Significant contribution of combustion-related emissions to the atmospheric phosphorus budget


Atmospheric phosphorus fertilizes plants and contributes to Earth’s biogeochemical phosphorus cycle. However, calculations of the global budget of atmospheric phosphorus have been unbalanced, with global deposition exceeding estimated emissions from dust and sea-salt transport, volcanic eruptions, biogenic sources and combustion of fossil fuels, biofuels and biomass, the latter of which thought to contribute about 5% of total emissions. Here we use measurements of the phosphorus content of various fuels and estimates of the partitioning of phosphorus during combustion to calculate phosphorus emissions to the atmosphere from all combustion sources. We estimate combustion-related emissions of 1.8 Tg P yr−1, which represent over 50% of global atmospheric sources of phosphorus. Using these estimates in atmospheric transport model simulations, we find that the total global emissions of atmospheric phosphorus (3.5 Tg P yr−1) translate to a depositional sink of 2.7 Tg P yr−1 over land and 0.8 Tg P yr−1 over the oceans. The modelled spatial patterns of phosphorus deposition agree with observations from globally distributed measurement stations, and indicate a near balance of the phosphorus budget. Our finding suggests that the perturbation of the global phosphorus cycle by anthropogenic emissions is larger thanpreviously thought.

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Figure 1: Frequency distributions of phosphorus contents of different fuels.
Figure 2: Historical trends of phosphorus emissions from fossil fuels, biofuels, deforestation fires and natural fires.
Figure 3: Spatial distributions of phosphorus deposition.
Figure 4: Comparison between modelled and observed phosphorus deposition with or without accounting for phosphorus emissions from combustion.
Figure 5: Historical evolution of atmospheric sources of phosphorus and nitrogen.


  1. 1

    Peñuelas, J. et al. Human-induced nitrogen–phosphorus imbalances alter natural and managed ecosystems across the globe. Nature Commun. 4, 2934 (2013).

    Article  Google Scholar 

  2. 2

    Vitousek, P. M., Porder, S., Houlton, B. Z. & Chadwick, O. A. Terrestrial phosphorus limitation: Mechanisms, implications and nitrogen–phosphorus interactions. Ecol. Appl. 20, 5–15 (2010).

    Article  Google Scholar 

  3. 3

    Broecker, W. S. Ocean chemistry during glacial time. Geochim. Cosmochim. Acta 46, 1689–1705 (1982).

    Article  Google Scholar 

  4. 4

    Handoh, I. C. & Lenton, T. M. Periodic mid-Cretaceous oceanic anoxic events linked by oscillations of the phosphorus and oxygen biogeochemical cycles. Glob. Biogeochem. Cycles 17, 1092 (2003).

    Article  Google Scholar 

  5. 5

    Rockström, J. et al. A safe operating space for humanity. Nature 461, 472–475 (2009).

    Article  Google Scholar 

  6. 6

    Smil, V. Phosphorus in the environment: Natural flows and human interferences. Annu. Rev. Energy Environ. 25, 53–88 (2000).

    Article  Google Scholar 

  7. 7

    Camarero, L. & Catalan, J. Atmospheric phosphorus deposition may cause lakes to revert from phosphorus limitation back to nitrogen limitation. Nature Commun. 3, 1118 (2012).

    Article  Google Scholar 

  8. 8

    Wu, J. et al. Phosphate depletion in the western North Atlantic Ocean. Science 289, 759–762 (2000).

    Article  Google Scholar 

  9. 9

    Okin, G. S. et al. Impact of desert dust on the biogeochemistry of phosphorus in terrestrial ecosystems. Glob. Biogeochem. Cycles 18, GB2005 (2004).

    Article  Google Scholar 

  10. 10

    Graham, W. F. & Duce, R. A. Atmospheric pathways of the phosphorus cycle. Geochim. Cosmochim. Acta 43, 1195–1208 (1979).

    Article  Google Scholar 

  11. 11

    Mahowald, N. et al. Impacts of biomass burning emissions and land use change on Amazonian atmospheric phosphorus cycling and deposition of phosphorus. Glob. Biogeochem. Cycles 19, GB4030 (2005).

    Google Scholar 

  12. 12

    Mahowald, N. et al. Global distribution of atmospheric phosphorus sources, concentrations and deposition rates, and anthropogenic impacts. Glob. Biogeochem. Cycles 22, GB4026 (2008).

    Article  Google Scholar 

  13. 13

    Tipping, E. et al. Atmospheric deposition of phosphorus to land and freshwater. Environ. Sci.: Processes Impacts 16, 1608–1617 (2014).

    Google Scholar 

  14. 14

    Bertine, K. K. & Goldberg, E. D. Fossil fuel combustion and the major sedimentary cycle. Science 173, 233–235 (1971).

    Article  Google Scholar 

  15. 15

    Chen, Y. et al. Global mercury emissions from combustion in light of international fuel trading. Environ. Sci. Technol. 48, 1727–1735 (2014).

    Article  Google Scholar 

  16. 16

    Wang, R. et al. Sources and pathways of polycyclic aromatic hydrocarbons transported to Alert, the Canadian High Arctic. Environ. Sci. Technol. 44, 1017–1022 (2010).

    Article  Google Scholar 

  17. 17

    Meij, R. Trace element behavior in coal-fired power plants. Fuel Process. Technol. 39, 199–217 (1994).

    Article  Google Scholar 

  18. 18

    Raison, R. J., Khanna, P. K. & Woods, P. V. Mechanisms of element transfer to the atmosphere during vegetation fires. Can. J. Forest Res. 15, 132–140 (1985).

    Article  Google Scholar 

  19. 19

    Cotton, F. A. & Wilkinson, G. Advanced Inorganic Chemistry: A Comprehensive Text 3rd edn, 381–383 (Interscience Publishers, 1972).

    Google Scholar 

  20. 20

    Beck, J. et al. The behaviour of phosphorus in flue gases from coal and secondary fuel co-combustion. Fuel 84, 1911–1919 (2005).

    Article  Google Scholar 

  21. 21

    Smith, R. et al. Characterization and formation of submicron particles in coal-fired plants. Atmos. Environ. 13, 607–617 (1979).

    Article  Google Scholar 

  22. 22

    Mamane, Y. et al. Characterization of individual fly ash particles emitted from coal-and oil-fire power plants. Atmos. Environ. 20, 2125–2135 (1986).

    Article  Google Scholar 

  23. 23

    Olmez, I. et al. Compositions of particles from selected sources in Philadelphia for receptor modeling applications. J. Air Pollut. Control Assoc. 38, 1392–1402 (1988).

    Google Scholar 

  24. 24

    Mahowald, N. et al. Observed 20th century desert dust variability: Impact on climate and biogeochemistry. Atmos. Chem. Phys. 10, 10875–10893 (2010).

    Article  Google Scholar 

  25. 25

    Neff, J. C. et al. Increasing eolian dust deposition in the western United States linked to human activity. Nature Geosci. 1, 189–195 (2008).

    Article  Google Scholar 

  26. 26

    McDowell, R. W. & Sharpley, A. N. Atmospheric deposition contributes little nutrient and sediment to stream flow from an agricultural watershed. Agric. Ecosyst. Environ. 134, 19–23 (2009).

    Article  Google Scholar 

  27. 27

    Lamarque, J. F. et al. Historical (1850-2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: Methodology and application. Atmos. Chem. Phys. 10, 7017–7039 (2010).

    Article  Google Scholar 

  28. 28

    Monks, P. S. et al. Atmospheric composition change–global and regional air quality. Atmos. Environ. 43, 5268–5350 (2009).

    Article  Google Scholar 

  29. 29

    Shindell, D. et al. Simultaneously mitigating near-term climate change and improving human health and food security. Science 335, 183–189 (2012).

    Article  Google Scholar 

  30. 30

    Mahowald, N. Aerosol indirect effect on biogeochemical cycles and climate. Science 334, 794–796 (2011).

    Article  Google Scholar 

  31. 31

    Wang, R. et al. High resolution mapping of combustion processes and implications for CO2 emissions. Atmos. Chem. Phys. 13, 5189–5203 (2013).

    Article  Google Scholar 

  32. 32

    Van der Werf, G. R. et al. Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997–2009). Atmos. Chem. Phys. 10, 11707–11735 (2010).

    Article  Google Scholar 

  33. 33

    Schultz, M. G. et al. Global wildland fire emissions from 1960 to 2000. Glob. Biogeochem. Cycles 22, GB2002 (2008).

    Article  Google Scholar 

  34. 34

    Wang, R. et al. Trend in Global Black Carbon Emissions from 1960 to 2007. Environ. Sci. Technol. 48, 6780–6787 (2014).

    Article  Google Scholar 

  35. 35

    Wang, R. et al. Black carbon emissions in China from 1949 to 2050. Environ. Sci. Technol. 46, 7595–7603 (2012).

    Article  Google Scholar 

  36. 36

    Wang, R. et al. Exposure to ambient black carbon derived from a unique inventory and high resolution model. Proc. Natl Acad. Sci. USA 111, 2459–2463 (2014).

    Article  Google Scholar 

  37. 37

    Balkanski, Y. et al. Direct radiative effect of aerosols emitted by transport: From road, shipping and aviation. Atmos. Chem. Phys. 10, 4477–4489 (2010).

    Article  Google Scholar 

  38. 38

    Jaenicke, R. Abundance of cellular material and proteins in the atmosphere. Science 308, 73 (2005).

    Article  Google Scholar 

  39. 39

    Andres, R. J. & Kasgnoc, A. D. A time-averaged inventory of subaerial volcanic sulfur emissions. J. Geophys. Res. 103, 251–261 (1998).

    Article  Google Scholar 

  40. 40

    Bergametti, G. et al. A mesoscale study of the composition of aerosols emitted from Mt. Etna Volcano. Bull. Volcanol. 47, 1107–1114 (1984).

    Article  Google Scholar 

  41. 41

    Sansone, F. et al. Geochemistry of atmospheric aerosols generated from lava-seawater interactions. Geophys. Res. Lett. 29, 49-1–49-4 (2002).

    Article  Google Scholar 

  42. 42

    Han, C. et al. Free atmospheric phosphine concentrations and fluxes in different wetland ecosystems, China. Environ. Pollut. 159, 630–635 (2011).

    Article  Google Scholar 

  43. 43

    Devai, I. & DeLaune, R. D. Evidence for phosphine production and emission from Louisiana and Florida marsh soils. Org. Geochem. 23, 277–279 (1995).

    Article  Google Scholar 

  44. 44

    Han, S. H. et al. Phosphorus cycling through phosphine in paddy fields. Sci. Total Environ. 258, 195–203 (2000).

    Article  Google Scholar 

  45. 45

    Aselmann, I. & Crutzen, P. J. Global distribution of natural freshwater wetlands and rice paddies, their net primary productivity, seasonality and possible methane emissions. J. Atmos. Chem. 8, 307–358 (1989).

    Article  Google Scholar 

  46. 46

    Schumann, U. & Huntrieser, H. The global lightning-induced nitrogen oxides source. Atmos. Chem. Phys. 7, 3823–3907 (2007).

    Article  Google Scholar 

  47. 47

    Granier, C. et al. Evolution of anthropogenic and biomass burning emissions of air pollutants at global and regional scales during the 1980–2010 period. Climatic Change 109, 163–190 (2011).

    Article  Google Scholar 

  48. 48

    Price, C. G., Penner, J. E. & Prather, M. J. NOx from lightning, Part I: Global distribution based on lightning physics. J. Geophys. Res. 102, 5229–5241 (1997).

    Google Scholar 

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The authors thank Ether/ECCAD for distribution of emission data used in this study. We thank B. G. Li, F. Zhou, W. M. Hao, Y. Ying and M. McGrath for discussions, and J. Gash for editing the English. R.W. was supported by the ‘FABIO’ project, a Marie Curie International Incoming Fellowship from the European Commission. This work was also conducted as part of the ‘IMBALANCE-P’ project of the European Research Council (ERC-2013-SyG-610028). S.T. was supported by the National Nature Science Foundation of China (41390240, 41130754) and the 111 Program (B14001). Some of the computations were performed using HPC resources from GENCI-TGCC (grant 2014-t2014012201).

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R.W. designed the research, performed all calculations and analysed the uncertainties. All authors took part in interpreting the results and writing the paper.

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Correspondence to Rong Wang.

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Wang, R., Balkanski, Y., Boucher, O. et al. Significant contribution of combustion-related emissions to the atmospheric phosphorus budget. Nature Geosci 8, 48–54 (2015).

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