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Carbonate-rich crust subduction drives the deep carbon and chlorine cycles

Nature volume 620, pages 576–581 (2023)Cite this article

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Abstract

The flux balances of carbon and chlorine between subduction into the deep mantle and volcanic emissions into the atmosphere are crucial for the habitability of our planet1,2. However, pervasive loss of fluids from subducting slabs has been thought to cut off the delivery of both carbon and chlorine to the deep mantle owing to their high mobility under hydrous conditions3,4. Our new high-pressure experiments show that most carbonates (>75 wt%) in carbonate-rich crustal rocks—one of the main subducting carbon reservoirs—survive devolatilization and hydrous melting in cold and warm subduction zones, indicating that their subduction has driven the deep carbon cycle since the Mesoproterozoic. We found that KCl and NaCl, respectively, become stable phases crystallizing from hydrous carbonatite melts with low chlorine solubility in warm and hot subduction zones, resulting in the sequestration of chlorine in the solid residue in downwelling slabs. Accordingly, the subduction of carbonate-rich rocks facilitated highly effective recycling of both chlorine and carbon into the deep mantle at intermediate stages of Earth’s history and led to declining atmospheric pCO2 and the formation of carbon-rich and chlorine-rich mantle reservoirs since the Mesoproterozoic. This period of optimal carbon and chlorine subduction may explain the ages of eclogitic diamonds and the formation of the HIMU mantle source.

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Fig. 1: The hydrous melting of carbonate-rich crustal rocks relative to subduction slab surface geotherms.
Fig. 2: Modal abundances of experimental phases at 5 GPa.
Fig. 3: Key compositional features of experimental minerals and melts.
Fig. 4: Evolution of surface and deep carbon and chlorine controlled by subduction regime through time.

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Data availability

The data that support the findings of this study are available in the paper or in the supplementary files and are also available at https://doi.org/10.6084/m9.figshare.22698292.v1. Source data are provided with this paper.

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Acknowledgements

S.F.F. and C.C. are funded by ARC grant FL180100134 and S.S.S. by Macquarie University support funds for the FL project. M.W.F. is funded by Macquarie University grant MQRF0001074-2020. The Ocean Discovery Project provided the marine limestone and sediment samples. We acknowledge the facilities of the Centre for Advanced Microscopy at the Australian National University, Canberra. We thank Z. Hu and T. He for analysis of Cl contents of the starting materials. We acknowledge I. Ezad for proofreading this manuscript.

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Authors and Affiliations

  1. School of Natural Sciences, Macquarie University, North Ryde, New South Wales, Australia

    Chunfei Chen, Michael W. Förster, Stephen F. Foley & Svyatoslav S. Shcheka

  2. Research School of Earth Sciences, Australian National University, Canberra, Australian Capital Territory, Australia

    Michael W. Förster & Stephen F. Foley

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  1. Chunfei Chen
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Contributions

C.C., M.W.F. and S.F.F. designed the study. C.C. and S.S.S. carried out the experiments. C.C. and M.W.F. performed analytical measurements. C.C. wrote the manuscript and all authors contributed to interpreting data and revising the manuscript.

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Correspondence to Chunfei Chen.

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Extended data figures and tables

Extended Data Fig. 1 The compositions of starting materials in this study compared with previous high-pressure experiments and natural sediments and altered basalts.

a, CO2 and H2O contents of starting materials from this study (CS2, CS1 and CS5) and from previous high-pressure experiments on carbonated sediments26,27,50,60,61 and oceanic crust12,14,62,63,64. The model CaO–Al2O3–SiO2–CO2–H2O system is shown for comparison13. b–f, Chemical compositions of sedimentary columns subducting at global trenches17, the Lesser Antilles sediments from DODP Site 144 (ref. 77), altered oceanic crust18 and starting materials in this study. The global weighted average composition of subducted sediments (GLOSS-II)17 is shown for comparison.

Source data

Extended Data Fig. 2 Representative backscattered electron images of run products at 3 and 4 GPa.

a–c, 3 GPa. d–i, 4 GPa. a,d–e, Subsolidus experiments. b,c,f–i, Above-solidus experiments. Silicate melt at 3 GPa (b,c) and 4 GPa (g). Carbonatite melt at T = 900 °C and 4 GPa (f). KCl at T = 850 °C (h) and both KCl and NaCl at T = 900 °C (i).

Extended Data Fig. 3 Representative backscattered electron images of experimental charges at 5 GPa.

a–c, Subsolidus experiments. d–i, Above-solidus experiments. KCl in carbonatite melt (f) and in the solid residues (g). NaCl in carbonatite melts (h) and in the solid residues (i).

Extended Data Fig. 4 The melting curve of carbonate-rich crustal rocks compared with those of sediments and altered basalt/gabbro.

The solidus of hydrous carbonate-rich sediments (CS2 and CS5) in this study, hydrous carbonate-free silicate sediments75, carbonated basalt/gabbro12 and average sediments26,27. The shaded areas represent the P–T conditions in which carbonatite melts (CbM) are stable.

Extended Data Fig. 5 Variation of the modal abundances of experimental phases at 3 and 4 GPa for CS2.

Source data

Extended Data Fig. 6 The chemical compositions of carbonate-rich phases in the experiments.

The chemical compositions of carbonate precipitated from fluid and of calcite (a) and compositions of silicate and carbonatite melts (b) in this study. Carbonate precipitates and melts from previous experiments on hydrated carbonated gabbro12 and carbonated sediments26,27,50 are shown for comparison. The stability regions of (Mg, Fe)-calcite and siderite–magnesite solid solution are from ref. 78.

Source data

Extended Data Fig. 7 Subduction of carbonate-rich crustal rocks through time.

a, Schematic illustration showing subduction of carbonate-rich crustal rocks and replenishment of carbon and/or chlorine to cratonic mantle roots and deep sources of HIMU-type ocean island basalts (OIBs). Stability of carbonate and chloride during subduction of carbonate-rich crustal rocks influenced by the infiltration of Cl-rich fluid in the cold (b), warm (c) and hot (d) subduction regimes.

Extended Data Fig. 8 The chemical compositions of minerals in the experiments.

Major element chemistry of garnet, jadeite and carbonates showing systematic changes with temperature. Their compositions are independent of the bulk compositions of the starting materials.

Source data

Extended Data Fig. 9 Representative backscattered electron images of the experimental charges in the unpolished halves of capsules.

KCl coexists with other residual minerals as inclusions (a) and coexists with carbonatite melts (b) in the experiment at 950 °C. c, NaCl coexists with carbonatite melts in the experiment at 1,100 °C.

Extended Data Table 1 Conditions and results of experiments on carbonate-rich sediments
Full size table
Extended Data Table 2 The chemical compositions of starting materials and experimental melts
Full size table

Supplementary information

Supplementary Data 1

Compilation of age of eclogitic diamonds constrained by Sm–Nd and Re–Os isochrons for inclusions (n > 2) in diamonds. n = the number of inclusions for the isochron. Note that we compile the isochron ages only when n > 2.

Supplementary Data 2

Major element compositions of phengite, garnet, jadeite, aragonite, (Mg, Fe) calcite, epidote and calcite in the experiments.

Source data

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Chen, C., Förster, M.W., Foley, S.F. et al. Carbonate-rich crust subduction drives the deep carbon and chlorine cycles. Nature 620, 576–581 (2023). https://doi.org/10.1038/s41586-023-06211-4

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