A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

Atmospheric Measurement Techniques - Tập 9 Số 11 - Trang 5637-5653
Yanping Zhang1, Brent J. Williams1, A. H. Goldstein2, Kenneth S. Docherty3,4,5, J. L. Jiménez3,4
1Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, Missouri, USA
2Department of Environmental Science, Policy, & Management, University of California, Berkeley, California, USA
3Cooperative Institute for Research in the Environmental Sciences (CIRES), University of Colorado, Boulder, California, USA
4Dept. of Chemistry & Biochemistry, University of Colorado, Boulder, Colorado, USA
5currently at: Alion Science and Technology, US EPA Office of Research and Development, Research Triangle Park, North Carolina, USA

Tóm tắt

Abstract. We present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography–mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level resolution on other bulk aerosol components commonly observed by the AMS.

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Tài liệu tham khảo

Allan, J. D., Jimenez, J. L., Williams, P. I., Alfarra, M. R., Bower, K. N., Jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an Aerodyne aerosol mass spectrometer – 1. Techniques of data interpretation and error analysis, J. Geophys. Res.-Atmos., 108, 4090, https://doi.org/10.1029/2002jd002358, 2003.

Ahlm, L., Shakya, K. M., Russell, L. M., Schroder, J. C., Wong, J. P. S., S. J., Hayden, K. L., Liggio, J., Wentzell, J. J. B., Wiebe, H. A., Mihele, C., Leaitch, W. R., and Macdonald, A. M.: Temperature-dependent accumulation mode particle and cloud nuclei concentrations from biogenic sources during WACS 2010, Atmos. Chem. Phys., 13, 3393–3407, https://doi.org/10.5194/acp-13-3393-2013, 2013.

Canagaratna, M. R., Jayne, J. T., Jimenez, J. L., Allan, J. D., Alfarra, M. R., Zhang, Q., Onasch, T. B., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L. R., Trimborn, A. M., Northway, M. J., DeCarlo, P. F., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer, Mass Spectrom. Rev., 26, 185–222, https://doi.org/10.1002/mas.20115, 2007.

Chueinta, W., Hopke, P. K., and Paatero, P.: Investigation of sources of atmospheric aerosol at urban and suburban residential areas in Thailand by positive matrix factorization, Atmos. Environ., 34, 3319–3329, 2000.

Docherty, K. S., Stone, E. A., Ulbrich, I. M., DeCarlo, P. F., Snyder, D. C., Schauer, J. J., Peltier, R. E., Weber, R. J., Murphy, S. M., Seinfeld, J. H., Grover, B. D., Eatough, D. J., and Jimenez, J. L.: Apportionment of Primary and Secondary Organic Aerosols in Southern California during the 2005 Study of Organic Aerosols in Riverside (SOAR-1), Environ. Sci. Technol., 42, 7655–7662, https://doi.org/10.1021/es8008166, 2008.

Docherty, K. S., Aiken, A. C., Huffman, J. A., Ulbrich, I. M., DeCarlo, P. F., Sueper, D., Worsnop, D. R., Snyder, D. C., Peltier, R. E., Weber, R. J., Grover, B. D., Eatough, D. J., Williams, B. J., Goldstein, A. H., Ziemann, P. J., and Jimenez, J. L.: The 2005 Study of Organic Aerosols at Riverside (SOAR-1): instrumental intercomparisons and fine particle composition, Atmos. Chem. Phys., 11, 12387–12420, https://doi.org/10.5194/acp-11-12387-2011, 2011.

Dominici, F., Peng, R. D., Bell, M. L., Pham, L., McDermott, A., Zeger, S. L., and Samet, J. M.: Fine particulate air pollution and hospital admission for cardiovascular and respiratory diseases, JAMA-J. Am. Med. Assoc., 295, 1127–1134, https://doi.org/10.1001/jama.295.10.1127, 2006.

Gauderman, W. J., Urman, R., Avol, E., Berhane, K., McConnell, R., Rappaport, E., Chang, R., Lurmann, F., and Gilliland, F.: Association of Improved Air Quality with Lung Development in Children, New Engl. J. Med., 372, 905–913, https://doi.org/10.1056/NEJMoa1414123, 2015.

Goldstein, A. H. and Galbally, I. E.: Known and unexplored organic constituents in the earth's atmosphere, Environ. Sci. Technol., 41, 1514–1521, https://doi.org/10.1021/es072476p, 2007.

Goldstein, A. H., Worton, D. R., Williams, B. J., Hering, S. V., Kreisberg, N. M., Panic, O., and Gorecki, T.: Thermal desorption comprehensive two-dimensional gas chromatography for in-situ measurements of organic aerosols, J. Chromatogr. A, 1186, 340–347, https://doi.org/10.1016/j.chroma.2007.09.094, 2008.

Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.

IPCC: Climate Change 2013: The Physical Science Basis, 2013.

Isaacman, G., Kreisberg, N. M., Worton, D. R., Hering, S. V., and Goldstein, A. H.: A versatile and reproducible automatic injection system for liquid standard introduction: application to in-situ calibration, Atmos. Meas. Tech., 4, 1937–1942, https://doi.org/10.5194/amt-4-1937-2011, 2011.

Isaacman, G., Kreisberg, N. M., Yee, L. D., Worton, D. R., Chan, A. W. H., Moss, J. A., Hering, S. V., and Goldstein, A. H.: Online derivatization for hourly measurements of gas- and particle-phase semi-volatile oxygenated organic compounds by thermal desorption aerosol gas chromatography (SV-TAG), Atmos. Meas. Tech., 7, 4417–4429, https://doi.org/10.5194/amt-7-4417-2014, 2014.

Ito, K., Xue, N., and Thurston, G.: Spatial variation of PM2.5 chemical species and source-apportioned mass concentrations in New York City, Atmos. Environ., 38, 5269–5282, 2004.

Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prévôt, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.

Junjun, D., Zhenyu, X., Bingliang, Z., and Ke, D.: Comparative study on long-term visibility trend and its affecting factors on both sides of the Taiwan Strait, Atmos. Res., 143, 266–278, https://doi.org/10.1016/j.atmosres.2014.02.018, 2014.

Jaeckels, J. M., Bae, M. S., and Schauer, J. J.: Positive matrix factorization (PMF) analysis of molecular marker measurements to quantify the sources of organic aerosols, Environ. Sci. Technol., 41, 5763–5769, 2007.

Lee, E., Chan, C. K., and Paatero, P.: Application of positive matrix factorization in source apportionment of particulate pollutants in Hong Kong, Atmos. Environ., 33, 3201–3212, 1999.

Martinez, R. E., Williams, B. J., Zhang, Y., Hagan, D., Walker, M., Kreisberg, N. M., Hering, S. V., Hohaus, T., Jayne, J. T., and Worsnop, D. R.: Development of a volatility and polarity separator (VAPS) for volatility- and polarity-resolved organic aerosol measurement, Aerosol Sci. Technol., 50, 255–271, 2016.

Murphy, D. M., Cziczo, D. J., Froyd, K. D., Hudson, P. K., Matthew, B. M., Middlebrook, A. M., Peltier, R. E., Sullivan, A., Thomson, D. S., and Weber, R. J.: Single-particle mass spectrometry of tropospheric aerosol particles, J. Geophys. Res.-Atmos., 111, D23s32, https://doi.org/10.1029/2006jd007340, 2006.

Ng, N. L., Herndon, S. C., Trimborn, A., Canagaratna, M. R., Croteau, P. L., Onasch, T. B., Sueper, D., Worsnop, D. R., Zhang, Q., Sun, Y. L., and Jayne, J. T.: An Aerosol Chemical Speciation Monitor (ACSM) for Routine Monitoring of the Composition and Mass Concentrations of Ambient Aerosol, Aerosol Sci. Technol., 45, 780–794, https://doi.org/10.1080/02786826.2011.560211, 2011.

Paatero, P.: Least squares formulation of robust non-negative factor analysis, Chemometr. Intell. Lab., 37, 23–35, https://doi.org/10.1016/s0169-7439(96)00044-5, 1997.

Ramadan, Z., Song, X. H., and Hopke, P. K.: Identification of sources of Phoenix aerosol by positive matrix factorization, J. Air Waste Manage. Assoc., 50, 1308–1320, 2000.

Schauer, J. J., Rogge, W. F., Hildemann, L. M., Mazurek, M. A., Cass, G. R., and Simoneit, B. R. T.: Source apportionment of airborne particulate matter using organic compounds as tracers, Atmos. Environ., 30, 3837–3855, 1996.

Sun, Y. L., Zhuang, G. S., Tang, A. H., Wang, Y., and An, Z. S.: Chemical characteristics of PM2.5 and PM10 in haze-fog episodes in Beijing, Environ. Sci. Technol., 40, 3148–3155, https://doi.org/10.1021/es051533g, 2006.

Ulbrich, I. M., Canagaratna, M. R., Zhang, Q., Worsnop, D. R., and Jimenez, J. L.: Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data, Atmos. Chem. Phys., 9, 2891–2918, https://doi.org/10.5194/acp-9-2891-2009, 2009.

Williams, B. J., Goldstein, A. H., Kreisberg, N. M., and Hering, S. V.: An in-situ instrument for speciated organic composition of atmospheric aerosols: Thermal Desorption Aerosol GC ∕ MS-FID (TAG), Aerosol Sci. Technol., 40, 627–638, https://doi.org/10.1080/02786820600754631, 2006.

Williams, B. J., Goldstein, A. H., Kreisberg, N. M., Hering, S. V., Worsnop, D. R., Ulbrich, I. M., Docherty, K. S., and Jimenez, J. L.: Major components of atmospheric organic aerosol in southern California as determined by hourly measurements of source marker compounds, Atmos. Chem. Phys., 10, 11577–11603, https://doi.org/10.5194/acp-10-11577-2010, 2010.

Williams, B. J., Jayne, J. T., Lambe, A. T., Hohaus, T., Kimmel, J. R., Sueper, D., Brooks, W., Williams, L. R., Trimborn, A. M., Martinez, R. E., Hayes, P. L., Jimenez, J. L., Kreisberg, N. M., Hering, S. V., Worton, D. R., Goldstein, A. H., and Worsnop, D. R.: The First Combined Thermal Desorption Aerosol Gas Chromatograph–Aerosol Mass Spectrometer (TAG-AMS), Aerosol Sci. Technol., 358-370, https://doi.org/10.1080/02786826.2013.875114, 2014.

Williams, B. J., Zhang, Y., Zuo, X., Martinez, R. E., Walker, M. J., Kreisberg, N. M., Goldstein, A. H., Docherty, K. S., and Jimenez, J. L.: Organic and inorganic decomposition products from the thermal desorption of atmospheric particles, Atmos. Meas. Tech., 9, 1569–1586, https://doi.org/10.5194/amt-9-1569-2016, 2016.

Zenkevich, I. G. and Pavlovskii, A. A.: Overloading control of gas chromatographic systems, J. Sep. Sci., 38, 2848–2856, https://doi.org/10.1002/jssc.201401471, 2015.

Zhang, Q., Jimenez, J. L., Canagaratna, M. R., Ulbrich, I. M., Ng, N. L., Worsnop, D. R., and Sun, Y. L.: Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review, Anal. Bioanal. Chem., 401, 3045–3067, https://doi.org/10.1007/s00216-011-5355-y, 2011.

Zhang, Y., Williams, B. J., Goldstein, A. H., Docherty, K., Ulbrich, I. M., and Jimenez, J. L.: A Technique for Rapid Gas Chromatography Analysis Applied to Ambient Organic Aerosol Measurements from the Thermal Desorption Aerosol Gas Chromatograph (TAG), Aerosol Sci. Technol. 48, 1166–1182, https://doi.org/10.1080/02786826.2014.967832, 2014.

Zhao, Y. L., Kreisberg, N. M., Worton, D. R., Teng, A. P., Hering, S. V., and Goldstein, A. H.: Development of an In Situ Thermal Desorption Gas Chromatography Instrument for Quantifying Atmospheric Semi-Volatile Organic Compounds, Aerosol Sci. Technol., 47, 258–266, https://doi.org/10.1080/02786826.2012.747673, 2013.

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Atmospheric Measurement Techniques

Tập 9 Số 11

5637-5653

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