Characterization of PM 10 sources in the central Mediterranean

Abstract. The Mediterranean Basin atmosphere is influenced by both strong natural and anthropogenic aerosol emissions and is also subject to important climatic forcings. Several programs have addressed the study of the Mediterranean basin; nevertheless important pieces of information are still missing. In this framework, PM10 samples were collected on a daily basis on the island of Lampedusa (35.5° N, 12.6° E; 45 m a.s.l.), which is far from continental pollution sources (the nearest coast, in Tunisia, is more than 100 km away). After mass gravimetric measurements, different portions of the samples were analyzed to determine the ionic content by ion chromatography (IC), the soluble metals by inductively coupled plasma atomic emission spectrometry (ICP-AES), and the total (soluble + insoluble) elemental composition by particle-induced x-ray emission (PIXE). Data from 2007 and 2008 are used in this study. The Positive Matrix Factorization (PMF) model was applied to the 2-year long data set of PM10 mass concentration and chemical composition to assess the aerosol sources affecting the central Mediterranean basin. Seven sources were resolved: sea salt, mineral dust, biogenic emissions, primary particulate ship emissions, secondary sulfate, secondary nitrate, and combustion emissions. Source contributions to the total PM10 mass were estimated to be about 40 % for sea salt, around 25 % for mineral dust, 10 % each for secondary nitrate and secondary sulfate, and 5 % each for primary particulate ship emissions, biogenic emissions, and combustion emissions. Large variations in absolute and relative contributions are found and appear to depend on the season and on transport episodes. In addition, the secondary sulfate due to ship emissions was estimated and found to contribute by about one-third to the total sulfate mass. Results for the sea-salt and mineral dust sources were compared with estimates of the same contributions obtained from independent approaches, leading to an estimate of the water content bound to the sea salt in the marine source.

[1]  M. Lazaridis,et al.  Physico-chemical characteristics of particulate matter in the Eastern Mediterranean , 2012 .

[2]  Sea-salt aerosol forecasts compared with daily measurements at the island of Lampedusa (Central Mediterranean) , 2011 .

[3]  N. Pérez,et al.  Transport of desert dust mixed with North African industrial pollutants in the subtropical Saharan Air Layer , 2011 .

[4]  Mar Viana,et al.  Chemical tracers of particulate emissions from commercial shipping. , 2009, Environmental science & technology.

[5]  R. Draxler.  HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) Model access via NOAA ARL READY Website , 2010 .

[6]  S. Pandis,et al.  Water content of aged aerosol , 2010 .

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

[8]  F. Monteleone,et al.  Seasonal evolution of the tropospheric aerosol vertical profile in the central Mediterranean and role of desert dust , 2009 .

[9]  P. Bousquet,et al.  Tropospheric aerosol ionic composition in the Eastern Mediterranean region , 1997 .

[10]  R. Harrison,et al.  AIRUSE-LIFE+: a harmonized PM speciation and source apportionment in five southern European cities , 2015 .

[11]  Daniela Meloni,et al.  Forest fire aerosol over the Mediterranean basin during summer 2003 , 2005 .

[12]  F. Monteleone,et al.  Influence of transport and trends in atmospheric CO2 at Lampedusa , 2009 .

[13]  Albert Ansmann,et al.  Profiling of Saharan dust and biomass-burning smoke with multiwavelength polarization Raman lidar at Cape Verde , 2011 .

[14]  Dominik Brunner,et al.  Assessment of parameters describing representativeness of air quality in-situ measurement sites , 2009 .

[15]  M. Stafoggia,et al.  African dust outbreaks over the Mediterranean Basin during 2001–2011: PM 10 concentrations, phenomenology and trends, and its relation with synoptic and mesoscale meteorology , 2012 .

[16]  William J. Teesdale,et al.  The Guelph PIXE software package II , 1989 .

[17]  A. Unal,et al.  Summertime aerosol chemical composition in the Eastern Mediterranean and its sensitivity to temperature , 2012 .

[18]  Nikos Mihalopoulos,et al.  Seasonal variation of dimethylsulfide in the gas phase and of methanesulfonate and non-sea-salt sulfate in the aerosols phase in the Eastern Mediterranean atmosphere , 2002 .

[19]  P. Paatero,et al.  Atmospheric aerosol over Alaska: 2. Elemental composition and sources , 1998 .

[20]  Franco Lucarelli,et al.  A comparison between PIXE and ICP-AES measurements of metals in aerosol particulate collected in urban and marine sites in Italy , 2014 .

[21]  U. Dayan,et al.  Relationship between methanesulfonate (MS−) in atmospheric particulate and remotely sensed phytoplankton activity in oligo-mesotrophic central Mediterranean Sea , 2013 .

[22]  A. Avila,et al.  Mineralogical composition of African dust delivered by red rains over northeastern Spain , 1997 .

[23]  Mihalis Vrekoussis,et al.  Origin and variability of particulate matter (PM10) mass concentrations over the Eastern Mediterranean , 2006 .

[24]  S. Pandis,et al.  Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis , 2011 .

[25]  A. D'Alessandro,et al.  Characterization of particulate matter sources in an urban environment. , 2008, The Science of the total environment.

[26]  Mathias Kluge,et al.  Principles Of Geochemistry , 2016 .

[27]  Franco Lucarelli,et al.  Saharan dust aerosol over the central Mediterranean Sea: PM10 chemical composition and concentration versus optical columnar measurements , 2014 .

[28]  A. Piazzalunga,et al.  Technical Note: On the effect of water-soluble compounds removal on EC quantification by TOT analysis in urban aerosol samples , 2011 .

[29]  A. Migliori,et al.  The new external beam facility for environmental studies at the Tandetron accelerator of LABEC , 2006 .

[30]  X. Querol,et al.  Variations of levels and composition of PM10 and PM2.5 at an insular site in the Western Mediterranean , 2009 .

[31]  R. Vecchi,et al.  Saharan dust impact in central Italy: An overview on three years elemental data records , 2012 .

[32]  Timo Mäkelä,et al.  Chemical composition and sources of fine and coarse aerosol particles in the Eastern Mediterranean , 2008 .

[33]  Cinzia Perrino,et al.  Particulate matter and gaseous pollutants in the Mediterranean Basin: results from the MED-PARTICLES project. , 2014, The Science of the total environment.

[34]  Davide Meloni,et al.  Mediterranean aerosol radiative forcing and influence of the single scattering albedo , 2009 .

[35]  On the autarchic use of solely PIXE data in particulate matter source apportionment studies by receptor modeling , 2015 .

[36]  F. Petrucci,et al.  May 14C be used to date contemporary art , 2013 .

[37]  U. Dayan,et al.  MBAS (Methylene Blue Active Substances) and LAS (Linear Alkylbenzene Sulphonates) in Mediterranean coastal aerosols: Sources and transport processes , 2011 .

[38]  Operational considerations to improve total ozone measurements with a Microtops II ozone monitor , 2011 .

[39]  Michael Cusack,et al.  Variability in regional background aerosols within the Mediterranean , 2009 .

[40]  S. Pandis,et al.  Contribution of particulate water to the measured aerosol optical properties of aged aerosol , 2014 .

[41]  H. Jorquera.  Source apportionment of PM10 and PM2.5 at Tocopilla, Chile (22°05’S, 70°12’W) , 2009, Environmental monitoring and assessment.

[42]  J. Randerson,et al.  Global burned area and biomass burning emissions from small fires , 2012 .

[43]  Ying Wang,et al.  Characterization of the single particle mixing state of individual ship plume events measured at the Port of Los Angeles. , 2010, Environmental science & technology.

[44]  P. Hopke,et al.  Source characterization of ambient fine particles at multiple sites in the Seattle area , 2008 .

[45]  N. Pérez,et al.  Source apportionment of fine PM and sub-micron particle number concentrations at a regional background site in the western Mediterranean: a 2.5 year study , 2013 .

[46]  P. Paatero.  Least squares formulation of robust non-negative factor analysis , 1997 .

[47]  M. Pujadas,et al.  Individual particle characteristics of North African dust under different long-range transport scenarios , 2009 .

[48]  D. Ie,et al.  Profiling of Saharan dust and biomass-burning smoke with multiwavelength polarization Raman lidar at Cape Verde , 2011 .

[49]  David R. Cocker,et al.  In-use gaseous and particulate matter emissions from a modern ocean going container vessel , 2008 .

[50]  Jay R. Herman,et al.  Comparison of ground‐based and Total Ozone Mapping Spectrometer erythemal UV doses at the island of Lampedusa in the period 1998–2003: Role of tropospheric aerosols , 2005 .

[51]  P. Quinn,et al.  Variations in the methanesulfonate to sulfate molar ratio in submicrometer marine aerosol particles over the south Pacific Ocean , 1992 .

[52]  F. Lucarelli,et al.  Proton induced γ-ray emission yields for the analysis of light elements in aerosol samples in an external beam set-up , 2010 .

[53]  A. Piazzalunga,et al.  A mass closure and PMF source apportionment study on the sub-micron sized aerosol fraction at urban sites in Italy , 2008 .

[54]  Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site during SAPUSS -diurnal variations and PMF receptor modelling , 2013 .

[55]  S. Pugnaghi,et al.  Shortwave and longwave radiative effects of the intense Saharan dust event of 25–26 March 2010 at Lampedusa (Mediterranean Sea) , 2011 .

[56]  Franco Lucarelli,et al.  Evidence for heavy fuel oil combustion aerosols from chemical analyses at the island of Lampedusa: a possible large role of ships emissions in the Mediterranean , 2012 .

[57]  R. Vecchi,et al.  The new sample preparation line for radiocarbon measurements on atmospheric aerosol at LABEC , 2011 .

[58]  A. Piazzalunga,et al.  Radiocarbon analysis on organic and elemental carbon in aerosol samples and source apportionment at an urban site in Northern Italy , 2013 .

[59]  J. Smol,et al.  Chemical composition of size-resolved atmospheric aerosols in the eastern Mediterranean during summer and winter , 2002 .

[60]  V. Aneja,et al.  Regional analysis of cloud chemistry at high elevations in the eastern United States , 1992 .

[61]  Nilgün Kubilay,et al.  Chemical composition of the fine and coarse fraction of aerosols in the northeastern Mediterranean , 2007 .

[62]  J. Lelieveld,et al.  Importance of mineral cations and organics in gas-aerosol partitioning of reactive nitrogen compounds : case study based on MINOS results , 2005 .

[63]  D. Massabò,et al.  Source apportionment of PM10 in the Western Mediterranean based on observations from a cruise ship , 2014 .

[64]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1997 .

[65]  Barbara J. Turpin,et al.  Species Contributions to PM2.5 Mass Concentrations: Revisiting Common Assumptions for Estimating Organic Mass , 2001 .

[66]  X. Querol,et al.  Daily and hourly sourcing of metallic and mineral dust in urban air contaminated by traffic and coal-burning emissions , 2013 .

[67]  Gary A. Norris,et al.  Methods for estimating uncertainty in factor analytic solutions , 2013 .

[68]  F. Amato,et al.  Biomass burning contributions estimated by synergistic coupling of daily and hourly aerosol composition records. , 2015, The Science of the total environment.

[69]  X. Querol,et al.  African dust outbreaks over the western Mediterranean Basin: 11-year characterization of atmospheric circulation patterns and dust source areas , 2014 .

[70]  Daniela Meloni,et al.  Aerosol optical properties at Lampedusa (Central Mediterranean). 1. Influence of transport and identification of different aerosol types , 2005 .

[71]  X. Querol,et al.  Origin of the exceedances of the European daily PM limit value in regional background areas of Spain , 2007 .

[72]  F. Lucarelli,et al.  Is PIXE still a useful technique for the analysis of atmospheric aerosols? The LABEC experience , 2011 .

[73]  G. Zhuang,et al.  Characteristics and sources of formic；acetic and oxalic acids in PM2.5 and PM10 aerosols in Beijing；China , 2007 .

[74]  E. Manoli,et al.  Concentrations and source apportionment of PM10 and associated major and trace elements in the Rhodes Island, Greece. , 2012, The Science of the total environment.

[75]  P. Formenti,et al.  Self‐attenuation artifacts and correction factors of light element measurements by X‐ray analysis: Implication for mineral dust composition studies , 2010 .