Hourly emission estimation of black carbon and brown carbon absorption from domestic coal burning in China

Author(s):  
Qin Yan ◽  
Shaofei Kong ◽  
Yingying Yan ◽  
Xi Liu ◽  
Shurui Zheng ◽  
...  
2020 ◽  
Author(s):  
Jie Luo ◽  
Yongming Zhang ◽  
Qixing Zhang

Abstract. In this work, we developed a numerical method to investigate the effects of black carbon morphology on the estimation of brown carbon (BrC) absorption using the Absorption Ångström exponent (AAE) method. Pseudo measurements of the total absorption were generated based on several morphologically mixed black carbon (BC) models, then the BrC absorption was inferred based on different AAE methods. By comparing the estimated BrC absorption with True BrC absorption, we found that both AAE = 1 and Mie AAE methods do not provide accurate estimation for the BrC absorption, and the estimated BrC absorption can deviate several times from True BrC absorption. The newly proposed Wavelength Dependent AAE (WDA) method does not necessarily improve the estimations, sometimes it may even provide worse estimations than the AAE = 1 and Mie AAE methods. Fixing the fractal dimension to be 1.8, the deviation between the estimated BrC mass absorption cross-section (MAC) and True BrC MAC can reach approximately 9 m2/g, which is far more than brown carbon MAC itself. Therefore, the estimation of BrC absorption based on the AAE method should carefully consider the morphological effects of BC. Our findings highlight the BC morphological effects on the BrC absorption estimation.


2013 ◽  
Vol 13 (5) ◽  
pp. 2415-2422 ◽  
Author(s):  
D. A. Lack ◽  
R. Bahreini ◽  
J. M. Langridge ◽  
J. B. Gilman ◽  
A. M. Middlebrook

Abstract. Traditional gas and particle phase chemical markers used to identify the presence of biomass burning (BB) emissions were measured for a large forest fire near Boulder, Colorado. Correlation of the organic matter mass spectroscopic m/z 60 with measured particle light absorption properties found no link at 532 nm, and a strong correlation at 404 nm. Non-black carbon absorption at 404 nm was well correlated to the ratio of the mass fractions of particulate organic matter (POM) that was m/z 60 (f60) to m/z 44 (f44). The f60 to f44 ratio did not fully explain the variability in non-BC absorption, due to contributions of brown carbon (BrC) absorption and absorption due to internal mixing of POM with black carbon (BC). The absorption Ångstrom exponent (ÅAbs) showed a good correlation to f60/f44; however the best correlation resulted from the mass absorption efficiency (MAE) of BrC at 404 nm (MAEPOM-404 nm) and f60/f44. This result indicates that the absorption of POM at low visible and UV wavelengths is linked to emissions of organic matter that contribute to the m/z 60 mass fragment, although they do not contribute to 532 nm absorption. m/z 60 is often attributed to levoglucosan and related compounds. The linear relationship between MAEPOM-404 nm and f60/f44 suggests that the strength of BrC absorption for this fire can be predicted by emissions of f60-related organic matter.


2021 ◽  
Vol 14 (4) ◽  
pp. 2113-2126 ◽  
Author(s):  
Jie Luo ◽  
Yongming Zhang ◽  
Qixing Zhang

Abstract. In this work, we developed a numerical method to investigate the effects of black carbon (BC) morphology on the estimation of brown carbon (BrC) absorption using the absorption Ångström exponent (AAE) methods. Pseudo measurements of the total absorption were generated based on several morphologically mixed BC models, then the BrC absorption was inferred based on different BC AAE methods. By investigating the estimated BrC absorption at different parameters, we have demonstrated under what conditions the AAE methods can provide good or bad estimations. As recent studies have shown that both externally and internally mixed BC still exhibits a relatively small fractal dimension value, the AAE = 1 method is still a reasonable method to estimate the BrC absorption as the AAE of fluffy BC does not deviate significantly from 1. However, the deviation between the “true” and the estimated BrC mass absorption cross section (MAC) should also be carefully considered as sometimes the MAC deviation estimated using the AAE = 1 method can reach a value that is comparable to the true BrC MAC for internally mixed particles. The Mie AAE method can just provide relatively reasonable estimations for small particles, and the BrC absorption deviations estimated using the Mie AAE methods are rather substantial for large particles. If the BC core still exhibits a fluffy structure, the deviation between the true and the estimated BrC MAC can reach 4.8 and 5.8 m2/g for large externally and internally mixed particles, respectively. Even for a compact BC core, the BrC MAC deviation estimated using the Mie AAE method can reach approximately 2.8 m2/g when the BC size is large. By comparing the AAE of spherical BC and detailed BC models, we found that the AAE does not deviate significantly from 1 if BC presents a fluffy fractal structure, while it varies considerably with particle size if BC exhibits a spherical structure, and the AAE value of spherical BC can vary from a negative value to approximately 1.4. The precalculated wavelength dependence of AAE (WDA) method does not necessarily improve the estimations. In many cases, the WDA method even provides a worse estimation than the BC AAE =1 and Mie AAE methods. Our results showed that the WDA does not deviate significantly from 0 if the BC core presents a fluffy structure, while the WDA of spherical BC can vary significantly as the particle size changes. The deviation between the true and the estimated BrC MAC using the WDA method can reach approximately 9 m2/g for externally mixed particles, which is far more than BrC MAC itself. As recent studies have shown that BC commonly exhibits a fluffy structure but not a spherical structure, the estimation of BrC absorption based on the AAE method should carefully consider the effects of BC morphologies.


2018 ◽  
Vol 18 (16) ◽  
pp. 12345-12361 ◽  
Author(s):  
Christian M. Zdanowicz ◽  
Bernadette C. Proemse ◽  
Ross Edwards ◽  
Wang Feiteng ◽  
Chad M. Hogan ◽  
...  

Abstract. Black carbon aerosol (BC), which is emitted from natural and anthropogenic sources (e.g., wildfires, coal burning), can contribute to magnify climate warming at high latitudes by darkening snow- and ice-covered surfaces, and subsequently lowering their albedo. Therefore, modeling the atmospheric transport and deposition of BC to the Arctic is important, and historical archives of BC accumulation in polar ice can help to validate such modeling efforts. Here we present a > 250-year ice-core record of refractory BC (rBC) deposition on Devon ice cap, Canada, spanning the years from 1735 to 1992. This is the first such record ever developed from the Canadian Arctic. The estimated mean deposition flux of rBC on Devon ice cap for 1963–1990 is 0.2 mg m−2 a−1, which is at the low end of estimates from Greenland ice cores obtained using the same analytical method ( ∼ 0.1–4 mg m−2 a−1). The Devon ice cap rBC record also differs from the Greenland records in that it shows only a modest increase in rBC deposition during the 20th century. In the Greenland records a pronounced rise in rBC is observed from the 1880s to the 1910s, which is largely attributed to midlatitude coal burning emissions. The deposition of contaminants such as sulfate and lead increased on Devon ice cap in the 20th century but no concomitant rise in rBC is recorded in the ice. Part of the difference with Greenland could be due to local factors such as melt–freeze cycles on Devon ice cap that may limit the detection sensitivity of rBC analyses in melt-impacted core samples, and wind scouring of winter snow at the coring site. Air back-trajectory analyses also suggest that Devon ice cap receives BC from more distant North American and Eurasian sources than Greenland, and aerosol mixing and removal during long-range transport over the Arctic Ocean likely masks some of the specific BC source–receptor relationships. Findings from this study suggest that there could be a large variability in BC aerosol deposition across the Arctic region arising from different transport patterns. This variability needs to be accounted for when estimating the large-scale albedo lowering effect of BC deposition on Arctic snow/ice.


2018 ◽  
Vol 18 (24) ◽  
pp. 17843-17861 ◽  
Author(s):  
Nivedita K. Kumar ◽  
Joel C. Corbin ◽  
Emily A. Bruns ◽  
Dario Massabó ◽  
Jay G. Slowik ◽  
...  

Abstract. We investigate the optical properties of light-absorbing organic carbon (brown carbon) from domestic wood combustion as a function of simulated atmospheric aging. At shorter wavelengths (370–470 nm), light absorption by brown carbon from primary organic aerosol (POA) and secondary organic aerosol (SOA) formed during aging was around 10 % and 20 %, respectively, of the total aerosol absorption (brown carbon plus black carbon). The mass absorption cross section (MAC) determined for black carbon (BC, 13.7 m2 g−1 at 370 nm, with geometric standard deviation GSD =1.1) was consistent with that recommended by Bond et al. (2006). The corresponding MAC of POA (5.5 m2 g−1; GSD =1.2) was higher than that of SOA (2.4 m2 g−1; GSD =1.3) at 370 nm. However, SOA presents a substantial mass fraction, with a measured average SOA ∕ POA mass ratio after aging of ∼5 and therefore contributes significantly to the overall light absorption, highlighting the importance of wood-combustion SOA as a source of atmospheric brown carbon. The wavelength dependence of POA and SOA light absorption between 370 and 660 nm is well described with absorption Ångström exponents of 4.6 and 5.6, respectively. UV-visible absorbance measurements of water and methanol-extracted OA were also performed, showing that the majority of the light-absorbing OA is water insoluble even after aging.


2009 ◽  
Vol 9 (6) ◽  
pp. 2035-2050 ◽  
Author(s):  
M. Yang ◽  
S. G. Howell ◽  
J. Zhuang ◽  
B. J. Huebert

Abstract. Black carbon, brown carbon, and mineral dust are three of the most important light absorbing aerosols. Their optical properties differ greatly and are distinctive functions of the wavelength of light. Most optical instruments that quantify light absorption, however, are unable to distinguish one type of absorbing aerosol from another. It is thus instructive to separate total absorption from these different light absorbers to gain a better understanding of the optical characteristics of each aerosol type. During the EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) campaign near Beijing, we measured light scattering using a nephelometer, and light absorption using an aethalometer and a particulate soot absorption photometer. We also measured the total mass concentrations of carbonaceous (elemental and organic carbon) and inorganic particulates, as well as aerosol number and mass distributions. We were able to identify periods during the campaign that were dominated by dust, biomass burning, fresh (industrial) chimney plumes, other coal burning pollution, and relatively clean (background) air for Northern China. Each of these air masses possessed distinct intensive optical properties, including the single scatter albedo and Ångstrom exponents. Based on the wavelength-dependence and particle size distribution, we apportioned total light absorption to black carbon, brown carbon, and dust; their mass absorption efficiencies at 550 nm were estimated to be 9.5, 0.5 (a lower limit value), and 0.03 m2/g, respectively. While agreeing with the common consensus that black carbon is the most important light absorber in the mid-visible, we demonstrated that brown carbon and dust could also cause significant absorption, especially at shorter wavelengths.


2017 ◽  
Author(s):  
Jianzhong Sun ◽  
Guorui Zhi ◽  
Regina Hitzenberger ◽  
Yingjun Chen ◽  
Chongguo Tian ◽  
...  

Abstract. Brown carbon (BrC) draws increasing attention due to its effects on climate and other fields. In China, household coal burned for heating/cooking purposes releases huge amounts of carbonaceous particles every year; however, BrC emissions have rarely been estimated in a persuasive manner due to the unavailable emission characteristics. Here 7 coals jointly covering geological maturity from low to high were burned in 4 typical stoves at both chunk and briquette styles. The optical integrating sphere (IS) method was applied to measure the emission factors (EFs) of BrC and BC via an iterative process using the different spectral dependence of light absorption for BrC and BC. It is found that (i) the average EFs of BrC for anthracite coal chunks and briquettes are (1.08 ± 0.80) g kg−1 and (1.52 ± 0.16) g kg−1, respectively, and those for bituminous coal chunks and briquettes are (8.59 ± 2.70) g kg−1 and (4.01 ± 2.19) g kg−1, respectively, reflecting a more significant decline of BrC EFs for bituminous coals than for anthracites due to briquetting, (ii) the BrC EF peaks at the middle of coal's geological maturity, displaying a bell shaped curve between EF and volatile matter (Vdaf), (iii) the calculated BrC emissions from China's residential coal burning amounted to 592 Gg (1 Gg = 109 g) in 2013, which is nearly half of China's total BC emissions, (iv) absorption Ångström exponent (AAEs) of all coal briquettes are higher than those of coal chunks, indicating that the measure of coal briquetting increases the BrC / BC emission ratio and thus offsets some of the climate cooling effect of briquetting, and (v) in the scenario of current household coal burning in China, solar light absorption by BrC (350–850 nm in this study) accounts for more than a quarter (0.265) of the total absorption. This implies the significance of BrC to climate modeling.


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