Inter-comparison of source apportionment models for the estimation of wood burning aerosols during wintertime in an Alpine city (Grenoble, France)

Abstract. The emission of organic aerosols (OA) in the ambient air by residential wood burning is nowadays a subject of great scientific concern and a growing number of studies aim at apportioning the influence of such emissions on urban air quality. In the present study, results obtained using two commonly-used source apportionment models, i.e., Chemical Mass Balance (CMB, performed with off-line filter measurements) and Positive Matrix Factorization (PMF, applied to Aerosol Mass Spectrometer measurements), as well as using the recently-proposed Aethalometer model (based on the measurement of the aerosol light absorption at different wavelengths) are inter-compared. This work is performed using field data obtained during the winter season (14 to 29 January 2009) at an urban background site of a French Alpine city (Grenoble). Converging results from the different models indicate a major contribution of wood burning organic aerosols (OMwb) to the ambient aerosol organic fraction, with mean OMwb contributions to total OA of 68%, 61% and 37% for the CMB, the Aethalometer and the AMS-PMF models respectively, during the period when the three modelling studies overlapped (12 days). Quantitative discrepancies might notably be due to the overestimation of OMwb calculated by the CMB due to the loss of semi-volatile compounds from sources to receptor site, as well as to the accounting of oxidized primary wood burning organic (OPOAwb) aerosols within the Oxygenated Organic Aerosol (OOA) PMF-factor. This OOA factor accounts on average for about 50% of total OM, while non-combustion sources contribute to about 25% and 28% of total OM according to the CMB and Aethalometer models respectively. Each model suggests a mean contribution of fossil fuel emissions to total OM of about 10%. A good agreement is also obtained for the source apportionment of elemental carbon (EC) by both the CMB and the Aethalometer models, with fossil fuel emissions representing on average more than 80% of total EC.

Download Full-text

Inter-comparison of source apportionment models for the estimation of wood burning aerosols during wintertime in an Alpine city (Grenoble, France)

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-10-559-2010 ◽

2010 ◽

Vol 10 (1) ◽

pp. 559-613 ◽

Cited By ~ 6

Author(s):

O. Favez ◽

I. El Haddad ◽

C. Piot ◽

A. Boréave ◽

E. Abidi ◽

...

Keyword(s):

Source Apportionment ◽

Fossil Fuel ◽

Winter Season ◽

Organic Aerosols ◽

Receptor Site ◽

Ambient Air ◽

Aerosol Mass ◽

Wood Burning ◽

Study Results ◽

Fossil Fuel Emissions

Abstract. The emission of organic aerosols (OA) in the ambient air by residential wood burning is nowadays a subject of great scientific concern and a growing number of studies aim at apportioning the influence of such emissions on urban air quality. In the present study, results obtained using two commonly-used source apportionment models, i.e., Chemical Mass Balance (CMB, performed with off-line filter measurements) and Positive Matrix Factorization (PMF, applied to aerosol mass spectrometer measurements), as well as using the recently-proposed aethalometer model (based on the measurement of the aerosol light absorption at different wavelengths) are inter-compared. This work is performed using field data obtained during the winter season (14 to 30 January 2009) at an urban background site of a French Alpine city (Grenoble). Converging results from the different models indicate a major contribution of wood burning organic aerosols (OMwb) to the organic fraction, with mean OMwb contributions to total OA of about 67%, 60% and 38% for the CMB, the aethalometer and the AMS-PMF models, respectively. Quantitative discrepancies might notably be due to the overestimation of OMwb calculated by the CMB due to the loss of semi-volatile compounds from sources to receptor site, as well as to the accounting of oxidized primary wood burning organic (OPOAwb) aerosols within the Oxygenated Organic Aerosol (OOA) PMF-factor. This OOA factor accounts on average for about 50% of total OM, while non-combustion sources contribute to about 25% and 28% of total OM according to the CMB and aethalometer models, respectively. Each model suggests a mean contribution of fossil fuel emissions to total OM of about 10%. A good agreement is also obtained for the source apportionment of elemental carbon (EC) by both the CMB and aethalometer models, with fossil fuel emissions representing on average more than 80% of total EC.

Download Full-text

Sources of organic aerosols in Europe: a modeling study using CAMx with modified volatility basis set scheme

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-15247-2019 ◽

2019 ◽

Vol 19 (24) ◽

pp. 15247-15270 ◽

Cited By ~ 3

Author(s):

Jianhui Jiang ◽

Sebnem Aksoyoglu ◽

Imad El-Haddad ◽

Giancarlo Ciarelli ◽

Hugo A. C. Denier van der Gon ◽

...

Keyword(s):

Air Quality ◽

Source Apportionment ◽

Biomass Burning ◽

Agricultural Waste ◽

Organic Aerosols ◽

Basis Set ◽

Anthropogenic Sources ◽

Wood Burning ◽

Gasoline Vehicles

Abstract. Source apportionment of organic aerosols (OAs) is of great importance to better understand the health impact and climate effects of particulate matter air pollution. Air quality models are used as potential tools to identify OA components and sources at high spatial and temporal resolution; however, they generally underestimate OA concentrations, and comparisons of their outputs with an extended set of measurements are still rare due to the lack of long-term experimental data. In this study, we addressed such challenges at the European level. Using the regional Comprehensive Air Quality Model with Extensions (CAMx) and a volatility basis set (VBS) scheme which was optimized based on recent chamber experiments with wood burning and diesel vehicle emissions, and which contains more source-specific sets compared to previous studies, we calculated the contribution of OA components and defined their sources over a whole-year period (2011). We modeled separately the primary and secondary OA contributions from old and new diesel and gasoline vehicles, biomass burning (mostly residential wood burning and agricultural waste burning excluding wildfires), other anthropogenic sources (mainly shipping, industry and energy production) and biogenic sources. An important feature of this study is that we evaluated the model results with measurements over a longer period than in previous studies, which strengthens our confidence in our modeled source apportionment results. Comparison against positive matrix factorization (PMF) analyses of aerosol mass spectrometric measurements at nine European sites suggested that the modified VBS scheme improved the model performance for total OA as well as the OA components, including hydrocarbon-like (HOA), biomass burning (BBOA) and oxygenated components (OOA). By using the modified VBS scheme, the mean bias of OOA was reduced from −1.3 to −0.4 µg m−3 corresponding to a reduction of mean fractional bias from −45 % to −20 %. The winter OOA simulation, which was largely underestimated in previous studies, was improved by 29 % to 42 % among the evaluated sites compared to the default parameterization. Wood burning was the dominant OA source in winter (61 %), while biogenic emissions contributed ∼ 55 % to OA during summer in Europe on average. In both seasons, other anthropogenic sources comprised the second largest component (9 % in winter and 19 % in summer as domain average), while the average contributions of diesel and gasoline vehicles were rather small (∼ 5 %) except for the metropolitan areas where the highest contribution reached 31 %. The results indicate the need to improve the emission inventory to include currently missing and highly uncertain local emissions, as well as further improvement of VBS parameterization for winter biomass burning. Although this study focused on Europe, it can be applied in any other part of the globe. This study highlights the ability of long-term measurements and source apportionment modeling to validate and improve emission inventories, and identify sources not yet properly included in existing inventories.

Download Full-text

Exploiting multi-wavelength aerosol absorption coefficients in a multi-time resolution source apportionment study to retrieve source-dependent absorption parameters

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-11235-2019 ◽

2019 ◽

Vol 19 (17) ◽

pp. 11235-11252 ◽

Cited By ~ 3

Author(s):

Alice Corina Forello ◽

Vera Bernardoni ◽

Giulia Calzolai ◽

Franco Lucarelli ◽

Dario Massabò ◽

...

Keyword(s):

Source Apportionment ◽

Biomass Burning ◽

Time Resolution ◽

Fossil Fuel ◽

Traditional Approach ◽

Optical Data ◽

Optical Parameters ◽

Bootstrap Analysis ◽

Aerosol Absorption ◽

Fossil Fuel Emissions

Abstract. In this paper, a new methodology coupling aerosol optical and chemical parameters in the same source apportionment study is reported. In addition to results on source contributions, this approach provides information such as estimates for the atmospheric absorption Ångström exponent (α) of the sources and mass absorption cross sections (MACs) for fossil fuel emissions at different wavelengths. A multi-time resolution source apportionment study using the Multilinear Engine (ME-2) was performed on a PM10 dataset with different time resolutions (24, 12, and 1 h) collected during two different seasons in Milan (Italy) in 2016. Samples were optically analysed by an in-house polar photometer to retrieve the aerosol absorption coefficient bap (in Mm−1) at four wavelengths (λ=405, 532, 635, and 780 nm) and were chemically characterized for elements, ions, levoglucosan, and carbonaceous components. The dataset joining chemically speciated and optical data was the input for the multi-time resolution receptor model; this approach was proven to strengthen the identification of sources, thus being particularly useful when important chemical markers (e.g. levoglucosan, elemental carbon) are not available. The final solution consisted of eight factors (nitrate, sulfate, resuspended dust, biomass burning, construction works, traffic, industry, aged sea salt); the implemented constraints led to a better physical description of factors and the bootstrap analysis supported the goodness of the solution. As for bap apportionment, consistent with what was expected, biomass burning and traffic were the main contributors to aerosol absorption in the atmosphere. A relevant feature of the approach proposed in this work is the possibility of retrieving a lot of other information about optical parameters; for example, in contrast to the more traditional approach used by optical source apportionment models, here we obtained source-dependent α values without any a priori assumption (α biomass burning =1.83 and α fossil fuels =0.80). In addition, the MACs estimated for fossil fuel emissions were consistent with literature values. It is worth noting that the approach presented here can also be applied using more common receptor models (e.g. EPA PMF instead of multi-time resolution ME-2) if the dataset comprises variables with the same time resolution as well as optical data retrieved by widespread instrumentation (e.g. an Aethalometer instead of in-house instrumentation).

Download Full-text

Introduction and Application of the PMF Model to Estimate the Source Apportionment of PM2.5 at Various Sites

Journal of the Institute of Engineering ◽

10.3126/jie.v8i3.5928 ◽

1970 ◽

Vol 8 (3) ◽

pp. 25-31 ◽

Cited By ~ 1

Author(s):

Injo Hwang

Keyword(s):

Air Quality ◽

Source Apportionment ◽

Receptor Site ◽

Ambient Air ◽

Receptor Modeling ◽

Ambient Air Quality ◽

Receptor Models ◽

Pmf Model ◽

Source Contributions ◽

Reduction Strategies

To manage ambient air quality and establish effective emissions reduction strategies, it is necessary to identify sources and to apportion the ambient PM mass. To do so, receptor models have been developed that analyze various measured properties of the pollutants at the receptor site, identify the sources, and estimate their contributions. Receptor modeling is based on a mathematical model that analyzes the physicochemical properties of gaseous and/or particulate pollutants at various atmospheric receptors. Among the multivariate receptor models used for PM source identification and apportionment, positive matrix factorization (PMF) has been developed by Paatero in 1997. PMF have been developed for providing a new approach to multivariate receptor modeling based on explicit least-squares technique. Also, PMF shown to be a powerful technique relative to traditional multivariate receptor models. PMF has been implemented in two different algorithms: PMF2 (or PMF3) and the multilinear engine (ME). Since the release of PMF2 and ME, these programs have been successfully applied to assess ambient PM source contributions at many locations in the world. In this study, I would like to introduce about outline of the PMF model and application of the PMF model to estimate the source apportionment of ambient PM2.5 at various sampling sites in USA and Korea. This study suggests the possible role for maintain and manage ambient air quality and achieve reasonable air pollution strategies. DOI: http://dx.doi.org/10.3126/jie.v8i3.5928 JIE 2011; 8(3): 25-31

Download Full-text

Assessment of Ambient Air Toxics and Wood Smoke Pollution among Communities in Sacramento County

International Journal of Environmental Research and Public Health ◽

10.3390/ijerph17031080 ◽

2020 ◽

Vol 17 (3) ◽

pp. 1080 ◽

Cited By ~ 1

Author(s):

Steven G. Brown ◽

Janice Lam Snyder ◽

Michael C. McCarthy ◽

Nathan R. Pavlovic ◽

Stephen D’Andrea ◽

...

Keyword(s):

Survey Data ◽

Fossil Fuel ◽

Ambient Air ◽

Wood Smoke ◽

Air Toxics ◽

Wood Burning ◽

Sacramento County ◽

Phone Survey ◽

Significant Difference ◽

Smoke Pollution

Ambient air monitoring and phone survey data were collected in three environmental justice (EJ) and three non-EJ communities in Sacramento County during winter 2016–2017 to understand the differences in air toxics and in wood smoke pollution among communities. Concentrations of six hazardous air pollutants (HAPs) and black carbon (BC) from fossil fuel (BCff) were significantly higher at EJ communities versus non-EJ communities. BC from wood burning (BCwb) was significantly higher at non-EJ communities. Correlation analysis indicated that the six HAPs were predominantly from fossil fuel combustion sources, not from wood burning. The HAPs were moderately variable across sites (coefficient of divergence (COD) range of 0.07 for carbon tetrachloride to 0.28 for m- and p-xylenes), while BCff and BCwb were highly variable (COD values of 0.46 and 0.50). The BCwb was well correlated with levoglucosan (R2 of 0.68 to 0.95), indicating that BCwb was a robust indicator for wood burning. At the two permanent monitoring sites, wood burning comprised 29–39% of the fine particulate matter (PM2.5) on nights when PM2.5 concentrations were forecasted to be high. Phone survey data were consistent with study measurements; the only significant difference in the survey results among communities were that non-EJ residents burn with indoor devices more often than EJ residents.

Download Full-text

Exploiting multi-wavelength aerosol absorption coefficients in a multi-time source apportionment study to retrieve source-dependent absorption parameters

10.5194/acp-2019-123 ◽

2019 ◽

Author(s):

Alice C. Forello ◽

Vera Bernardoni ◽

Giulia Calzolai ◽

Franco Lucarelli ◽

Dario Massabò ◽

...

Keyword(s):

Absorption Coefficient ◽

Source Apportionment ◽

Biomass Burning ◽

Fossil Fuel ◽

Optical Parameters ◽

Bootstrap Analysis ◽

Mass Absorption ◽

Aerosol Absorption ◽

Multi Wavelength ◽

Fossil Fuel Emissions

Abstract. In this paper, a new methodology coupling aerosol optical and chemical parameters in the same source apportionment study is reported. This approach gives additional relevant information such as estimates for the atmospheric Ångström Absorption Exponent (α) of the sources and Mass Absorption Coefficient (MAC) for fossil fuel emissions at different wavelengths. A multi-time source apportionment study using Multilinear Engine ME-2 was performed on a PM10 dataset with different time resolution (24 hours, 12 hours, and 1 hour) collected during two different seasons in Milan (Italy) in 2016. Samples were optically analysed to retrieve the aerosol absorption coefficient bap (in Mm−1) at four wavelengths (λ = 405 nm, 532 nm, 635 nm and 780 nm) and chemically characterised for elements, ions, levoglucosan, and carbonaceous components. Time-resolved chemically speciated data were coupled with bap multi-wavelength measurements and introduced as input data in the multi-time receptor model; this approach was proven to strengthen the identification of sources being particularly useful when important chemical markers (e.g. levoglucosan, elemental carbon, ...) are not available. The final solution consisted in 8 factors (nitrate, sulphate, resuspended dust, biomass burning, construction works, traffic, industry, aged sea salt); the implemented constraints led to a better physical description of factors and the bootstrap analysis supported the goodness of the solution. As for bap apportionment, consistently to what expected, the two factors assigned to biomass burning and traffic were the main contributors to aerosol absorption in atmosphere. A relevant feature of the approach proposed in this work is the possibility of retrieving many other information about optical parameters; for example, opposite to the more traditional approach used by optical source apportionment models, here we obtained the atmospheric Ångström Absorption Exponent (α) of the sources (α biomass burning = 1.83 and α fossil fuels = 0.80), without any a priori assumption. In addition, an estimate for the Mass Absorption Cross section (MAC) for fossil fuel emissions at four wavelengths was obtained and found to be consistent with literature ranges.

Download Full-text

A 2.5 year's source apportionment study of black carbon from wood burning and fossil fuel combustion at urban and rural sites in Switzerland

Atmospheric Measurement Techniques ◽

10.5194/amt-4-1409-2011 ◽

2011 ◽

Vol 4 (7) ◽

pp. 1409-1420 ◽

Cited By ~ 110

Author(s):

H. Herich ◽

C. Hueglin ◽

B. Buchmann

Keyword(s):

Black Carbon ◽

Source Apportionment ◽

Cross Sections ◽

Light Absorption ◽

Fossil Fuel ◽

Data Sets ◽

Near Ultraviolet ◽

Wood Burning ◽

Multi Wavelength ◽

Rural Sites

Abstract. The contributions of fossil fuel (FF) and wood burning (WB) emissions to black carbon (BC) have been investigated in the recent past by analysis of multi-wavelength aethalometer data. This approach utilizes the stronger light absorption of WB aerosols in the near ultraviolet compared to the light absorption of aerosols from FF combustion. Here we present 2.5 years of seven-wavelength aethalometer data from one urban and two rural background sites in Switzerland measured from 2008–2010. The contribution of WB and FF to BC was directly determined from the aerosol absorption coefficients of FF and WB aerosols which were calculated by using confirmed Ångstrom exponents and aerosol light absorption cross-sections that were determined for all sites. Reasonable separation of total BC into contributions from FF and WB was achieved for all sites and seasons. The obtained WB contributions to BC are well correlated with measured concentrations of levoglucosan and potassium while FF contributions to BC correlate nicely with NOx. These findings support our approach and show that the applied source apportionment of BC is well applicable for long-term data sets. During winter, we found that BC from WB contributes on average 24–33 % to total BC at the considered measurement sites. This is a noticeable high fraction as the contribution of wood burning to the total final energy consumption is in Switzerland less than 4 %.

Download Full-text

A method to dynamically constrain black carbon aerosol sources with online monitored potassium

npj Climate and Atmospheric Science ◽

10.1038/s41612-021-00200-y ◽

2021 ◽

Vol 4 (1) ◽

Author(s):

Huang Zheng ◽

Shaofei Kong ◽

Nan Chen ◽

Zewei Fan ◽

Ying Zhang ◽

...

Keyword(s):

Black Carbon ◽

Source Identification ◽

Fossil Fuel ◽

Pearson Correlation ◽

Pearson Correlation Coefficient ◽

Fossil Fuel Combustion ◽

Wood Burning ◽

Study Results ◽

Black Carbon Aerosol ◽

Aerosol Sources

AbstractThe result of Aethalometer model to black carbon (BC) source apportionment is highly determined by the absorption Ångström exponent (α) of aerosols from fossil fuel combustion (αff) and wood burning (αwb). A method using hourly measured potassium to calculate the αff and αwb values was developed in this study. Results showed that the optimal αff and αwb were 1.09 and 1.79 for the whole dataset. The optimal α values in the diurnal resolution were also calculated with αff and αwb varied in 1.02 –1.19 and 1.71–1.90, respectively. Using the dynamic α values, the Pearson correlation coefficient between BC and potassium from wood burning substantially improved compared to the results derived from the fixed α values. The method developed in this study is expected to provide more reasonable BC source identification results, which are helpful for air quality, climate, and human health modeling studies.

Download Full-text

Spatial and Temporal Variations in PM10 Concentrations between 2010–2017 in South Africa

International Journal of Environmental Research and Public Health ◽

10.3390/ijerph182413348 ◽

2021 ◽

Vol 18 (24) ◽

pp. 13348

Author(s):

Oluwaseyi Olalekan Arowosegbe ◽

Martin Röösli ◽

Temitope Christina Adebayo-Ojo ◽

Mohammed Aqiel Dalvie ◽

Kees de Hoogh

Keyword(s):

South Africa ◽

Winter Season ◽

Ambient Air ◽

Air Pollutant ◽

Pm10 Concentration ◽

World Health ◽

Spatial And Temporal Variation ◽

Western Cape ◽

Study Results ◽

Kwazulu Natal

Particulate matter less than or equal to 10 μm in aerodynamic diameter (PM10 µg/m3) is a priority air pollutant and one of the most widely monitored ambient air pollutants in South Africa. This study analyzed PM10 from monitoring 44 sites across four provinces of South Africa (Gauteng, Mpumalanga, Western Cape and KwaZulu-Natal) and aimed to present spatial and temporal variation in the PM10 concentration across the provinces. In addition, potential influencing factors of PM10 variations around the three site categories (Residential, Industrial and Traffic) were explored. The spatial trend in daily PM10 concentration variation shows PM10 concentration can be 5.7 times higher than the revised 2021 World Health Organization annual PM10 air quality guideline of 15 µg/m3 in Gauteng province during the winter season. Temporally, the highest weekly PM10 concentrations of 51.4 µg/m3, 46.8 µg/m3, 29.1 µg/m3 and 25.1 µg/m3 at Gauteng, Mpumalanga, KwaZulu-Natal and Western Cape Province were recorded during the weekdays. The study results suggest a decrease in the change of annual PM10 levels at sites in Gauteng and Mpumalanga Provinces. An increased change in annual PM10 levels was reported at most sites in Western Cape and KwaZulu-Natal.

Download Full-text

Natural climate solutions for Canada

Science Advances ◽

10.1126/sciadv.abd6034 ◽

2021 ◽

Vol 7 (23) ◽

pp. eabd6034

Author(s):

C. Ronnie Drever ◽

Susan C. Cook-Patton ◽

Fardausi Akhter ◽

Pascal H. Badiou ◽

Gail L. Chmura ◽

...

Keyword(s):

Cover Crops ◽

Fossil Fuel ◽

Paris Agreement ◽

Soil Productivity ◽

Potential Contribution ◽

Mitigation Potential ◽

Natural Systems ◽

Clean Air ◽

Natural Climate ◽

Fossil Fuel Emissions

Alongside the steep reductions needed in fossil fuel emissions, natural climate solutions (NCS) represent readily deployable options that can contribute to Canada’s goals for emission reductions. We estimate the mitigation potential of 24 NCS related to the protection, management, and restoration of natural systems that can also deliver numerous co-benefits, such as enhanced soil productivity, clean air and water, and biodiversity conservation. NCS can provide up to 78.2 (41.0 to 115.1) Tg CO2e/year (95% CI) of mitigation annually in 2030 and 394.4 (173.2 to 612.4) Tg CO2e cumulatively between 2021 and 2030, with 34% available at ≤CAD 50/Mg CO2e. Avoided conversion of grassland, avoided peatland disturbance, cover crops, and improved forest management offer the largest mitigation opportunities. The mitigation identified here represents an important potential contribution to the Paris Agreement, such that NCS combined with existing mitigation plans could help Canada to meet or exceed its climate goals.

Download Full-text