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Abstract Lithium isotope ratios (δ7Li) of rivers are increasingly serving as a diagnostic of the balance between chemical and physical weathering contributions to overall landscape denudation rates. Here, we show that intermediate weathering intensities and highly enriched stream δ7Li values typically associated with lowland floodplains can also describe small upland watersheds subject to cool, wet climates. This behavior is revealed by stream δ7Li between +22.4 and +23.5‰ within a Critical Zone observatory located in the Cévennes region of southern France, where dilute stream solute concentrations and significant atmospheric deposition otherwise mask evidence of incongruence. The water‐rock reaction pathways underlying this behavior are quantified through a multicomponent, isotope‐enabled reactive transport model. Using geochemical characterization of soil profiles, bedrock, and long‐term stream samples as constraints, we evolve the simulation from an initially unweathered granite to a steady state weathering profile which reflects the balance between (a) fluid infiltration and drainage and (b) bedrock uplift and soil erosion. Enriched stream δ7Li occurs because Li is strongly incorporated into actively precipitating secondary clay phases beyond what prior laboratory experiments have suggested. Chemical weathering incongruence is maintained despite relatively slow reaction rates and moderate clay accumulation due to a combination of two factors. First, reactive primary mineral phases persist across the weathering profile and effectively “shield” the secondary clays from resolubilization due to their greater solubility. Second, the clays accumulating in the near‐surface profile are relatively mature weathering byproducts. These factors promote characteristically low total dissolved solute export from the catchment despite significant input of exogenous dust.
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Competition or collaboration: Clay formation sets the relationship between silicate weathering and organic carbon burial in soil
Silicate weathering and organic carbon (OC) burial in soil regulate atmospheric CO2, but their influence on each other remains unclear. Generally, OC oxidation can generate acids that drive silicate weathering, yet clay minerals that form during weathering can protect OC and limit oxidation. This poses a conundrum where clay formation and OC preservation either compete or cooperate. Debate remains about their relative contributions because quantitative tools to simultaneously probe these processes are lacking while those that exist are often not measured in concert. Here we demonstrate that Li isotope ratios of sediment, commonly used to trace clay formation, can help constrain OC cycling. Measurements of river suspended sediment from two watersheds of varying physiography and analysis of published data from Hawaii soil profiles show negative correlations between solid-phase d7Li values and OC content, indicating the association of clay mineral formation with OC accumulation. Yet, the localities differ in their ranges of d7Li values and OC contents, which we interpret with a model of soil formation. We find that temporal trends of Li isotopes and OC are most sensitive to mineral dissolution/clay formation rates, where higher rates yield greater OC stocks and lower d7Li values. Whereas OC-enhanced dissolution primarily dictates turnover times of OC and silicate minerals, clay protection distinctly modifies soil formation pathways and is likely required to explain the range of observations. These findings underscore clay mineral formation, driven primarily by bedrock chemistry and secondarily by climate, as a principal modulator of weathering fluxes and OC accumulation in soil.
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- PAR ID:
- 10490453
- Publisher / Repository:
- Elsevier
- Date Published:
- Journal Name:
- Earth and Planetary Science Letters
- Volume:
- 628
- Issue:
- C
- ISSN:
- 0012-821X
- Page Range / eLocation ID:
- 118584
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1016/j.epsl.2024.118584
