JRC Initiative on Source Apportionment Harmonization in Europe: Outline and Developments

1. JRC Initiative on Source Apportionment Harmonization in Europe: Outline and Developments Claudio A. Belis Joint Research Centre – IES – Air and Climate Unit FAIRMODE MEETING Antwerp 10th-12th April 2013

2. Structure of the presentation • JRC initative on Source Apportionment • Progress of work: • Survey and review of RM studies in Europe • Intercomparison for RM first step • Intercomparison for RM second step • RM Technical Protocol

3. Receptor Models • Use measured concentrations at the receptor • Are based on least square multivariate analysis to solve a chemical mass balance linear equation • Mainly used for PM, PAH and VOC • Not appropriate for reactive species • Appropriate for urban and regional scales Concentration of the jth species in the ith sample Concentration of the jth species in the pth source Basic equation Contribution of pth source to ith sample

4. APPRAISAL WP2 Receptor and source oriented models FIRST REVIEW ON RM IN EUROPE assess the impact of the metodology, list used tools and identify needs Completed Karagulian & Belis, 2012 IJEP INTERCOMPARISON EXERCISE FOR RM assess model performances and quantify uncertainty First step completed Karagulian & Belis, 2012 EUR REPORT Second step: in progress JRC INITIATIVE ON SOURCE APPORTIONMENT HARMONIZATION COMMON RECEPTOR MODELLING TECHNICAL PROTOCOL find common procedures and criteria to assure quality standards and improve comparability among studies In progress CRITICAL REVIEW AND META-ANALYSIS OF SA STUDIES take advantage of available data to estimate sources at the European level Completed Belis et al. 2013 AE FAIRMODE WG1 SG 2 ON NATURAL SOURCES AND SOURCE APPORTIONMENT

5. Critical Review of RM methods and quantification of main PM Sources in Europe

6. Critical Review of RM methods and quantification of PM Sources in Europe - Critical discussion of methods used in Europe - Meta-analysis of 272 records present in more than 100 papers and reports published until the beginning of 2012: - Identification of main source categories. - Description of geographical and seasonal variation of these sources were studied and mapped. - A special analysis of PM concentrations was made to assess the causes of exceedances

7. Critical Review of RM methods and quantification of PM Sources in Europe Classification of receptor models with particular reference to those used in Europe

8. @ Critical Review of RM methods and quantification of PM Sources in Europe SOURCES OF PARTICULATE MATTER IN EUROPE six major source categories for PM were defined that comprise the majority of the individual sources apportioned in Europe salt sulphate nitrate crustal traffic point bio. burn SIA Additional source coal combustion observed in specific areas e.g. Poland Marker Median ± 25P-75P (box) ± Min-Max (whiskers) Source Contributions estimated with receptor models using measured PM10 and PM2.5 chemical composition in urban background areas (preliminary results). 108 studies until 2012 - 272 records

9. Critical Review of RM methods and quantification of PM Sources in Europe Statistical analysis of the influence of: size fraction site type seasonal trends geographical patterns

10. Critical Review of RM methods and quantification of PM Sources in Europe For the OC fraction three main source categories were identified (60 records)

11. Critical Review of RM methods and quantification of PM Sources in Europe SOURCES OF PARTICULATE MATTER IN EUROPE Marker Median ± 25P-75P (box) ± Min-Max (whiskers) A special analysis of PM concentrations that exceed the current European air quality limits indicated SIA and traffic as the most important source categories to target for abatement throughout the year together with biomass burning during the cold season.

12. Critical Review of RM methods and quantification of PM Sources in Europe FINAL REMARKS • - Receptor models evolve towards tools with refined uncertainty treatment. • - Positive Matrix Factorization and Chemical Mass Balance are the most used models. • - Gas-to-particle conversion is the main PM mass and particulate organic carbon source. • - To abate exceedances, sources of secondary inorganic and traffic are the main target. • - More long term speciated PM datasets would foster source identification studies • - There is a need for harmonization in the methodology, with particular reference to the nomenclature of source categories.

13. Intercomparison for Receptor Models

14. Overall test sequence to identify the correspondence between participants factor/sources to each source category Preliminary tests If5out of10tests are nor meet then factor is considereddubious FINGERPRINTS Pearson and weighted difference SPECIES CONTRIBUTIONS (%) Pearson Final tests Z-score(SCE) TIME TRENDS Pearson Comparison factor/sources among each other and with reference source Model performance Participant performance Karagulian & Belis, 2012 IJEP, 50

15. Final test (ISO 13528) indicator: “OK” • SCE of participant’s source profile are optimal if: • considered coherent and satisfactory if: “acceptable” • results are considered questionable if: “warning” • results are unsatisfactory if: “action”

16. Intercomparison first step (real-world database) 16 participants First step: Real-world database  data elaboration completed Report completed Presentation in EAC 2012

17. Intercomparison first step: results PARTICIPANT’s Z(SCE) MODELS’ Z(SCE) unsatisfactory unsatisfactory warning warning • There is a good quantitative agreement between SCE. 86% of the factors meet the acceptability criteria (OK or acceptable). • The participant median bias in the SCEs is consistent with the 50% standard uncertainty acceptability criterion used in this evaluation. • PMF and CMB present the best performances, PCA showed the poorest performance but still acceptable acceptable acceptable OK OK

18. Intercomparison second step (synthetic database) 22 participants second step: synthetic database  data elaboration in progress Presentation in EAC 2013 (planned)

19. Synthetic database (in collab. with G. Pirovano, RSE) • Generated for PM2.5 using CAMx PSAT using the Po Valley dataset and extracted in selected points • The receptor corresponding to the city of Milan was used for the intercomparison • Emission profiles in literature were used to obtain the concentration of trace elements • Total sulphate, nitrate and ammonium calclulated to make them comparable to those measured in monitoring sites • Dust resuspension profile modulated using the wind speed measured in the area • Noise has been introduced using a random sampling from a log-normal distribution

20. Intercomparison second step: preliminary results

21. Z scores: conclusive remarks (1) • The previous evaluations were made using as reference a value that represents the average of all participants. In this test we use the same algorithm but the reference value represent the actual contribution added when constructing the database. • In the test with an external reference value participants/solutions with median values in the optimum area (<1) are 18 out 26. • Factor/sources in the acceptability area (<=2) are 85%, there is a 6% in the warning area and a 9% in the action area.

22. Z scores: conclusive remarks (2) • In this test, FA-MLRA median is in the warning area. And the the median of CMB robotic solutions is close to the warning area. • The advantage of this test is that is not necessary to remove solutions to avoid distortions. In addition, it is possible to assess possible bias of the solution that are not evident when using the average.

23. European Common Technical Protocol for Receptor Modelling • C.A. Belis1, F. Karagulian1, B. R. Larsen2, F. Amato3,4, O. Favez5, I. El Haddad6, R.M. Harrison7, A.S.H. Prevot6, U. Quass8, R. Vecchi9, M. Viana3, P. Paatero10, P.K. Hopke11 1European Commission, Institute for Environment and Sustainability - Joint Research Centre, Ispra, 21027, Italy 2European Commission, Institute for Health and Consumer Protection - Joint Research Centre, Ispra 21027, Italy 3Institute of Environmental Assessment and Water Research (IDAEA), Barcelona, 08034, Spain 4TNO Buil Environment and Geosciences, Dept. Air Quality and Climate, TA 3508,Utrecht, The Netherlands 5Institut National de l’Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, 60550, France 6Laboratory of Atmospheric Chemistry (LAC), Paul Scherrer Institut, Villigen, 5234, Switzerland 7National Centre for Atmospheric Science, University of Birmingham, Birmingham, B15 2TT, UK 8Air Quality and Sustainable nanotechnology (IUTA), D- Duisburg, 47229, Germany 9Department of Physics, Università degli Studi di Milano and INFN, Milan, 20133, Italy 10University of Helsinki, Finland 11Center for Air Resources Engineering and Science, Clarkson University, Potsdam, NY 13699-5708, USA

24. Common Receptor Model Technical Protocol (RMTP) Driving elements • The objective is to promote the best available operating procedures and to harmonize their application across Europe. • Target : -practitioners involved in the model execution and in the interpretation of results- policy makers interested in the output of RMs for the design of abatement measures, -air quality experts and scientists non familiar with this methodology • Different levels of complexity according to the reader skills • It is organized following a logical sequence • Contains tutorials, technical recommendations and check lists • It is not meant to report all the information but to provide relevant references to the information sources • The technical protocol is a guide and cannot substitute training and expertise

25. Common RMTP Outline PART A: INTRODUCTION TO SOURCE APPORTIONMENT WITH RECEPTOR MODELS Presents the work and provides the unskilled reader with basic elements on Source Apportionment and Receptor Modelling PART B: STANDARD RECEPTOR MODEL TECHNICAL PROTOCOL Is the core of the document. Contains description of the steps required in the most traditional and widespread Receptor Modelling techniques with particular reference to CMB and Factor Analysis PART C: SOPHISTICATED AND ADVANCED MODELS This section contains innovative and advanced methods most of which under continuous development. Also methods on trajectories that although have been available for long time their potentials have not been completely exploited

26. Common RMTP Outline PART A: INTRODUCTION TO SOURCE APPORTIONMENT WITH RECEPTOR MODELS Glossary Structure of the Document Identification of pollution sources What are RM? When to use RM? Harmonization of RM

27. PART B: STANDARD RECEPTOR MODEL TECHNICAL PROTOCOL PRELIMINARY EVALUATION OF THE STUDY AREA DEFINING A METHODOLOGICAL FRAMEWORK EXPERIMENTAL DESIGN DATA COLLECTION / FIELD WORK/ CHEMICAL ANALYSES KNOWING YOUR DATASET: BASIC STATISTICS PRELIMINARY DATA QUALITY CHECK INPUT DATA UNCERTAINTY CALCULATION CHEMICAL MASS BALANCE MODELS FACTOR ANALYSIS I: SELECTION OF THE NUMBER OF FACTORS FACTOR ANALYSIS II: EVALUATION OF SCE AND MODEL PERFORMANCE INDICATORS FACTOR ANALYSIS III: CRITERIA FOR FACTOR LABELLING OTHER MODEL PERFORMANCE TESTS REPORTING RESULTS PRELIMINARY ACTIVITIES FIELD AND LAB WORK DATA PRE-TREATMENT RECOMMENDATIONS SPECIFIC FOR CMB RECOMMENDATIONS SPECIFIC FOR FACTOR ANALYSIS COMPLEMENTARY TESTS AND REPORTING more details

28. PART C: ADVANCED MODELS 1. WIND AND TRAJECTORY ANALYSIS IN SOURCE APPORTIONMENT Combination of trajectories and wind direction analysis with receptor models makes it possible to evaluate the geographic provenience of sources. These techniques are also useful for RM output validation. 2. CONSTRAINED AND EXPANDED MODELS IN FACTOR ANALYSIS These models represent the new frontier of RM since make it possible to combine different type of data and make advanced data treatment 3. THE USE OF PMF IN AMS DATA PROCESSING Thanks to the application of (PMF) to find factors this methodology has many analogies with the traditional RMs. The experience gained by the community working with these tools may be useful for RM experts and viceversa. This is a promising technique that opens the opportunity for mutual validation with traditional RMs. 4. THE AETHALOMETER MODEL 5. ISOTOPIC RATIOS COMBINED WITH MACROTRACER ENRICHMENT FACTORS

29. Reporting results • The results are described according to the steps proposed in sections B1- B12. • Expert decisions concerning the identification of the number of sources and factor assignment are described providing evidence of the objective information that support them. • The quantitative uncertainty of the output should be estimated and reported using the embedded tests included in the most robust methodologies. • In addition, estimation of overall uncertainty and validation should be achieved using Monte Carlo permutations approach, by comparing outputs from independent models on the same data set, or applying other validated techniques.

30. Conclusions • The use of Receptor Models in Europe is widespread and there is a steady increasing trend. • In addition, RMs are useful for the validation of other techniques • The Common RMTP aims at answering:the need to inform and guide potential users (e.g. policy makers) the practitioners demand for common rules andthe request from final users of harmonization and quality assurance of SA output. • The Common RMTP is complementary with the RMIE which provides information on the performance and uncertainty of these techniques. • The Common RMTP is a support to practitioner that apply RM but cannot substitute experience and training • The Common RMTP is a living document that needs to be updated according to the development of the methodologies.

31. Thank you for your attention