scholarly journals Impacts of Regional-transported Biomass Burning Emissions on Chemical and Optical Properties of Carbonaceous Aerosols in Nanjing, East China

2019 ◽  
Author(s):  
Xiaoyan Liu ◽  
Yan-Lin Zhang ◽  
Yiran Peng ◽  
Lulu Xu ◽  
Chunmao Zhu ◽  
...  

Abstract. Biomass burning can significantly impact the chemical and optical properties of carbonaceous aerosols. Here, the impacts of biomass burning emissions on chemical and optical properties of carbonaceous aerosols were studied during wintertime in a megacity of Nanjing, East China. The high abundance of biomass burning tracers such as levoglucosan (lev), mannosan (man), galactosan (gal) and non-sea-salt potassium (nss-K+) was found during the studied period with the concentration ranges of 22.4–1476 ng m−3, 2.1–56.2 ng m−3, 1.4–32.2 ng m−3, and 0.2–3.8 μg m−3, respectively. Backward air mass origin analysis, potential emission sensitivity of element carbon (EC), and MODIS fire spot information indicated that the elevations of the carbonaceous aerosols were due to the transported biomass-burning aerosols from Southeast China. The characteristic mass ratio maps of lev/man and lev/nss-K+ suggested that the biomass fuels were mainly crop residuals. Furthermore, the strong correlation (p 

2019 ◽  
Vol 19 (17) ◽  
pp. 11213-11233 ◽  
Author(s):  
Xiaoyan Liu ◽  
Yan-Lin Zhang ◽  
Yiran Peng ◽  
Lulu Xu ◽  
Chunmao Zhu ◽  
...  

Abstract. Biomass burning can significantly impact the chemical and optical properties of carbonaceous aerosols. Here, the biomass burning impacts were studied during wintertime in a megacity of Nanjing, eastern China. The high abundance of biomass burning tracers such as levoglucosan (lev), mannosan (man), galactosan (gal) and non-sea-salt potassium (nss-K+) was found during the studied period with the concentration ranges of 22.4–1476 ng m−3, 2.1–56.2 ng m−3, 1.4–32.2 ng m−3 and 0.2–3.8 µg m−3, respectively. The significant contribution of biomass burning to water-soluble organic carbon (WSOC; 22.3±9.9 %) and organic carbon (OC; 20.9±9.3 %) was observed in this study. Backward air mass origin analysis, potential emission sensitivity of elemental carbon (EC) and MODIS fire spot information indicated that the elevations of the carbonaceous aerosols were due to the transported biomass-burning aerosols from southeastern China. The characteristic mass ratio maps of lev∕man and lev∕nss-K+ suggested that the biomass fuels were mainly crop residuals. Furthermore, the strong correlation (p < 0.01) between biomass burning tracers (such as lev) and light absorption coefficient (babs) for water-soluble brown carbon (BrC) revealed that biomass burning emissions played a significant role in the light-absorption properties of carbonaceous aerosols. The solar energy absorption due to water-soluble brown carbon and EC was estimated by a calculation based on measured light-absorbing parameters and a simulation based on a radiative transfer model (RRTMG_SW). The solar energy absorption of water-soluble BrC in short wavelengths (300–400 nm) was 0.8±0.4 (0.2–2.3) W m−2 (figures in parentheses represent the variation range of each parameter) from the calculation and 1.2±0.5 (0.3–1.9) W m−2 from the RRTMG_SW model. The absorption capacity of water-soluble BrC accounted for about 20 %–30 % of the total absorption of EC aerosols. The solar energy absorption of water-soluble BrC due to biomass burning was estimated as 0.2±0.1 (0.0–0.9) W m−2, considering the biomass burning contribution to carbonaceous aerosols. Potential source contribution function model simulations showed that the solar energy absorption induced by water-soluble BrC and EC aerosols was mostly due to the regionally transported carbonaceous aerosols from source regions such as southeastern China. Our results illustrate the importance of the absorbing water-soluble brown carbon aerosols in trapping additional solar energy in the low-level atmosphere, heating the surface and inhibiting the energy from escaping the atmosphere.


2015 ◽  
Vol 15 (9) ◽  
pp. 13607-13656 ◽  
Author(s):  
G. L. Schuster ◽  
O. Dubovik ◽  
A. Arola

Abstract. We describe a method of using the aerosol robotic network (AERONET) size distributions and complex refractive indices to retrieve the relative proportion of carbonaceous aerosols and iron oxide minerals. We assume that soot carbon has a spectrally flat refractive index, and that enhanced imaginary indices at the 440 nm wavelength are caused by brown carbon or hematite. Carbonaceous aerosols can be separated from dust in imaginary refractive index space because 95% of biomass burning aerosols have imaginary indices greater than 0.0042 at the 675–1020 nm wavelengths, and 95% of dust has imaginary refractive indices of less than 0.0042 at those wavelengths. However, mixtures of these two types of particles can not be unambiguously partitioned on the basis of optical properties alone, so we also separate these particles by size. Regional and seasonal results are consistent with expectations. Monthly climatologies of fine mode soot carbon are less than 1.0% by volume for West Africa and the Middle East, but the southern Africa and South America biomass burning sites have peak values of 3.0 and 1.7%. Monthly-averaged fine mode brown carbon volume fractions have a peak value of 5.8% for West Africa, 2.1% for the Middle East, 3.7% for southern Africa, and 5.7% for South America. Monthly climatologies of iron oxide volume fractions show little seasonal variability, and range from about 1.1 to 1.7% for coarse mode aerosols in all four study regions. Finally, our sensitivity study indicates that the soot carbon retrieval is not sensitive to the component refractive indices or densities assumed for carbonaceous and iron oxide aerosols, and differs by only 15.4% when these parameters are altered from our chosen baseline values. The associated soot carbon absorption aerosol optical depth (AAOD) does not vary at all when these parameters are altered, however, because the retrieval is constrained by the AERONET optical properties.


2003 ◽  
Vol 3 (5) ◽  
pp. 1743-1757 ◽  
Author(s):  
J. Sciare ◽  
H. Cachier ◽  
K. Oikonomou ◽  
P. Ausset ◽  
R. Sarda-Estève ◽  
...  

Abstract. During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T>550ºC) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) mass concentrations were on average respectively 1.19±0.56 and 3.62±1.08 mgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 mgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope=1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33±22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these two methods for determining BC brings here new insights on the origin of carbonaceous aerosols in a complex mixture of different sources. It brings also to our attention that important deviations in BC levels are observed using three widely used EGA's techniques and most probably none of the EGA tested here are well adapted to fully characterize this aerosol mixture. Spherical, smooth and silico-aluminated fly-ash observed by an Analytical Scanning Electron Microscope (ASEM) confirm the influence of coal combustion on the carbonaceous aerosol load throughout the campaign. A rough calculation based on a BC/nss-SO4 mass ratio suggests that biomass burning could be responsible for half of the BC concentration recorded during the MINOS campaign. From the plot of BC as a function of TC, two linear correlations were observed corresponding to 2 times series (before and after 12 August). Such good correlations suggest, from a first look, that both BC and OC have similar origin and atmospheric transport. On the other hand, the plot of BC as a function of TC obtained from the 2-step thermal method applied to DEKATI Low Pressure Cascade Impactor samples does not show a similar correlation and points out a non conservative distribution of this ratio with 2 super micron modes enriched in OC, correlated with sea salt aerosols and probably originating from gas-to-particle conversion.


2020 ◽  
Vol 20 (24) ◽  
pp. 15537-15549
Author(s):  
Qiyuan Wang ◽  
Huikun Liu ◽  
Ping Wang ◽  
Wenting Dai ◽  
Ting Zhang ◽  
...  

Abstract. Source-specific optical properties of light-absorbing carbonaceous (LAC) aerosols in the atmosphere are poorly understood because they are generated by various sources. In this study, a receptor model combining multi-wavelength absorption and chemical species was used to explore the source-specific optical properties of LAC aerosols in a tropical marine monsoon climate zone. The results showed that biomass burning and ship emissions were the dominant contributors to average aerosol light absorption. The source-specific absorption Ångström exponent (AAE) indicated that black carbon (BC) was the dominant LAC aerosol in ship and motor vehicle emissions. Moreover, brown carbon (BrC) was present in biomass-burning emissions. The source-specific mass absorption cross section (MAC) showed that BC from ship emissions had a stronger light-absorbing capacity compared to emissions from biomass burning and motor vehicles. The BrC MAC derived from biomass burning was also smaller than the BC MAC and was highly dependent on wavelength. Furthermore, radiative effect assessment indicated a comparable atmospheric forcing and heating capacity of LAC aerosols between biomass burning and ship emissions. This study provides insights into the optical properties of LAC aerosols from various sources. It also sheds more light on the radiative effects of LAC aerosols generated by ship emissions.


2003 ◽  
Vol 3 (4) ◽  
pp. 3373-3410 ◽  
Author(s):  
J. Sciare ◽  
H. Cachier ◽  
K. Oikonomou ◽  
P. Ausset ◽  
R. Sarda-Estève ◽  
...  

Abstract. During the major part of the Mediterranean Intensive Oxidant Study (MINOS) campaign (summer 2001, Crete Isl.), the Marine Boundary Layer (MBL) air was influenced by long range transport of biomass burning from the northern and western part of the Black Sea. During this campaign, carbonaceous aerosols were collected on quartz filters at a Free Tropospheric (FT) site, and at a MBL site together with size-resolved distribution of aerosols. Three Evolution Gas Analysis (EGA) protocols have been tested in order to better characterize the collected aged biomass burning smoke: A 2-step thermal method (Cachier et al., 1989) and a thermo-optical technique using two different temperature programs. The later temperature programs are those used for IMPROVE (Interagency Monitoring of Protected Visual Environments) and NIOSH 5040 (National Institute of Occupational Safety and Health). Artifacts were observed using the NIOSH temperature program and identified as interactions between carbon and dust deposited on the filter matrix at high temperature (T=550°C) under the pure helium step of the analysis. During the MINOS campaign, Black Carbon (BC) and Organic Carbon (OC) concentrations were on average respectively 1.19±0.56 and 3.62±1.08 μgC/m3 for the IMPROVE temperature program, and 1.09±0.36 and 3.75±1.24 μgC/m3 for the thermal method. Though these values compare well on average and the agreement between the Total Carbon (TC) measurements sample to sample was excellent (slope = 1.00, r2=0.93, n=56), important discrepancies were observed in determining BC concentrations from these two methods (average error of 33&amp;plusmn22%). BC from the IMPROVE temperature program compared well with non-sea-salt potassium (nss-K) pointing out an optical sensitivity to biomass burning. On the other hand, BC from the thermal method showed a better agreement with non-sea-salt sulfate (nss-SO4), considered as a tracer for fossil fuel combustion during the MINOS campaign. The coupling between these two methods for determining BC brings here new insights on the origin of carbonaceous aerosols in a complex mixture of different sources. It brings also to our attention that important deviations in BC levels are observed using three widely used EGA techniques and most probably none of the EGA tested here are well adapted to fully characterize this aerosol mixture. Spherical, smooth and silico-aluminated fly-ash observed by Analytical Scanning Electron Microscope (ASEM) confirm the influence of coal combustion on the carbonaceous aerosol load throughout the campaign. A raw calculation based on BC/nss-SO4 mass ratio suggests that biomass burning could be responsible for half of the BC concentration recorded during the MINOS campaign. From the plot of BC as a function of TC, two linear correlations were observed corresponding to 2 times series (before and after 12 August). Such good correlations suggest, from a first look, that both BC and OC have similar origin and atmospheric transport. On the other hand, the plot of BC as a function of TC obtained from the 2-step thermal method applied to DEKATI Low Pressure Cascade Impactor samples does not show a similar correlation and points out a non conservative distribution of this ratio with 2 super micron modes enriched in OC, correlated with sea salt aerosols and probably originating from gas-to-particle conversion.


2021 ◽  
Vol 11 (4) ◽  
pp. 1434
Author(s):  
Chang Hoon Jung ◽  
Sang Hee Han ◽  
Ji Yi Lee ◽  
Yong Pyo Kim

In this study, the source-based optical properties of polydisperse carbonaceous aerosols were determined from PM2.5 concentrations measured at a Global Atmospheric Watch station in South Korea. The extinction and absorption coefficients of carbonaceous aerosols were calculated using the Mie theory and assuming a lognormal size distribution. Based on the mass concentration from the EPA’s Positive Matrix Factorization (PMF) receptor model, which considers five source identification and apportionment factors (biogenic source, local biomass burning, secondary organic aerosol, transported biomass burning, and mixed sources), the source-based size-resolved mass extinction and absorption efficiencies were estimated for each source using a multilinear regression model. The results show that the source-based optical properties depend on the aerosol size and physicochemical characteristics of the chemical compounds. The long-range transport of biomass burning (LBB) aerosol, which has a mass concentration of 20%, holds a 12.1–23.1% total extinction efficiency—depending on the size and refractive index—in the range of 0.1–0.5 μm in geometric mean diameter and humic-like substances (HULIS) imaginary refractive index of 0.006–0.3. Biogenic sources of aerosols with small diameters have higher mass absorption efficiencies (MAE) than other sources, depending on the size and refractive index.


2018 ◽  
Vol 18 (19) ◽  
pp. 14371-14391 ◽  
Author(s):  
Christina Theodosi ◽  
Maria Tsagkaraki ◽  
Pavlos Zarmpas ◽  
Georgios Grivas ◽  
Eleni Liakakou ◽  
...  

Abstract. In an attempt to take effective action towards mitigating pollution episodes in Athens, precise knowledge of PM2.5 composition and its sources is a prerequisite. Thus, a 2-year chemical composition dataset from aerosol samples collected in an urban background site in central Athens from December 2013 to March 2016 has been obtained and a positive matrix factorization (PMF) was applied in order to identify and apportion fine aerosols to their sources. A total of 850 aerosol samples were collected on a 12 to 24 h basis and analyzed for major ions, trace elements, and organic and elemental carbon, allowing us to further assess the impact of residential heating as a source of air pollution over Athens. The ionic and carbonaceous components were found to constitute the major fraction of the PM2.5 aerosol mass. The annual contribution of the ion mass (IM), particulate organic mass (POM), dust, elemental carbon (EC), and sea salt (SS) was calculated at 31 %, 38 %, 18 %, 8 %, and 3 %, respectively, and exhibited considerable seasonal variation. In winter, the share of IM was estimated down to 23 %, with POM + EC being the dominant component accounting for 52 % of the PM2.5 mass, while in summer, IM (42 %) and carbonaceous aerosols (41 %) contributed almost equally. Results from samples collected on a 12 h basis (day and night) during the three intensive winter campaigns indicated the impact of heating on the levels of a series of compounds. Indeed, PM2.5, EC, POM, NO3-, C2O42-, non sea salt (nss) K+ and selected trace metals including Cd and Pb were increased by up to a factor of 4 in the night compared to the day, highlighting the importance of heating on air quality in Athens. Furthermore, in order to better characterize wintertime aerosol sources and quantify the impact of biomass burning on PM2.5 levels, source apportionment was performed. The data can be interpreted on the basis of six sources, namely biomass burning (31 %), vehicular emissions (19 %), heavy oil combustion (7 %), regional secondary (21 %), marine aerosols (9 %), and dust particles (8 %). Regarding night-to-day patterns their contributions shifted from 19 %, 19 %, 8 %, 31 %, 12 %, and 10 % of the PM2.5 mass during day to 39 %, 19 %, 6 %, 14 %, 7 %, and 7 % during the night, underlining the significance of biomass burning as the main contributor to fine particle levels during nighttime in winter.


2019 ◽  
Author(s):  
Yunjiang Zhang ◽  
Olivier Favez ◽  
Jean-Eudes Petit ◽  
Francesco Canonaco ◽  
Francois Truong ◽  
...  

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly-time resolved year-round characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of Aerosol Chemical Speciation Monitor (ACSM) and multi-wavelength aethalometer from November 2011 to March 2018 at a background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase of LO-OOA concentrations and contributions (50–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely high concentrations and OA contributions (32–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter, and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about 200 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil fuel and biomass burning black carbon components), and no trend for LO-OOA over the 6+-year investigated period.


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