Supplementary material to "Technical Note: A new approach to discriminate different black carbon sources by utilising fullerenes and metals in Positive Matrix Factorisation analysis of High-Resolution Soot Particle Aerosol Mass Spectrometer data"

Abstract. Atmospheric aerosol particles are known to have detrimental effects on human health and climate. Black carbon is an important constituent of atmospheric aerosol particulate matter (PM), emitted from the incomplete combustion process and cause significant effects on the air quality and human health. Source apportionment of BC is very important, to identify the fraction of BC that has an anthropogenic origin and to evaluate the influence of different sources. The High-Resolution Soot Particle Aerosol Mass Spectrometer (HR-SP-AMS) instrument uses a laser vaporizer, which allows the real-time detection and characterization of refractory BC and its internally mixed particles such as metals, coating species and rBC subcomponent in the form of fullerene. In this case study, the soot data was collected by using HR-SP-AMS during Guy Fawkes Night on 5th of November 2014. Positive matrix factorization (PMF) was applied in order to positively discriminate between different wood-burning sources for the first time, in this case, BC from domestic wood-burning and bonfires, which no existing black carbon source apportionment technique is currently able to do. Along with this, the use of the fullerene signals in differentiating between soot sources and the use of metals as a tracer for fireworks has also been investigated, which has not significantly contributed to the BC concentrations. The addition of fullerenes signals and successful application of PMF on SP-AMS data apportioned BC into more than two sources. These bonfire sources are hydrocarbon-like Fullerenes, biomass burning organic aerosol, HULIS (humic-like substance) and non-bonfire sources such as hydrocarbon-like OA and domestic burning. The result of correlation analysis between HR-SP-AMS data with previously published Aethalometer, MAAP and CIMS data provides an effective way of quickly gaining insights in relations between the variables and also provide a quantitative estimate of the source contributions to the BC budget during this period. This research study is an important demonstration of using HR-SP-AMS for the purpose of BC source apportionment.

[1]  M. G. Adam,et al.  Characterization of carbonaceous aerosols in Singapore: insight from black carbon fragments and trace metal ions detected by a soot particle aerosol mass spectrometer , 2020 .

[2]  James D. Lee,et al.  Contrasting physical properties of black carbon in urban Beijing between winter and summer , 2018, Atmospheric Chemistry and Physics.

[3]  J. Allan,et al.  Observations of Isocyanate, Amide, Nitrate, and Nitro Compounds From an Anthropogenic Biomass Burning Event Using a ToF‐CIMS , 2018, Journal of Geophysical Research: Atmospheres.

[4]  C. Liousse,et al.  Highly controlled, reproducible measurements of aerosol emissions from combustion of a common African biofuel source , 2018 .

[5]  A. Prévôt,et al.  Improved source apportionment of organic aerosols in complex urban air pollution using the multilinear engine (ME-2) , 2017 .

[6]  M. Kleeman,et al.  Investigating diesel engines as an atmospheric source of isocyanic acid in urban areas , 2017 .

[7]  J. Allan,et al.  Simultaneous aerosol mass spectrometry and chemical ionisation mass spectrometry measurements during a biomass burning event in the UK: Insights into nitrate chemistry , 2017 .

[8]  C. Liousse,et al.  Highly-controlled, reproducible measurements of aerosol emissions from African biomass combustion , 2017 .

[9]  G. Mcfiggans,et al.  Black-carbon absorption enhancement in the atmosphere determined by particle mixing state , 2017 .

[10]  A. Prévôt,et al.  Organic aerosol source apportionment in London 2013 with ME-2: exploring the solution space with annual and seasonal analysis , 2016 .

[11]  J. K. Zhang,et al.  Characterization of submicron particles during biomass burning and coal combustion periods in Beijing, China. , 2016, The Science of the total environment.

[12]  Qi Zhang,et al.  Observation of Fullerene Soot in Eastern China , 2016 .

[13]  Qingzhu Zhang,et al.  HONO and its potential source particulate nitrite at an urban site in North China during the cold season. , 2015, The Science of the total environment.

[14]  H. Timonen,et al.  Characterization of trace metals on soot aerosol particles with the SP-AMS: detection and quantification , 2015 .

[15]  U. Lohmann,et al.  Peak-fitting and integration imprecision in the Aerodyne aerosol mass spectrometer: effects of mass accuracy on location-constrained fits , 2015 .

[16]  M. Lawrence,et al.  Overview of VOC emissions and chemistry from PTR-TOF-MS measurements during the SusKat-ABC campaign: high acetaldehyde, isoprene and isocyanic acid in wintertime air of the Kathmandu Valley , 2015 .

[17]  J. Murphy,et al.  Solubility and reactivity of HNCO in water: insights into HNCO's fate in the atmosphere , 2015 .

[18]  Edward Charles Fortner,et al.  Investigations of SP-AMS Carbon Ion Distributions as a Function of Refractory Black Carbon Particle Type , 2015 .

[19]  Siwatt Pongpiachan,et al.  Assessing risks to adults and preschool children posed by PM2.5-bound polycyclic aromatic hydrocarbons (PAHs) during a biomass burning episode in Northern Thailand. , 2015, The Science of the total environment.

[20]  S. Moussa,et al.  Comparison of negative-ion proton-transfer with iodide ion chemical ionization mass spectrometry for quantification of isocyanic acid in ambient air , 2014 .

[21]  R. Hillamo,et al.  Evaluation of the performance of a particle concentrator for online instrumentation , 2014 .

[22]  C. O'Dowd,et al.  Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach , 2014 .

[23]  A. Prévôt,et al.  SoFi, an IGOR-based interface for the efficient use of the generalized multilinear engine (ME-2) for the source apportionment: ME-2 application to aerosol mass spectrometer data , 2013 .

[24]  C. Percival,et al.  Airborne hydrogen cyanide measurements using a chemical ionisation mass spectrometer for the plume identification of biomass burning forest fires , 2013 .

[25]  P. DeCarlo,et al.  Primary and secondary organic aerosol origin by combined gas-particle phase source apportionment , 2013 .

[26]  T. Holzer-Popp,et al.  Recommendations for reporting "black carbon" measurements , 2013 .

[27]  Yele Sun,et al.  Aerosol composition, sources and processes during wintertime in Beijing, China , 2013 .

[28]  K. Unfried,et al.  Unhealthy diet and ultrafine carbon black particles induce senescence and disease associated phenotypic changes , 2013, Experimental Gerontology.

[29]  W. B. Knighton,et al.  Particulate Emissions Measured During the TCEQ Comprehensive Flare Emission Study , 2012 .

[30]  Edward Charles Fortner,et al.  Soot Particle Aerosol Mass Spectrometer: Development, Validation, and Initial Application , 2012 .

[31]  Qun Xu,et al.  Fine Particulate Matter Constituents and Cardiopulmonary Mortality in a Heavily Polluted Chinese City , 2012, Environmental health perspectives.

[32]  A. Prévôt,et al.  Light‐absorbing soluble organic aerosol in Los Angeles and Atlanta: A contrast in secondary organic aerosol , 2011 .

[33]  Yaqi Cai,et al.  Effect of fireworks display on perchlorate in air aerosols during the Spring Festival , 2011 .

[34]  P. DeCarlo,et al.  Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments , 2010 .

[35]  D. Koch,et al.  Quantifying immediate radiative forcing by black carbon and organic matter with the Specific Forcing Pulse , 2010 .

[36]  R. Harrison,et al.  Inferences over the sources and processes affecting polycyclic aromatic hydrocarbons in the atmosphere derived from measured data. , 2010, The Science of the total environment.

[37]  A. Zelenyuk,et al.  Comparison of FTIR and particle mass spectrometry for the measurement of particulate organic nitrates. , 2010, Environmental science & technology.

[38]  Xiao-Feng Huang,et al.  Abundance and size distribution of HULIS in ambient aerosols at a rural site in South China , 2009 .

[39]  James D. Lee,et al.  Contributions from transport, solid fuel burning and cooking to primary organic aerosols in two UK cities , 2009 .

[40]  T. Grahame,et al.  Cardiovascular health and particulate vehicular emissions: a critical evaluation of the evidence , 2009, Air quality, atmosphere, & health.

[41]  Edward Charles Fortner,et al.  Mexico City Aerosol Analysis during MILAGRO using High Resolution Aerosol Mass Spectrometry , 2009 .

[42]  Sönke Szidat,et al.  Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter. , 2008, Environmental science & technology.

[43]  J. Jimenez,et al.  Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data , 2008 .

[44]  P. DeCarlo,et al.  Elemental analysis of organic species with electron ionization high-resolution mass spectrometry. , 2007, Analytical chemistry.

[45]  Martin Mohr,et al.  Identification of the mass spectral signature of organic aerosols from wood burning emissions. , 2007, Environmental science & technology.

[46]  Katrin Fuhrer,et al.  Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. , 2006, Analytical chemistry.

[47]  R. Kinnersley,et al.  When smoke gets in our eyes: the multiple impacts of atmospheric black carbon on climate, air quality and health. , 2006, Environment international.

[48]  Hugh Coe,et al.  Simplification of the representation of the organic component of atmospheric particulates. , 2005, Faraday discussions.

[49]  Qi Zhang,et al.  Deconvolution and quantification of hydrocarbon-like and oxygenated organic aerosols based on aerosol mass spectrometry. , 2005, Environmental science & technology.

[50]  M. Fontugne,et al.  Measurement of the carbon 14 activity at natural level in air samples , 2005 .

[51]  S. Martin,et al.  Products and mechanisms of the reaction of oleic acid with ozone and nitrate radical. , 2005, The journal of physical chemistry. A.

[52]  D. Ceburnis,et al.  Advances in characterization of size-resolved organic matter in marine aerosol over the North Atlantic , 2004 .

[53]  J. Jimenez,et al.  A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data , 2004 .

[54]  Charles E. Kolb,et al.  Chase Studies of Particulate Emissions from in-use New York City Vehicles , 2004 .

[55]  G. O. Thomas,et al.  Atmospheric emissions of polybrominated diphenyl ethers and other persistent organic pollutants during a major anthropogenic combustion event. , 2004, Environmental science & technology.

[56]  G. Kiss,et al.  Chemical characterization of humic‐like substances (HULIS) formed from a lignin‐type precursor in model cloud water , 2004 .

[57]  F. J. Cox,et al.  Formation of oligomers in secondary organic aerosol. , 2004, Environmental science & technology.

[58]  Tomas Alsberg,et al.  Estimation of the average molecular weight of humic-like substances isolated from fine atmospheric aerosol , 2003 .

[59]  Philip K. Hopke,et al.  Discarding or downweighting high-noise variables in factor analytic models , 2003 .

[60]  R. Kamens,et al.  Particle growth by acid-catalyzed heterogeneous reactions of organic carbonyls on preexisting aerosols. , 2003, Environmental science & technology.

[61]  M. Kiisk,et al.  Accelerator mass spectrometry: an overview , 2003 .

[62]  M. Facchini,et al.  Water‐soluble organic compounds in biomass burning aerosols over Amazonia 2. Apportionment of the chemical composition and importance of the polyacidic fraction , 2002 .

[63]  M. Facchini,et al.  Water‐soluble organic compounds in biomass burning aerosols over Amazonia 1. Characterization by NMR and GC‐MS , 2002 .

[64]  R. Kamens,et al.  Heterogeneous Atmospheric Aerosol Production by Acid-Catalyzed Particle-Phase Reactions , 2002, Science.

[65]  A. Hoffer,et al.  On the possible origin of humic matter in fine continental aerosol , 2002 .

[66]  P. Paatero,et al.  Understanding and controlling rotations in factor analytic models , 2002 .

[67]  N. Calace,et al.  Humic Marine Matter and Insoluble Materials in Antarctic Snow , 2001 .

[68]  William B. Whitten,et al.  Fullerene Evolution in Flame-Generated Soot , 2000 .

[69]  S. Eisenreich,et al.  Adsorption onto Aerosol Soot Carbon Dominates Gas-Particle Partitioning of Polycyclic Aromatic Hydrocarbons , 2000 .

[70]  C. Liousse,et al.  Construction of a 1° × 1° fossil fuel emission data set for carbonaceous aerosol and implementation and radiative impact in the ECHAM4 model , 1999 .

[71]  Hans-Christen Hansson,et al.  Inorganic, organic and macromolecular components of fine aerosol in different areas of Europe in relation to their water solubility , 1999 .

[72]  J. Logan,et al.  Global chlorine emissions from biomass burning: Reactive Chlorine Emissions Inventory , 1999 .

[73]  H. Clark Light blue touch paper and retire , 1997 .

[74]  P. Coleman,et al.  Dioxins in ambient air, bonfire night 1994 , 1997 .

[75]  Ian Colbeck,et al.  Ambient aerosol concentrations at a site in SE England during bonfire night 1995 , 1996 .

[76]  A. M. Stortini,et al.  Air-Sea Exchange: Sea Salt and Organic Microcomponents in Antarctic Snow , 1996 .

[77]  P. Paatero,et al.  Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values† , 1994 .

[78]  S. C. O'brien,et al.  C60: Buckminsterfullerene , 1985, Nature.

[79]  T. Novakov,et al.  The aethalometer — An instrument for the real-time measurement of optical absorption by aerosol particles , 1983 .

[80]  J. Martinsson Using the Aethalometer for Source Apportionment of Carbonaceous Aerosols , 2014 .

[81]  Karl Ropkins,et al.  openair - An R package for air quality data analysis , 2012, Environ. Model. Softw..

[82]  D. Ceburnis,et al.  Minimizing light absorption measurement artifacts of the Aethalometer: evaluation of five correction algorithms , 2009 .

[83]  Comero Sara,et al.  Positive Matrix Factorisation (PMF) - An Introduction to the Chemometric Evaluation of Environmental Monitoring Data Using PMF , 2009 .

[84]  Christoph Hueglin,et al.  Source attribution of submicron organic aerosols during wintertime inversions by advanced factor analysis of aerosol mass spectra. , 2008, Environmental science & technology.

[85]  Yinon Rudich,et al.  Atmospheric HULIS : how humic-like are they ? A comprehensive and critical review , 2005 .

[86]  Paul M. Lemieux,et al.  Emissions of organic air toxics from open burning: a comprehensive review , 2004 .

[87]  K. Homann,et al.  The formation of polyhedral carbon ions in fuel-rich acetylene and benzene flames , 1989 .

[88]  H. Mukai,et al.  Characterization of a humic acid-like brown substance in airborne particulate matter and tentative identification of its origin , 1986 .

[89]  B. Simoneit Eolian particulates from oceanic and rural areas—their lipids fulvic and humic acids and residual carbon , 1980 .