts of carbonaceous aerosols remain largely unknown. This study examines the absorption properties of water- and methanol-soluble organic carbon (WSOC, MeS_OC) in a city (Ioannina, Greece) heavily impacted by RWB. Measurements were performed during winter (December 2019 – February 2020) and summer (July – August 2019) periods, characterized by RWB and photochemical processing of organic aerosol (OA), respectively. PM2.5 filter extracts were analyzed spectrophotometrically for water- and methanol-soluble BrC (WS_BrC, MeS_BrC) absorption. WSOC concentrations were quantified using TOC analysis, while those of MeS_OC were determined using a newly developed direct quantification protocol, applied for the first time to an extended series of ambient samples. The direct method led to a mean MeS_OC/OC of 0.68 and a more accurate subsequent estimation of absorption efficiencies. The mean winter WS_BrC and MeS_BrC absorptions at 365 nm were 13.9 Mm−1 and 21.9 Mm−1, respectively, suggesting an important fraction of water-insoluble OA. Mean winter WS_BrC and MeS_BrC absorptions were over 10 times those observed in summer. MeS_OC was more absorptive than WSOC in winter (mean mass absorption efficiencies – MAE365: 1.81 vs 1.15 m2 gC−1) and especially in summer (MAE: 1.12 vs 0.27 m2 gC−1) due to photo-dissociation and volatilization of BrC chromophores. The winter radiative forcing (RF) of WS_BrC and MeS_BrC relative to elemental carbon (EC) was estimated at 8.7 % and 16.7 %, respectively, in the 300–2500 nm band. However, those values increased to 48.5 % and 60.2 % at 300–400 nm, indicating that, under intense RWB, BrC forcing becomes comparable to that of soot. The results highlight the consideration of urban BrC emissions in radiative transfer models, as a considerable climate forcing factor.

Tunnel measurements reveal significant reduction in traffic-related light-absorbing aerosol emissions in China

Light-absorbing aerosols (LAA), including black carbon (BC) and brown carbon (BrC), profoundly impact regional and global climate. Vehicle emission is an important source of LAA in urban areas, but real-world emission features of LAA from the urban vehicle fleet are not fully understood. This study evaluates traffic-related BC and BrC emission factors (EFs) and their vehicular emission inventories via road tunnel measurements in Tianjin, China, in 2017 and 2021. The distance-based and fuel-based EFs of BC for the mixed fleet were 1.05 ± 1.28 mg km−1 veh−1 and 0.057 ± 0.057 g (kg-fuel)−1, respectively, in 2021, with a dramatic decrease of 80.6 % compared to those in 2017. The BC EFs for gasoline vehicles (GVs, including traditional gasoline and hybrid vehicles) and diesel vehicles (DVs) were 0.55 ± 0.065 mg km−1 veh−1 and 10.5 ± 2.52 mg km−1 veh−1, respectively, in 2021. Compared to 2017, the BrC EFs also decreased significantly in 2021, by 10.8–53.6 %, with 0.32 ± 0.45 mg km−1 veh−1 and 0.018 ± 0.020 g (kg-fuel)−1 of distance-based and fuel-based EFs for mixed fleet. The BrC EFs for GVs and DVs were 0.091 ± 0.024 mg km−1 veh−1 and 3.06 ± 0.91 mg km−1 veh−1, respectively, in 2021. Based on the BC and BrC EFs for GVs and DVs and annual mileage for each vehicle category, the annual vehicular LAA emission inventories were estimated. From 2017 to 2021, the annual vehicular LAA emissions in Tianjin have been significantly reduced, by 69 % for BC and 10 % for BrC. DVs account for a small amount of the vehicle population (8.4 %), but contribute to most of the BC (83 %) and BrC (86 %). Our study demonstrates the significant reduction of vehicular light-absorbing aerosols emission due to vehicle pollution prevention and control in China.

Global brown carbon emissions from combustion sources

Light-absorbing organic carbon (OC), sometimes known as Brown Carbon (BrC), has been recognized as an important fraction of carbonaceous aerosols substantially affecting radiative forcing. This study firstly developed a bottom-up estimate of global primary BrC, and discussed its spatiotemporal distribution and source contributions from 1960 to 2010. The global total primary BrC emission from both natural and anthropogenic sources in 2010 was 7.26 (5.98–8.93 as an interquartile range) Tg, with 43.5% from anthropogenic sources. High primary BrC emissions were in regions such as Africa, South America, South and East Asia with natural sources (wild fires and deforestation) contributing over 70% in the former two regions, while in East Asia, anthropogenic sources, especially residential solid fuel combustion, accounted for over 80% of the regional total BrC emissions. Globally, the historical trend was mainly driven by anthropogenic sources, which increased from 1960 to 1990 and then started to decline. Residential emissions significantly impacted on emissions and temporal trends that varied by region. In South and Southeast Asia, the emissions increased obviously due to population growth and a slow transition from solid fuels to clean modern energies in the residential sector. It is estimated that in primary OC, the global average was about 20% BrC, but this ratio varied from 13% to 47%, depending on sector and region. In areas with high residential solid fuel combustion emissions, the ratio was generally twice the value in other areas. Uncertainties in the work are associated with the concept of BrC and measurement technologies, pointing to the need for more studies on BrC analysis and quantification in both emissions and the air.

Realistic operation of two residential cordwood-fired outdoor hydronic heater appliances—Part 3: Optical properties of black and brown carbon emissions

ABSTRACT Residential biomass combustion is a source of carbonaceous aerosol. Inefficient combustion, particularly of solid fuels produces large quantities of black and brown carbon (BC and BrC). These particle types are important as they have noted effects on climate forcing and human health. One method of measuring these quantities is by measurement of aerosol light-absorption and scattering, which can be performed using an aethalometer and nephelometer, respectively. These instruments are widely deployed in the study of ambient air and are frequently used in air quality modeling and source apportionment studies. In this study, we will describe (1) a method for measuring primary BC and BrC emissions from two residential log-fired wood hydronic heaters and (2) the BC and BrC emission from these devices over a wide range of operating conditions, such as cold-starts, warm-starts, four different levels of output ranging from 15% to 100% maximum rated output, and periods of repeated cycling. The range in flue-gas BC concentrations, measured using an aethalometer at the 880 nanometer (nm) wavelength, were between 5.09 × 102 and 2.24 × 104 micrograms per cubic meter (µg/m3) while the scattering coefficient of the flue-gas, measured by a nephelometer at 880 nm, ranged between 2.20 × 103 and 8.56 × 105 inverse megameters (Mm−1). The BrC concentrations, measured using the 370 nm wavelength of an aethalometer, were between 9.10 × 101 and 3.56 × 104 µg/m3. The calculated Angstrom Absorption Exponent (AAE) of the flue-gas aerosol ranged between 1.54 and 3.63. Performing a comparison between the measured BC concentration and an external particulate matter (PM) concentration showed that overall BC makes up roughly a quarter of the PM emitted by either of the two appliances. Further for both appliances, the cold-start and the test phase immediately following it had the highest BC and BrC concentrations, the highest measured scattering coefficient, as well as a low AAE. Implications: In this work we provide information on the black and brown carbon emissions from outdoor cordwood-fired hydronic heaters. Aethalometer based black carbon measurements are common in atmospheric science, but are uncommonly used in laboratory studies. This work helps to bridge that gap. This data helps to inform the work of modelers and policy makers interested in hydronic heaters and source apportioning biomass combustion emissions.

Source profiles of molecular structure and light absorption of PM2.5 brown carbon from residential coal combustion emission in Northwestern China

Residential coal combustion is a prominent source of brown carbon (BrC) aerosols, but knowledge of their molecular structures and optical absorption were limited, which have notable used in ambient BrC source identification and radiative forcing calculation. In this study, the Fourier transform–ion cyclotron resonance mass spectrometry combined with partial least squares regression analysis as well as Fourier transform infrared spectroscopy analysis were used to insight the molecular compounds and structures of BrC from anthracite and bituminous coal combustions between traditional and improved stoves. The absorption Ångström exponents (AAE) and mass absorption efficiency (MAE) values for the BrC emitted from the combinations of bituminous were both 1.2–2.5 times lower than those of anthracite, interpreting that the BrC from the anthracite emissions had greater light-absorbing capacity. In contrast, the emission factor of light absorption (EFAbs) at 365 nm for the bituminous coal combusted in the traditional stove was the highest among all the tested scenarios, which revealed that the incomplete combustion of bituminous coal could emit more BrC. It was noted that primary BrC emitted from the coal combustion with traditional stoves contains higher aromaticity groups of C–C and C＝O and higher S containing organics, whereas more aliphatic groups were found in BrC using the improved stoves. N-containing (CHON and CHONS) compounds were dominated in the total molecular formula of BrC, whereas the sum of CHON and CHO groups had high double-bond equivalent (DBE) values contributed 53.5%–87.1% to the total BrC absorption. Moreover, for CHOS, the lowest of estimated molecular absorption, DBE, and DBE/C should attribute to the non-chromophoric or weak absorptive S-containing compounds. This study supplied an effective evaluation method to compare BrC emissions and their absorption for coal combustion on regional scale.

Observationally constrained representation of brown carbon emissions from wildfires in a chemical transport model

Representing brown carbon absorption, photobleaching, and secondary organic aerosol formation in wildfire emissions results in improved agreement between WRF-Chem simulations and AERONET observations.

Concentration, optical characteristics, and emission factors of brown carbon emitted by on-road vehicles

Atmospheric brown carbon (BrC) is a light-absorbing component that affects radiative forcing; however, this effect requires further clarification, particularly with respect to BrC emission sources, chromophores, and optical properties. In the present study, the concentrations, optical properties, and emission factors of organic carbon (OC), water-soluble OC (WSOC), and humic-like substances (HULIS) in fine particulate matter (PM2.5) emitted from vehicles in three road tunnels (the Wucun, Xianyue, and Wenxing tunnels in Xiamen, China) were investigated. The mass concentrations and light absorption of OC, WSOC, and HULIS were higher at the exits of each tunnel than at entrances, demonstrating that vehicle emissions were a BrC source. At each tunnel's exit, the average light absorption contributed by HULIS-BrC to water-soluble BrC (WS-BrC) and total BrC at 365 nm was higher than the corresponding carbon mass concentration contributed by HULIS (HULIS-C) to WSOC and OC, indicating that the chromophores of HULIS emitted from vehicles had a disproportionately high effect on the light absorption characteristics of BrC. The emission factors (EFs) of HULIS-C and WSOC mass concentrations were highest at the Xianyue tunnel; however, the EFs of HULIS-BrC and WS-BrC light absorption were highest at the Wenxing tunnel, indicating that the chromophore composition of BrC was different among the tunnels and that the mass concentration EFs did not correspond directly to the light absorption EFs.

Modeling Investigation of Brown Carbon Aerosol and Its Light Absorption in China

Brown carbon (BrC) is a type of organic carbon with light-absorbing abilities, especially in ultraviolet (UV) radiation, which could significantly contribute to global warming. Observations have shown high BrC concentrations and absorption in China, suggesting potentially large BrC emissions. The potential contribution of fossil fuel combustion to BrC emission has been ignored in most previous studies. Here, we use GEOS-Chem to simulate BrC distribution and absorption in China, accounting for three major primary BrC sources: residential coal and biofuel combustion, vehicle exhausts, and open biomass burning. Based on the literature and related energy consumption data, we estimate the specific emission ratio of BrC versus BC, and BrC mass absorption efficiency (MAE) for each source. Combined with BC emission, total BrC emission in China is then estimated to be 3.42 Tg yr−1 in 2018, of which 71% is from residential combustion, 14% is from vehicle exhaust, and 15% is from open biomass burning. Residential combustion is the main source of surface BrC in China, accounting for 60% on average, followed by open biomass burning (23%) and vehicle exhaust emissions (17%). There is a clear seasonality in surface BrC concentrations with the maximum in winter (5.1 µg m−3), followed by spring (2.8 µg m−3), autumn (2.3 µg m−3), and summer (1.3 µg m−3). BrC AAOD at 365 nm ranges from 0.0017 to 0.060 in China, mainly dominated by residential combustion (73%), followed by open biomass burning (16%), and vehicle exhaust emissions (11%). It is also estimated that BrC accounts for 45–67% (52% on average) of total carbonaceous aerosol AAOD at 365 nm, implying an equal importance of BrC and BC regarding the absorption in UV radiation.

Brownness of Organic Aerosol over the United States: Evidence for Seasonal Biomass Burning and Photobleaching Effects.

Light-absorptivity of organic aerosol may play an important role in visibility and climate forcing, but it has not been assessed as extensively as black carbon (BC) aerosol. Based on multiwavelength thermal/optical analysis and spectral mass balance, this study quantifies BC for the U.S. Interagency Monitoring of Protected Visual Environments (IMPROVE) network while developing a brownness index (γBr) for non-BC organic carbon (OC*) to illustrate the spatiotemporal trends of light-absorbing brown carbon (BrC) content. OC* light absorption efficiencies range from 0 to 3.1 m2 gC-1 at 405 nm, corresponding to the lowest and highest BrC content of 0 and 100%, respectively. BC, OC*, and γBr explain >97% of the variability of measured spectral light absorption (405-980 nm) across 158 IMPROVE sites. Network-average OC* light absorptions at 405 nm are 50 and 28% those for BC over rural and urban areas, respectively. Larger organic fractions of light absorption occur in winter, partially due to higher organic brownness. Winter γBr exhibits a dramatic regional/urban-rural contrast consistent with anthropogenic BrC emissions from residential wood combustion. The spatial differences diminish to uniformly low γBr in summer, suggesting effective BrC photobleaching over the midlatitudes. An empirical relationship between BC, ambient temperature, and γBr is established, which can facilitate the incorporation of organic aerosol absorptivity into climate and visibility models that currently assume either zero or static organic light absorption efficiencies.

Seasonal features of brown carbon in northern China: Implications for BrC emission control

As brown carbon (BrC) consists of a collection of light-absorbing organic compounds, there is unlikely an individual substance that can be used as a proxy of all BrC constituents. Hence, available methods for distinguishing BrC from black carbon (BC) are often flawed. Moreover, the use of household solid fuels for winter rural heating is a common practice in northern China that significantly contributes to air pollution; however, it is unclear whether the intensive consumption of solid fuels during the heating season influences the yearly BrC emissions and the seasonal features of ambient BrC in northern China, which is a concern for future BrC control. Thus, a reliable method is necessary for determining the concentrations and optical properties of ambient BrC in different seasons. In this study, four typical months were selected to represent the four seasons of the year in Beijing. Daily atmospheric samples were collected using quartz filters for the analysis of BrC and BC. The integrating sphere (IS) approach was used for the first time to separate the light absorption of BrC from that of BC in ambient PM2.5. We found that the yearly average abundance of BrC was 0.82 ± 0.44 μg m−3, peaking at 2.31 ± 0.44 μg m−3 in winter, followed by autumn, spring, and summer. Meanwhile, the solar energy absorption by BrC relative to that by BrC + BC across 350–850 nm (FBrC) was the highest in winter (21.78 ± 3.56%), followed by autumn (11.53 ± 5.29%), spring (6.38 ± 4.06%), and summer (4.26 ± 2.57%). The seasonal variations in BrC abundance and absorption share were consistent with the use of household heating practices (highest in winter and minor uses in late autumn and early spring), with biomass and/or coal being the dominant energy types. As low-efficiency burning of solid biomass fuels and fossil fuels is considered an important source of BrC, the aforementioned correlation suggests that rural residential heating plays a dominant role in controlling the seasonal features of BrC and should therefore be a main focus for BrC control in northern China. Hence, the ongoing pursuit of clean heating (switching from coal to gas or electricity) in northern China will help to mitigate the climate-warming effects of both BrC and BC and offset some of the adverse impacts of clean air efforts on climate. Our findings also have wider implications for pollution mitigation in other global regions that use solid fuels.

Brown carbon's emission factors and optical characteristics in household biomass burning: developing a novel algorithm for estimating the contribution of brown carbon

Abstract. Recent studies have highlighted the importance of brown carbon (BrC) in various fields, particularly relating to climate change. The incomplete combustion of biomass in open and contained burning conditions is believed to be a significant contributor to primary BrC emissions. So far, few studies have reported the emission factors of BrC from biomass burning, and few studies have specifically addressed which form of light-absorbing carbon, such as black carbon (BC) or BrC, plays a leading role in the total solar light absorption by biomass burning. In this study, the optical integrating sphere (IS) approach was used, with carbon black and humic acid sodium salt as reference materials for BC and BrC, respectively, to distinguish BrC from BC on filter samples. A total of 11 widely used biomass types in China were burned in a typical stove to simulate the real household combustion process. (i) Large differences existed in the emission factors of BrC (EFBrC) among the tested biomass fuels, with a geometric mean EFBrC of 0.71 g kg−1 (0.24–2.09). Both the plant type (herbaceous or ligneous) and burning style (raw or briquetted biomass) might influence the value of EFBrC. The observed reduction in the emissions of light-absorbing carbon (LAC) confirmed an additional benefit of biomass briquetting in climate change mitigation. (ii) The calculated annual BrC emissions from China's household biomass burning amounted to 712 Gg, higher than the contribution from China's household coal combustion (592 Gg). (iii) The average absorption Ångström exponent (AAE) was (2.46±0.53), much higher than that of coal-chunk combustion smoke (AAE=1.30±0.32). (iv) For biomass smoke, the contribution of absorption by BrC to the total absorption by BC+BrC across the strongest solar spectral range of 350–850 nm (FBrC) was 50.8 %. This is nearly twice that for BrC in smoke from household coal combustion (26.5 %). (v) Based on this study, a novel algorithm was developed for estimating the FBrC for perhaps any combustion source (FBrC=0.5519ln⁡AAE+0.0067, R2=0.999); the FBrC value for all global biomass burning (open+contained) (FBrC-entire) was 64.5 % (58.5 %–69.9 %). This corroborates the dominant role of BrC in total biomass burning absorption. Therefore, the inclusion of BrC is not optional but indispensable when considering the climate energy budget, particularly for biomass burning emissions (contained and open).