ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-11-10845-2011 Black carbon emissions from biomass and fossil fuels in rural India Rehman I. H. 1 Ahmed T. 2 Praveen P. S. 2 Kar A. 1 Ramanathan V. 2 The Energy and Resources Institute, Darbari Seth Block, IHC Complex, Lodhi Road, New Delhi, 110003, India Center for Clouds, Chemistry and Climate, Scripps Institution of Oceanography, University of California, San Diego, 9500 Gilman Drive, MC 0221, La Jolla, CA 92093-0221, USA 07 04 2011 11 4 10845 10874 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys-discuss.net/11/10845/2011/acpd-11-10845-2011.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/11/10845/2011/acpd-11-10845-2011.pdf

Black carbon (BC) emissions from biofuel cooking in South Asia and its radiative forcing is a significant source of uncertainty for health and climate impact studies. Quantification of BC emissions in the published literature is either based on laboratory or remote field observations far away from the source. For the first time under Project Surya, we use field measurements taken simultaneously inside rural households, ambient air and vehicular emissions from highways in a rural area in the Indo-Gangetic-Plains region of India to establish the role of both solid biomass based cooking in traditional stoves and diesel vehicles in contributing to high BC and organic carbon (OC), and solar absorption. The major finding of this study is that BC concentrations, both indoors and outdoors, have anomalously large twice-daily peak concentrations reaching 60 μg m<sup>−3</sup> (median 15-min average value) during the early morning (05:00 to 08:00) and early evening (17:00 to 19:00) hours coinciding with the morning and evening cooking hours. The BC during the non-cooking hours were also large, in the range of 2 to 30 μg m<sup>−3</sup>. The peak BC concentrations reached as high as 1000 μg m<sup>−3</sup>. The large diurnal peaks seen in this study lead to the conclusion that satellite based aerosol studies that rely on once- daily daytime measurements may severely underestimate the BC loading of the atmosphere. The concentration of OC was a factor of 5 larger than BC and furthermore optical data show that absorbing brown carbon was a major component of the OC. The imprint of the cooking hour peaks were seen in the outdoor BC both in the village as well as in the highway. The results have significant implications for climate and epidemiological studies.

 References Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, http://dx.doi.org/10.5194/acp-6-3131-2006doi:10.5194/acp-6-3131-2006, 2006. Auffhammer, M., Ramanathan, V., and Vincent, J. R.: Integrated model shows that atmospheric brown clouds and greenhouse gases have reduced rice harvests in India, PNAS, 103, 19668–19672, http://dx.doi.org/10.1073/pnas.0609584104doi:10.1073/pnas.0609584104, 2006. Beegum, G. N., Moorthy, K. K., Babu, S. S., Sathhesh, S., Vinoj, V., Badarinath, K., Safai, P., Devara, P., Singh, S., Vinod, Dumka, U., and Pant, P.: Spatial distribution of aerosol black carbon over India during pre-monsoon season, Atmos. Environ., 43, 1071–1078, 2009. Bond, T. C., Bhardwaj, E., Dong, R., Jogani, R., Jung, S., Roden, C., Streets, D. G., Fernandes, S., and Trautmann, N.: Historical emissions of black and organic carbon aerosol from energyrelated combustion, 1850–2000, Global Biogeochem. Cy., 21, GB2018, http://dx.doi.org/10.1029/2006GB002840doi:10.1029/2006GB002840, 2007. Di Girolamo, L., T. C. Bond, D. Bramer, D. J. Diner, F. Fettinger, R. A. Kahn, J. V. Martonchik, M. V. Ramana, V. Ramanathan, and Rasch, P.J.: Analysis of Multi-angle Imaging SpectroRadiometer (MISR) Aerosol Optical Depths Over Greater India During Winter 2001–2004, Geophys. Res. Lett., 31, L23115, http://dx.doi.org/10.1029/2004GL021273doi:10.1029/2004GL021273, 2004. Dockery, D. W. and Stone, P. H.: Cardiovascular risks from fine particulate air pollution, New Engl. J. Med., 365, 511–513, 2007. Ezzati, M. and Kamen, D. M.: The health impact of exposure to indoor air pollution from solid fuels in developing countries: Knowledge, gaps and data needs, Environ. Health Persp., 110, 1057–1068, 2002. Flanner, M. G., Zender, C. S., Hess, P. G., Mahowald, N. M., Painter, T. H., Ramanathan, V., and Rasch, P. J.: Springtime warming and reduced snow cover from carbonaceous particles, Atmos. Chem. Phys., 9, 2481–2497, http://dx.doi.org/10.5194/acp-9-2481-2009doi:10.5194/acp-9-2481-2009, 2009. Forastiere, F.: Fine particles and lung cancer, Occup. Environ. Med., 61, 797–798, http://dx.doi.org/10.1136/oem.2004.014290doi:10.1136/oem.2004.014290, 2004. Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Changes in Atmospheric Constituents and in Radiative Forcing, in: Climate Change 2007: The Physical Science Basis, Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L., Cambridge University Press, Cambridge, UK and New York, NY, USA, 2007. Gonçalves, C., Alves, C., Evtyugina, M., Mirante, F., Pio, C., Caseiro, A., Schmidl, C., Bauer, H., and Carvalho, F.: Characterisation of PM$_10$ emissions from woodstove combustion of common woods grown in Portugal, Atmos. Environ., 44, 4474–4480, 2010. Gustafsson, O., Kruså, M., Zencak, Z., Sheesley, R. J., Granat, L., Engström, E., Praveen, P. S., Leck, R. C., and Rodhe, H.: Brown Clouds over South Asia: Biomass or Fossil Fuel Combustion?, Science, 323, 495–498, 2009. Hansen, A. D. A., Rosen, H., and Novakov, T.: The aethalometer, an instrument for the real time measurement of optical absorption by aerosol particles, Sci. Total Environ., 36, 191–196, 1984. IEA (International~Energy Agency): World Energy Outlook 2007: China and India Insights, International Energy Agency, Paris, France, 2007 Jacobson, M. Z.: Short-term effects of controlling fossil-fuel soot, biofuel soot and gases, and methane on climate, Arctic ice, and air pollution health, J. Geophys. Res., 115, D14209, http://dx.doi.org/10.1029/2009JD013795doi:10.1029/2009JD013795, 2010. Kar, A., Praveen, P. S., Suresh, R., Rehman, I. H., Singh, L. , Singh, V. K., Ahmed,~T., Burney, J., and Ramanathan, V.: Real time assessment of Black Carbon pollution in rural households due to cooking in traditional and improved biomass stoves, Environ. Sci. Technol., submitted, 2011. Kirchstetter, T. W., Novakov, T., and Hobbs, P.: Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon, J. Geophys. Res., 109, D21208, http://dx.doi.org/10.1029/2004JD004999doi:10.1029/2004JD004999, 2004. Lau, K.-M., Ramanathan, V., Wu, G.-X, Li, Z., Tsay, S. C., Hsu, C., Sikka, R., Holben, B., Lu, D., Tartari, G., Chin, M., Koudelova, P., Chen, H., Ma, Y., Huang, J., Taniguchi, K., and Zhang, R.: The joint aerosol – monsoon experiment : A new challenge for monsoon climate research, Am. Meteorol. Soc., 89, 369–383, 2008. Lawrence, M. G. and Lelieveld, J.: Atmospheric pollutant outflow from southern Asia: a review, Atmos. Chem. Phys., 10, 11017–11096, http://dx.doi.org/10.5194/acp-10-11017-2010doi:10.5194/acp-10-11017-2010, 2010. Menon, S., Hansen, J., Nazarenko, L., and Luo, Y.: Climate effects of black carbon aerosols in China and India, Science, 297, 2250–2253, 2002. Menon, S., Koch, D., Beig, G., Sahu, S., Fasullo, J., and Orlikowski, D.: Black carbon aerosols and the third polar ice cap, Atmos. Chem. Phys., 10, 4559–4571, http://dx.doi.org/10.5194/acp-10-4559-2010doi:10.5194/acp-10-4559-2010, 2010. Novakov, T., Andreae, M. O., Gabriel, R., Kirchstetter, T. W., Mayol-Bracero, O. L., and Ramanathan, V.: Origin of carbonaceous aerosols over the tropical Indian Ocean: Biomass burning or fossil fuels?, Geophys. Res. Lett., 27, 4061–4064, 2000. Penn, A., Murphy, G., Barker, S., Henk, W., and Penn, L.: Combustion-derived ultrafine particles transport organic toxicants to target respiratory cells, Environ. Health Persp., 113, 956–963, 2005. Pope, C. A., Thun, M. J., Namboodiri, M. M., Dockery, D. W., Evans, J. S., Speizer, F. E., and Heath, C.W.: Particulate Air-Pollution as a Predictor of Mortality in a Prospective-Study of US Adults, Am. J. Respir. Crit. Care Med, 151, 669–674, 1995. Praveen, P. S., Kar, A., Ahmed, T., Rehman, I. H., and Ramanathan, V.: Local to regional scale solar absorption by black carbon from cooking: Base line data analysis of Project Surya, Atmos. Chem. Phys. Discuss., submitted, 2011. Ramana, M. V., Ramanathan, V., Podgorny, I. A., Pradhan, B. B., and Shrestha, B.: The Direct Observations of Large Aerosol Radiative Forcing in the Himalayan Region, Geophys. Res. Lett., 31, L05111, http://dx.doi.org/10.1029/2003GL018824doi:10.1029/2003GL018824, 2004. Ramanathan, V. and Balakrishnan, K.: Project Surya: Reduction of air pollution and global warming by cooking with renewable sources, White paper, available at: http://www.projectsurya.org/storage/Surya-WhitePaper.pdf, 2007. Ramanathan, V. and Carmichael, G.: Global and regional climate changes due to black carbon, Nat. Geosci., 1, 221–227, 2008. Ramanathan, V. and Ramana, M. V.: Persistent, Widespread, and Strongly Absorbing Haze Over the Himalayan Foothills and the Indo-Ganges Plains, Pure and Applied Geophysics, 162, 1609–1626, 2005. Ramanathan, V., Crutzen, P. J., Kiehl, J. T., and Rosenfeld, D.: Aerosols, Climate, and The Hydrological Cycle, Science, 294, 2119–2124, 2001. Ramanathan, V., Chung, C., Kim, D., Bettge, T., Buja, L., Kiehl, J. T., Washington, W. M., Fu, Q., Sikka, D. R, and Wild, M.: Atmospheric Brown Clouds: Impacts on South Asian Climate and Hydrological Cycle, Proceedings of the Natl. Acad. Sci. USA, 102(15), 5326–5333, 2005. Ramanathan, V., Ramana, M. V., Roberts, G., Kim, D., Corrigan, C., Chung, C., and Winker, D.: Warming trends in Asia amplified by brown cloud solar absorption; Nature, 448, 575–578, http://dx.doi.org/10.1038/nature06019doi:10.1038/nature06019, 2007. Ramanathan, V., Rehman, I. H., and Ramanathan, N.: Project Surya Prospectus. University of California, San Diego, 14~pp., 2010. Ramanathan, N., Lukac, M., Ahmed, T., Kar, A., Siva, P., Honles, T., Leong, I., Rehman, I.H., Schauer, J., and Ramanathan, V.: A Cellphone Based System for Global Monitoring of Black Carbon, Atmos. Environ., submitted, 2011. Roden, C. A., Bond, T. C., Conway, S., and Pinel, A. B. O.: Emission factors and real-time optical properties of particles emitted from traditional wood burning cook stoves, Environ. Sci. Technol., 40, 6750–6757, 2006. Roden, C. A., Bond, T. C., Conway, S., Pinel, A. B. O., MacCarty, N., and Still, D.: Laboratory and field investigation of particulate and carbon monoxide emissions from traditional and improved cookstoves, Atmos. Environ., 43, 1170–1181, 2009. Rom, W. N. and Samet, J. M.: Small particles with big effects, Am. J. Respir. Crit. Care, 173, 365–369, 2006. Satheesh, S. K., Ramanathan, V., Holben, B. N., Moorthy, K. K. , Loeb, N. G., Maring, H., Prospero, J. M., and Savoie, D.: Chemical, microphysical, and radiative effects of Indian Ocean aerosols, J. Geophys. Res., 107(D23), 4725, http://dx.doi.org/10.1029/2002JD002463doi:10.1029/2002JD002463, 2002. Sauvain, J.J ., Vu Duc, T., and Guillemin, M.: Exposure to Polycyclic Aromatic Compounds and health Risk Assessment for Diesel Exposed Workers, Int. Arch. Occ. Env. Hea., 76, 443–455, 2003. Schauer, J. J., Mader, B. T., DeMinter, J. T., Heidemann, G., Bae, M. S., Seinfeld, J. H., Flagan, R, C., Cary, R. A., Smith, D., Huebert, B. J., Bertram, T., Howell, S., Kline, J. T., Quinn, P., Bates, T., Turpin, B., Lim, H. J., Yu, J. Z., Yang, H., and Keywood, M. D.: ACE-Asia intercomparison of a thermal-optical method for the determination of particle-phase organic and elemental carbon, Environ. Sci. Technol., 37, 993–1001, 2003. Schwarze, P. E., Ovrevik, J., and Lag, M.: Particulate matter properties and health effects: consistency of epidemiological and toxicological studies, Human and Experimental Toxicology, 25, 559–579, 2006. Schmidl, C., Marr, I. L., Caseiro, A., Kotianova, P., Berner, A., Bauer, H., Kasper-Giebl., A., and Puxbaum, H.: Chemical characterisation of fine particles emissions from wood stove combustion of common woods growing in mid-European Alpine regions, Atmos. Environ., 42, 126–141, 2008. Tripathi, S. N., Dey, S., Tare, V., and Satheesh, S. K.: Aerosol black carbon radiative forcing at an industrial city in northern India, Geophys. Res. Lett., 32, L08802, doi:1029/2005GL022515, 2005. Venkataraman, C., Habib, G., Eiguren-Fernandez, A., Miguel, A. H., and Friedlander, S. K.: Residential Biofuels in South Asia: Carbonaceous Aerosol -Emissions and Climate Impacts, Science, 307, 1454-56, 2005. Venkataraman, C., Sagar, A. D., Habib, G., Lam, N., and Smith, K. R.: The Indian National Initiative for advanced biomass cookstoves: The benefits of clean combustion, Energy for Sustainable Development, 14, 63–72, 2010. World Health Organization: The World Health Report 2002: reducing risks, promoting healthy life, Geneva, Switzerland, World Health Organization, 2002. Zhu, A., Ramanathan, V., Li, F., and Kim, D.: Dust plumes over the Pacific, Indian, and Atlantic oceans: Climatology and radiative impact, J. Geophys. Res., 112, D16208, http://dx.doi.org/10.1029/2007JD008427doi:10.1029/2007JD008427, 2007.