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Louchouarn P 1 ,

Reconstructing the Record of Anthropogenic Pyrogenic Carbon Emissions Since the Onset of the Industrial Revolution: Location , Location, Location. Louchouarn P 1 , Kopp K 1 , Kjær K.K . 2 , Ilsoe P 2 , Andresen C 2 , Chillrud S 3 & Rumpel C 4

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Louchouarn P 1 ,

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  1. Reconstructing the Record of Anthropogenic Pyrogenic Carbon Emissions Since the Onset of the Industrial Revolution: Location, Location, Location Louchouarn P1, Kopp K1, KjærK.K.2, IlsoeP2, Andresen C2, ChillrudS3& RumpelC4 1 Department of Marine Science, Texas A&M University at Galveston, USA. 2 Department of Geosciences and Natural Resource Management, University of Copenhagen, Denmark. 3 Department of Earth and Environmental Sciences, Columbia University, USA. 4LaboratoireBiogéochimie et écologie des milieuxcontinentaux, Site du Centre INRA Versailles-Grignon, France.

  2. Why Study Pyrogenic Carbon? Radiatively important aerosols (direct and indirect impacts) “Short-circuit” in the carbon cycle? • Atmospheric chemistry and health impact (PM2.5-10, PAHs, BC, VOCs) • Prescribed fires and wildfires contribute20% of the PM2.5 emissions in the U.S. Cooney, C. (2008) ES&T. Vol. 42( 5).

  3. Pyrogenic (Black) Carbon: Structural properties of biochars/sootsand environmental application H/C Ratio 1.3 1.0 0.8 0.6 0.3 0.0 Masiello (2004) Marine Chemistry. Vol. 92 Chemically heterogeneous, biologically refractory (?) class of carbon compounds produced during biomass burning and fossil fuel combustion Charcoal: Remains of solid fuel phase (retain structural character) Soot: Condensation of hydrocarbon radicals from gas phase into submicron particles (usually nucleated)

  4. PyC: Structural properties and molecular tracers Honey Mesquite (HM) (Prosopisglandulosa) Cordgrass (CG) ( Spartinaspartinae) Kuo, L-J, B.E. Herbert, and P. Louchouarn. (2008). Organic Geochemistry. Vol. 39, 1466-1478. Kuo, L-J, P. Louchouarn, and B.E. Herbert. (2011). Chemosphere. Vol. 84, 797-805. Louchouarn, P., L-J. Kuo, T.L. Wade, and M. Schantz. (2009). Atmospheric Environment. Vol. 43, 5630-5636.

  5. PyC: Structural properties and molecular tracers • PAHs • Molecular carcinogenic contaminants • Emitted from incomplete combustion of organic matter. • Can be both pyrogenic as well as petrogenic. • Atmospheric increases primarily associated with the rise of industrial activities. Schneider, M., R.H. Smittenberg, T. Dittmar, and M.W.I. Schmidt. (2011). Organic Geochemistry, 42, 275–282. Keiluweit, M.; Kleber, M.; Sparrow, M. A.; Simoneit, B. R. T.; Prahl, F. G. (2012). Environ. Sci. Technol. 2012, 46, (17), 9333-9341.

  6. Pyrogenic (Black) Carbon and radiative forcing Hansen, J.E. and M. Sato (2001) . PNAS Vol. 98(26). Novakov et al. (2003) . GRL Vol. 30(6)

  7. Historical reconstruction of combustion:Working with historical archives Aquatic systems (and sedimentary systems) can be studied both in terms of their watershed and their airshed DeLuca and Aplet (2008) FEE. Vol. 6(1), 18-24 Lake Malawi - NASA: Visible Earth

  8. Methods • Sample Collection and analyses • Sediment Cores (urban lakes, urban coasts) • Dating methods • 210Pb and 137Cs • Pollens, biomarkers, historical events • Pyrogenic Carbon (PyC) • Two commonly used methods: CTO and GBC • PAHs (36 compounds) and diagnostic ratios

  9. Historical Air Quality:A Case Study I Black rain over NYC

  10. NYC Lakes Fluxes: An order of magnitude higher than other lakes BC inventory: CPL: 12625 mg/cm2 PPL: 12328 mg/cm2 Louchouarn et al. (2007) ES&T. Vol. 41(1), 82-87

  11. Sources of Soot-BC • d13C signatures of soot-BC • Homogeneity of inputs • Coal signatures with shift towards petroleum inputs in late 20th Century • Regional signatures (NYC vs Baltimore-DC)

  12. Puget SoundCase Study II HC-5 PS-1 HC-3 Kuo, Louchouarn et al. (2011) Envir. Poll. Vol. 159, 983-990 Louchouarn, et al. (2012). ES&T. Vol. 46(11), 5772−5781

  13. Puget Sound HC-5 HC-3 Kuo, Louchouarn et al. (2011) Envir. Poll. Vol. 159, 983-990 Louchouarn, et al. (2012). ES&T. Vol. 46(11), 5772−5781

  14. Historical Air Quality: A Case Study IIICity Core – Lake Botanisk(University of Copenhagen – Museum of Natural History)

  15. Lake StoraFrillingen: Sweden Elmquist, Zencak, and Gustafsson (2007) ES&T. Vol. 41, 6926−6932

  16. Lake StoraFrillingen vs. Lake Botanisk

  17. Lake StoraFrillingen vs. Lake Botanisk

  18. Oil Embargo Industrial Revolution Source: historoda.com 1974: Envirnonmental Protection Act and Clean Air Initiatives Source: EHS Journal/Nikita-Golovanov 1914 – 1918: World War I 1939 – 1945: World War II Germans troops parade in Copenhagen in April of 1940 to celebrate Hitler’s birthday 1860’s: Denmark’s Industrial Revolution 1810: Napoleonic Wars and the Battles of Copenhagen (1801 and 1807) Destruction of the Danish Fleet Before Copenhagen by Thomas Whitcombe 1795: Fire of Copenhagen The Spire of the Church of Our Lady on fire by Christoffer Wilhelm Eckersberg

  19. d13C Signatures of BC

  20. Conclusions • Local nature of fuel sources and consumption leads to geographical heterogeneities in PyC emissions and distribution  need for increased resolution of historical reconstructions. • A combination of elemental, isotopic, and molecular signatures of PyCin environmental archives show a strong potential for identifying fuel sources and regional distribution of combustion emissions from anthropogenic activities. • Urban lakes provides a unique opportunity for monitoring trends in markers of combustion over time in major urban system, but… Are they the best archives for climate reconstructions?

  21. Thank you M. Norwood1 Allison Myers-Pigg1 Kendra Kopp1 K. Pierce1* L-J. Kuo2* J.M. Brandenberger2* O. Harvey3* R. Amon1 G. Cornelissen4 R. Griffin5 K. Kjær6 C. Masiello5 A. Prokushkin7 R. Teissenrenc8 1Texas A&M University 2 Pacific Northwest National Laboratory 3 Univ. Southern Mississippi 4 Norwegian Geotechnical Institute 5 Rice University 6 Natural History Museum-University of Copenhagen 7 V N Sukachev Institute of Forest SB RAS 8Institut National Polytechniquede Toulouse, INP-ENSAT-ECOLAB * Former Students Funding sources

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