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Temperature control on CO2 emissions from the weathering of sedimentary rocks

Nature Geoscience volume 14, pages 665–671 (2021)Cite this article

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Abstract

Sedimentary rocks can release carbon dioxide (CO2) during the weathering of rock organic carbon and sulfide minerals. This sedimentary carbon could act as a feedback on Earth’s climate over millennial to geological timescales, yet the environmental controls on the CO2 release from rocks are poorly constrained. Here, we directly measure CO2 flux from weathering of sedimentary rocks over 2.5 years at the Draix-Bléone Critical Zone Observatory, France. Total CO2 fluxes approached values reported for soil respiration, with radiocarbon analysis confirming the CO2 source from rock organic carbon and carbonate. The measured CO2 fluxes varied seasonally, with summer fluxes five times larger than winter fluxes, and were positively correlated with temperature. The CO2 release from rock organic carbon oxidation increased by a factor of 2.2 when temperature increased by 10 °C. This temperature sensitivity is similar to that of degradation of recent-plant-derived organic matter in soils. Our flux measurements identify sedimentary-rock weathering as a positive feedback to warming, which may have operated throughout Earth’s history to force the surface carbon cycle.

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Fig. 1: The Laval field site.
Fig. 2: The source of CO2 sampled from chambers H4 and H6 on the basis of its isotopic composition.
Fig. 3: Measured total CO2 emissions from rock weathering in the Laval catchment for 2.5 years from late December 2016 to early May 2019.
Fig. 4: Temperature sensitivity of total CO2 release by sedimentary-rock weathering.
Fig. 5: Variability in the total CO2 emissions compared with the elevation of the rock chambers above the Laval river bed.

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Data availability

All data that support the findings of this study are available from the Natural Environment Research Council (NERC)—British Geological Survey (BGS) National Geoscience Data Centre with the identifier https://doi.org/10.5285/efc082aa-5c2b-4afb-aec8-344aebaea653. Source data are provided with this paper.

Code availability

Custom Matlab codes and accompanying \({p_{{\rm{CO}}_2}}\) source data are available on request from the corresponding authors.

References

  1. Sundquist, E. T. & Visser, K. in Treatise on Geochemistry (eds Holland, H. D. & Turekian, K. K.) 425–472 (Elsevier, 2003).

  2. Petsch, S. T., Berner, R. A. & Eglinton, T. I. A field study of the chemical weathering of ancient sedimentary organic matter. Org. Geochem. 31, 475–487 (2000).

    Article  Google Scholar 

  3. Hilton, R. G. & West, A. J. Mountains, erosion and the carbon cycle. Nat. Rev. Earth Environ. 1, 284–299 (2020).

    Article  Google Scholar 

  4. Keller, C. K. & Bacon, D. H. Soil respiration and georespiration distinguished by transport analyses of vadose CO2, 13CO2, and 14CO2. Glob. Biogeochem. Cycles 12, 361–372 (1998).

    Article  Google Scholar 

  5. Berner, R. A. & Canfield, D. E. A new model for atmospheric oxygen over Phanerozoic time. Am. J. Sci. 289, 333–361 (1989).

    Article  Google Scholar 

  6. Spence, J. & Telmer, K. The role of sulfur in chemical weathering and atmospheric CO2 fluxes: evidence from major ions, δ13CDIC, and δ34SSO4 in rivers of the Canadian Cordillera. Geochim. Cosmochim. Acta 69, 5441–5458 (2005).

    Article  Google Scholar 

  7. Calmels, D., Gaillardet, J., Brenot, A. & France-Lanord, C. Sustained sulfide oxidation by physical erosion processes in the Mackenzie River basin: climatic perspectives. Geology 35, 1003–1006 (2007).

    Article  Google Scholar 

  8. Torres, M. A., West, A. J. & Li, G. Sulphide oxidation and carbonate dissolution as a source of CO2 over geological timescales. Nature 507, 346–349 (2014).

    Article  Google Scholar 

  9. Berner, E. K. & Berner, R. A. Global Environment: Water, Air, and Geochemical Cycles 2nd edn (Princeton Univ. Press, 2012).

  10. Hartmann, J. & Moosdorf, N. The new global lithological map database GLiM: a representation of rock properties at the Earth surface. Geochem. Geophys. Geosyst. 13, Q12004 (2012).

    Article  Google Scholar 

  11. Copard, Y., Amiotte-Suchet, P. & Di-Giovanni, C. Storage and release of fossil organic carbon related to weathering of sedimentary rocks. Earth Planet. Sci. Lett. 258, 345–357 (2007).

    Article  Google Scholar 

  12. Petsch, S. T. in Treatise on Geochemistry 2nd edn (eds Holland, H. D. & Turekian, K. K.) 217–238 (Elsevier, 2014).

  13. Burke, A. et al. Sulfur isotopes in rivers: insights into global weathering budgets, pyrite oxidation, and the modern sulfur cycle. Earth Planet. Sci. Lett. 496, 168–177 (2018).

    Article  Google Scholar 

  14. Plank, T. & Manning, C. E. Subducting carbon. Nature 574, 343–352 (2019).

    Article  Google Scholar 

  15. Hedges, J. I. & Keil, R. G. Sedimentary organic matter preservation: an assessment and speculative synthesis. Mar. Chem. 49, 81–115 (1995).

    Article  Google Scholar 

  16. Torres, M. A., Moosdorf, N., Hartmann, J., Adkins, J. F. & West, A. J. Glacial weathering, sulfide oxidation, and global carbon cycle feedbacks. Proc. Natl Acad. Sci. USA 114, 8716–8721 (2017).

    Article  Google Scholar 

  17. Hilton, R. G., Gaillardet, J., Calmels, D. & Birck, J. L. Geological respiration of a mountain belt revealed by the trace element rhenium. Earth Planet. Sci. Lett. 403, 27–36 (2014).

    Article  Google Scholar 

  18. Horan, K. et al. Mountain glaciation drives rapid oxidation of rock-bound organic carbon. Sci. Adv. 3, e1701107 (2017).

    Article  Google Scholar 

  19. Bufe, A. et al. Co-variation of silicate, carbonate and sulfide weathering drives CO2 release with erosion. Nat. Geosci. 14, 211–216 (2021).

    Article  Google Scholar 

  20. Crawford, J. T., Hinckley, E.-L. S., Litaor, M. I., Brahney, J. & Neff, J. C. Evidence for accelerated weathering and sulfate export in high Alpine environments. Environ. Res. Lett. 14, 124092 (2019).

    Article  Google Scholar 

  21. Soulet, G. et al. Technical note: in situ measurement of flux and isotopic composition of CO2 released during oxidative weathering of sedimentary rocks. Biogeosciences 15, 4087–4102 (2018).

    Article  Google Scholar 

  22. Mathys, N., Brochot, S., Meunier, M. & Richard, D. Erosion quantification in the small marly experimental catchments of Draix (Alpes de Haute Provence, France). Calibration of the ETC rainfall–runoff–erosion model. Catena 50, 527–548 (2003).

    Article  Google Scholar 

  23. Gaillardet, J. et al. OZCAR: the French network of critical zone observatories. Vadose Zone J. https://doi.org/10.2136/vzj2018.04.0067 (2018).

  24. Cras, A., Marc, V. & Travi, Y. Hydrological behaviour of sub-Mediterranean Alpine headwater streams in a badlands environment. J. Hydrol. 339, 130–144 (2007).

    Article  Google Scholar 

  25. Graz, Y. et al. Annual fossil organic carbon delivery due to mechanical and chemical weathering of marly badlands areas. Earth Surf. Process. Landf. 37, 1263–1271 (2012).

    Article  Google Scholar 

  26. Maquaire, O. et al. Caractérisation des profils de formations superficielles par pénétrométrie dynamique à énergie variable: application aux marnes noires de Draix (Alpes-de-Haute-Provence, France). Comptes Rendus Geosci. 334, 835–841 (2002).

    Article  Google Scholar 

  27. Lofi, J. et al. Geological discontinuities, main flow path and chemical alteration in a marly hill prone to slope instability: assessment from petrophysical measurements and borehole image analysis. Hydrol. Process. 26, 2071–2084 (2012).

    Article  Google Scholar 

  28. Husson, J. M. & Peters, S. E. Atmospheric oxygenation driven by unsteady growth of the continental sedimentary reservoir. Earth Planet. Sci. Lett. 460, 68–75 (2017).

    Article  Google Scholar 

  29. Copard, Y., Di-Giovanni, C., Martaud, T., Albéric, P. & Olivier, J.-E. Using Rock-Eval 6 pyrolysis for tracking fossil organic carbon in modern environments: implications for the roles of erosion and weathering. Earth Surf. Process. Landf. 31, 135–153 (2006).

    Article  Google Scholar 

  30. Oertel, C., Matschullat, J., Zurba, K., Zimmermann, F. & Erasmi, S. Greenhouse gas emissions from soils—a review. Geochemistry 76, 327–352 (2016).

    Article  Google Scholar 

  31. Winnick, M. J. et al. Snowmelt controls on concentration–discharge relationships and the balance of oxidative and acid–base weathering fluxes in an Alpine catchment, East River, Colorado. Water Resour. Res. 53, 2507–2523 (2017).

    Article  Google Scholar 

  32. Tune, A. K., Druhan, J. L., Wang, J., Bennett, P. C. & Rempe, D. M. Carbon dioxide production in bedrock beneath soils substantially contributes to forest carbon cycling. J. Geophys. Res. Biogeosci. 125, e2020JG005795 (2020).

    Article  Google Scholar 

  33. Feng, G., Wu, L. & Letey, J. Evaluating aeration criteria by simultaneous measurement of oxygen diffusion rate and soil-water regime. Soil Sci. 167, 495–503 (2002).

    Article  Google Scholar 

  34. Brantley, S. L., Holleran, M. E., Jin, L. & Bazilevskaya, E. Probing deep weathering in the Shale Hills Critical Zone Observatory, Pennsylvania (USA): the hypothesis of nested chemical reaction fronts in the subsurface. Earth Surf. Process. Landf. 38, 1280–1298 (2013).

    Article  Google Scholar 

  35. Duvert, C., Butman, D. E., Marx, A., Ribolzi, O. & Hutley, L. B. CO2 evasion along streams driven by groundwater inputs and geomorphic controls. Nat. Geosci. 11, 813–818 (2018).

    Article  Google Scholar 

  36. Mallet, F. et al. Assessing soil water content variation in a small mountainous catchment over different time scales and land covers using geographical variables. J. Hydrol. 591, 125593 (2020).

    Article  Google Scholar 

  37. Hicks Pries, C. E., Castanha, C., Porras, R. C. & Torn, M. S. The whole-soil carbon flux in response to warming. Science 355, 1420–1423 (2017).

    Article  Google Scholar 

  38. Bond-Lamberty, B. & Thomson, A. A global database of soil respiration data. Biogeosciences 7, 1915–1926 (2010).

    Article  Google Scholar 

  39. Nicholson, R. V., Gillham, R. W. & Reardon, E. J. Pyrite oxidation in carbonate-buffered solution: 1. Experimental kinetics. Geochim. Cosmochim. Acta 52, 1077–1085 (1988).

    Article  Google Scholar 

  40. Percak-Dennett, E. et al. Microbial acceleration of aerobic pyrite oxidation at circumneutral pH. Geobiology 15, 690–703 (2017).

    Article  Google Scholar 

  41. Raich, J. W. & Schlesinger, W. H. The global carbon dioxide flux in soil respiration and its relationship to vegetation and climate. Tellus B 44, 81–99 (1992).

    Article  Google Scholar 

  42. Hemingway, J. D. et al. Microbial oxidation of lithospheric organic carbon in rapidly eroding tropical mountain soils. Science 360, 209–212 (2018).

    Article  Google Scholar 

  43. Petsch, S. T., Eglinton, T. I. & Edwards, K. J. 14C-dead living biomass: evidence for microbial assimilation of ancient organic carbon during shale weathering. Science 292, 1127–1131 (2001).

    Article  Google Scholar 

  44. Leifeld, J. & von Lützow, M. Chemical and microbial activation energies of soil organic matter decomposition. Biol. Fertil. Soils 50, 147–153 (2014).

    Article  Google Scholar 

  45. Maher, K. & Chamberlain, C. P. Hydrologic regulation of chemical weathering and the geologic carbon cycle. Science 343, 1502–1504 (2014).

    Article  Google Scholar 

  46. Li, G. et al. Temperature dependence of basalt weathering. Earth Planet. Sci. Lett. 443, 59–69 (2016).

    Article  Google Scholar 

  47. Galy, V., Beyssac, O., France-Lanord, C. & Eglinton, T. Recycling of graphite during Himalayan erosion: a geological stabilization of carbon in the crust. Science 322, 943–945 (2008).

    Article  Google Scholar 

  48. Gu, X., Heaney, P. J., Reis, F. D. A. A. & Brantley, S. L. Deep abiotic weathering of pyrite. Science 370, eabb8092 (2020).

    Article  Google Scholar 

  49. Jin, L. et al. The CO2 consumption potential during gray shale weathering: insights from the evolution of carbon isotopes in the Susquehanna Shale Hills critical zone observatory. Geochim. Cosmochim. Acta 142, 260–280 (2014).

    Article  Google Scholar 

  50. Berner, R. A. & Caldeira, K. The need for mass balance and feedback in the geochemical carbon cycle. Geology 25, 955–956 (1997).

    Article  Google Scholar 

  51. Caves Rugenstein, J. K., Ibarra, D. E. & von Blanckenburg, F. Neogene cooling driven by land surface reactivity rather than increased weathering fluxes. Nature 571, 99–102 (2019).

    Article  Google Scholar 

  52. Hardie, S. L. M. L., Garnett, M. H. H., Fallick, A. E., Rowland, A. P. & Ostle, N. J. J. Carbon dioxide capture using a zeolite molecular sieve sampling system for isotopic studies (13C and 14C) of respiration. Radiocarbon 47, 441–451 (2005).

    Article  Google Scholar 

  53. Observatoire hydrosédimentaire de montagne Draix-Bléone (Draix-Bléone Observatory, 2015); https://doi.org/10.17180/obs.draix

  54. Mathys, N. & Klotz, S. Draix: a field laboratory for research on hydrology and erosion in mountain areas. In Proc. 4th Canadian Conference on Geohazards: From Causes to Management (eds Locat, J., Perret, D., Turmel, D., Demers, D. & Leroueil, D.) (Presse de l’Université Laval, Québec, 2008).

  55. Pirk, N. et al. Calculations of automatic chamber flux measurements of methane and carbon dioxide using short time series of concentrations. Biogeosciences 13, 903–912 (2016).

    Article  Google Scholar 

  56. Garnett, M. H. & Murray, C. Processing of CO2 samples collected using zeolite molecular sieve for 14C analysis at the NERC Radiocarbon Facility (East Kilbride, UK). Radiocarbon 55, 410–415 (2013).

    Article  Google Scholar 

  57. Reimer, P. J., Brown, T. A. & Reimer, R. W. Discussion: reporting and calibration of post-bomb 14C data. Radiocarbon 46, 1299–1304 (2004).

    Article  Google Scholar 

  58. Mook, W. G., Bommerson, J. C. & Staverman, W. H. Carbon isotope fractionation between dissolved bicarbonate and gaseous carbon dioxide. Earth Planet. Sci. Lett. 22, 169–176 (1974).

    Article  Google Scholar 

  59. Tipper, E. T. et al. The short term climatic sensitivity of carbonate and silicate weathering fluxes: insight from seasonal variations in river chemistry. Geochim. Cosmochim. Acta 70, 2737–2754 (2006).

    Article  Google Scholar 

  60. Marc, V. et al. Groundwater–surface waters interactions at slope and catchment scales: implications for landsliding in clay-rich slopes. Hydrol. Process. 31, 364–381 (2017).

    Article  Google Scholar 

Download references

Acknowledgements

This research was funded by a European Research Council Starting Grant to R.G.H. (ROC-CO2 project, grant 678779). Radiocarbon measurements were funded by the Natural Environment Research Council (NERC), UK (allocation 2074.1017) to G.S., R.G.H. and M.H.G. We thank staff at NERC RCF and SUERC. We thank C. Flaux and A.-E. Paquier for field assistance in December 2016. This study was carried out in Draix-Bléone Observatory (France) and used its infrastructure and temperature and river discharge data. Draix-Bléone Observatory is funded by INRAE, INSU and OSUG, and is part of OZCAR Research Infrastructure, which is supported by the French Ministry of Research, French Research Institutions and Universities.

Author information

Author notes

  1. Guillaume Soulet

    Present address: Ifremer, GM, Plouzané, France

  2. Robert G. Hilton

    Present address: Department of Earth Sciences, University of Oxford, Oxford, UK

Authors and Affiliations

  1. Department of Geography, Durham University, Durham, UK

    Guillaume Soulet, Robert G. Hilton, Tobias Roylands, Thomas Croissant & Mathieu Dellinger

  2. NEIF Radiocarbon Laboratory, Glasgow, UK

    Mark H. Garnett

  3. Univ. Grenoble Alpes, INRAE, UR ETNA, Saint-Martin-d’Hères, France

    Sébastien Klotz & Caroline Le Bouteiller

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  1. Guillaume Soulet
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Contributions

R.G.H. conceived the research and designed the study with G.S. G.S. and S.K. built and maintained the chambers. G.S. and R.G.H. carried out fieldwork with additional assistance from T.R., T.C. and M.D. G.S. led the CO2 flux measurements and all related calculations and analysis. S.K. collected and provided field temperature data, discharge and precipitation data. M.H.G. provided materials for sampling CO2 for isotopic analyses. G.S. and M.H.G. carried out geochemical analyses. G.S. and R.G.H. analysed the results. G.S. and R.G.H. wrote the paper with inputs from all co-authors.

Corresponding authors

Correspondence to Guillaume Soulet or Robert G. Hilton.

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The authors declare no competing interest.

Additional information

Peer review information Nature Geoscience thanks Louis Derry, Aaron Bufe and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Rebecca Neely, in collaboration with the Nature Geoscience team.

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Extended data

Extended Data Fig. 1 CO2 emissions measured in the Laval catchment (Draix, France) compared to respiration CO2 flux in various soil types.

CO2 emissions measured in the Laval catchment (Draix, France) (red square; Supplementary Table 4) compared to respiration CO2 flux in various soil types (black hyphens). Median values are shown with the symbols, the minimum-maximum range is indicated with solid lines. As maximum value for cropland exceeds the scale of the y-axis, upper part of the cropland range is dashed and maximum value is indicated. The respiration soil compilation is from ref. 30. Note that the CO2 emission from oxidative weathering of sedimentary rocks in the Laval catchment reaches the magnitude of the CO2 emissions from respiration of all type of soils.

Source data

Extended Data Fig. 2 Temperature and hydrological controls on the CO2 emissions measured in the Laval catchment (Draix, France) in April-May 2019.

Temperature and hydrological controls on total CO2 emissions recorded in chambers H4 and H6 for one month from 10/04/2019 to 10/05/2019. Upper panel: Daily temperature average (black line) and amplitude (grey envelope) in the rock interior. Lower panels: CO2 flux measured in chamber H4 (pink circles) and H6 (green circles). Error bars indicate standard deviation on the flux measurements (Methods) when larger than the symbol size. Circles with a black dot inside denotes CO2 flux measurements performed in average 17 hours (15 to 19 hours) after a rainfall event. The rain events are visible as sharp peaks in the water discharge recorded in the Laval catchment (blue envelope).

Source data

Extended Data Fig. 3 Climate of the Laval catchment (Draix, France) from December 2016 to May 2019.

Climate of the Laval catchment (Draix, France) for two and a half years from December 2016 to May 2019 (study period). Monthly rain precipitation (bars) is compared to the monthly temperature average (red line). Drought periods are represented by the orange bars. Rainfall monitoring in the Laval catchment started in 1982. 2017 was the driest year ever recorded in the Laval catchment (annual precipitation 627 mm), whereas 2018 was the wettest (1327 mm), and 2019 the second wettest (1263 mm). Note the 4 month-long drought from July to October 2017. The climatic diagram shows the highly seasonal pattern of the air temperature in the Laval catchment.

Source data

Extended Data Fig. 4 The near surface water content of the Laval catchment (Draix, France) marls compared to the daily-averaged air temperature.

The near surface water content of the Laval catchment marls at station B3 (red line) and B4 (blue line) and the daily-averaged air temperature (green line) at ‘Le Plateau’ weather station (located ~500 metres from station B3 and B4) from 11/05/2016 to 29/11/2016 (ref. 36). b. The near surface water content at station B3 (red circles) and B4 (blue circles) versus daily-averaged air temperature recorded at the ‘le Plateau’ weather station. c. Box plots showing the variability of the near surface water content of the marls at station B3 (red) and B4 (blue) for the air temperature range -2 to 16 °C and 16 to 24 °C. Box plots show minimum, 25% percentile, median, 75% percentile and maximum values, as well as the mean (dot) and outliers (circles).

Source data

Supplementary information

Supplementary Information

Supplementary Figs. 1 and 2.

Supplementary Data

Supplementary Figs. 1 and 2.

Supplementary Tables

Supplementary Tables 1–4.

Source data

Source Data Fig. 2

Radiocarbon and δ13C values of all analysed samples, including CO2 in chambers H4 and H6, atmospheric CO2 and rock organic and inorganic carbon of chambers H4 and H6.

Source Data Fig. 3

Total CO2 fluxes with dates of measurements and corresponding temperature in the chamber, for chambers H4, H6, H7, H8 and H13.

Source Data Fig. 4

Total CO2 fluxes with dates of measurements and corresponding temperature in the chamber, for chambers H4, H6, H7, H8 and H13.

Source Data Fig. 5

F0 value and minimum, maximum, median, average, 25th and 75th percentiles, and height above river bed for chambers H4, H6, H7, H8 and H13.

Source Data Extended Data Fig. 1

Combined minimum, maximum, median, 25th and 75th percentiles for chambers H4, H6, H7, H8 and H13.

Source Data Extended Data Fig. 2

Total CO2 flux for H4 and H6 with chamber temperature and Laval river-water discharge from 10 April 2019 to 10 May 2019.

Source Data Extended Data Fig. 3

Monthly precipitation and air temperature in the Laval catchment from December 2016 to May 2019.

Source Data Extended Data Fig. 4

Marl water content and air temperature in the Laval catchment from 11 May 2016 to 29 November 2016.

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Soulet, G., Hilton, R.G., Garnett, M.H. et al. Temperature control on CO2 emissions from the weathering of sedimentary rocks. Nat. Geosci. 14, 665–671 (2021). https://doi.org/10.1038/s41561-021-00805-1

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