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A Diurnal Carbon Engine Explains 13C-Enriched Carbonates

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A Diurnal Carbon Engine Explains 13C-Enriched Carbonates A diurnal carbon engine explains 13C-enriched carbonates without increasing the global production of oxygen Emily C. Geymana,1 and Adam C. Maloofa aDepartment of Geosciences, Princeton University, Princeton, NJ 08544 Edited by Donald E. Canfield, Institute of Biology and Nordic Center for Earth Evolution, University of Southern Denmark, Odense M., Denmark, and approved October 8, 2019 (received for review May 21, 2019) In the past 3 billion years, significant volumes of carbonate processes can be constrained by visualizing the carbon evolution with high carbon-isotopic (δ13C) values accumulated on shallow of banktop seawater in a Deffeyes diagram (9) (Fig. 2B), since continental shelves. These deposits frequently are interpreted each mechanism induces a characteristic change in DIC and total as records of elevated global organic carbon burial. However, alkalinity (TA) (Table 1). Observations of TOC (5) and DIC vs. through the stoichiometry of primary production, organic carbon TA (7) from the GBB constrain the relative sizes of the net car- burial releases a proportional amount of O2, predicting unrealis- bonate, gas-exchange, and organic fluxes to be 62, 37, and <1%, tic rises in atmospheric pO2 during the 1 to 100 million year-long respectively (Fig. 2). Although the net burial of organic matter positive δ13C excursions that punctuate the geological record. is close to zero, the flux of carbon between organic matter and This carbon–oxygen paradox assumes that the δ13C of shallow the DIC pool over the course of a single diurnal (24-h) cycle water carbonates reflects the δ13C of global seawater-dissolved can exceed the gross atmospheric and carbonate fluxes by over inorganic carbon (DIC). However, the δ13C of modern shallow- a factor of 20 in shallow carbonate environments (12–15). In water carbonate sediment is higher than expected for calcite other words, photosynthesis drives substantial perturbations to or aragonite precipitating from seawater. We explain elevated the carbonate system during the day, but respiration covers up δ13C in shallow carbonates with a diurnal carbon cycle engine, the tracks each night. where daily transfer of carbon between organic and inorganic The diurnal cycle of photosynthesis and respiration per- 13 EARTH, ATMOSPHERIC, AND PLANETARY SCIENCES reservoirs forces coupled changes in carbonate saturation (ΩA) mits a δ C hysteresis (Fig. 3). As the sun rises, photo- and δ13C of DIC. This engine maintains a carbon-cycle hystere- synthesis consumes CO2 from the water column, driving up sis that is most amplified in shallow, sluggishly mixed waters ΩA. The maximum rate of carbonate precipitation (a func- with high rates of photosynthesis, and provides a simple mecha- tion of ΩA) is achieved as peak photosynthesis increases the 13 nism for the observed δ13C-decoupling between global seawater δ C of residual DIC, leading to carbonate sediment enriched 13 13 DIC and shallow carbonate, without burying organic matter or in C. As night falls, aerobic respiration lowers the δ C of DIC but also depresses ΩA, preventing significant car- generating O2. bonate production recording the low δ13C values. The net carbonates j carbon isotopes j chemostratigraphy j paleoclimate effect of this diurnal carbon cycle hysteresis is to produce a shallow carbonate sediment record that has δ13C higher than predicted for aragonite in equilibrium with average local ndros Island (Great Bahama Bank [GBB]), San Salvador seawater DIC. A(Bahamas), and Shark Bay (Western Australia) represent a wide range of seawater residence times and salinities, but all produce carbonate sediment ∼ 5 higher than the δ13C Significance values of open marine waters (Fig. 1).h Carbon-isotope enrich- ment factors for bicarbonate to inorganic calcite (∼ 1:1 ) We present stable carbon isotope (δ13C) data from modern and aragonite (∼ 2:7 ) are relatively insensitive to tempera-h carbonate sediment that require a decoupling of the carbon ture and precipitationh rate (1, 2) and only explain half of the cycles in the global ocean versus shallow carbonate shelves. elevated δ13C signal observed in these shallow carbonate sed- This realization is important because, for the first 97% of iments. The most common explanation for the production of Earth history, many inferences about global paleoclimate and high δ13C carbonate on a global (3) or local (4) scale involves seawater chemistry rely on interpretations of shallow carbon- increasing the export/burial of organic carbon relative to car- ates. We use modern observations and a simple model to bonate in order to leave the residual waters (from which car- show how ordinary diurnal carbon cycling in shallow waters bonates are precipitated) enriched in 13C. However, carbonate is sufficient to produce anomalously positive δ13C on shelves sediments on the GBB have low total organic carbon (TOC) today, and in the geological record. Our results alleviate the (∼0.3%) (5). Thus, the canonical organic burial explanation need to interpret positive δ13C excursions in the geologi- would require wholesale export of organic carbon off the shelf cal record as global reorganizations of the carbon cycle and without depleting nutrients. However, carbonates produced on instead link δ13C to local and/or global paleoenvironmental the GBB and exported to the periplatformal slope (6) also have and paleoecological controls. low TOC (5), refuting the idea of significant organic-carbon export. We propose an alternative mechanism whereby pho- Author contributions: E.C.G. and A.C.M. designed research, performed research, tosynthesis still drives high δ13C in shallow carbonates, even analyzed data, and wrote the paper.y if all of the organic matter produced each day is respired at The authors declare no competing interest.y night, such that net organic-matter burial and nutrient depletion This article is a PNAS Direct Submission. y is zero. Published under the PNAS license.y On shallow banks, the 3 most important mechanisms for 1 To whom correspondence may be addressed. Email: [email protected] exchanging carbon into and out of the DIC pool are 1) carbon- This article contains supporting information online at https://www.pnas.org/lookup/suppl/ ate precipitation/dissolution, 2) atmospheric gas exchange, and doi:10.1073/pnas.1908783116/-/DCSupplemental.y 3) photosynthesis/respiration. The relative contributions of these First published November 8, 2019. www.pnas.org/cgi/doi/10.1073/pnas.1908783116 PNAS j December 3, 2019 j vol. 116 j no. 49 j 24433–24439 Downloaded by guest on September 27, 2021 Fig. 1. Evidence in support of a diurnal organic car- A bon engine driving elevated δ13C in shallow carbon- ates. (A) Three modern carbonate shelves produce bulk sediment with δ13C that is too high to have pre- cipitated directly from open marine waters. (B) The δ13C values of GBB sediments rise abruptly near the shelf edge and remain high (>4.5 ) in the bank interior. The number of samples ish denoted as this study/ref. 4 (1,159/167), and the banktop water ages in B are computed from a spatial interpolation of the 14C ages in ref. 7 (Fig. 2). The diurnal organic carbon engine hypothesis predicts a number of observa- tions consistent with the dataset: 1 peak δ13C of DIC should be high enough to precipitate aragonite with the dominant value of δ13C∼ 5 ; 2 1.8 vari- ability in DIC is the same range predictedh h during B one diurnal photosynthesis–respiration cycle (Fig. 3); 3 banktop waters have a δ13C of DIC composition roughly equal to or higher than that of offshore waters; 4 sediments at the shelf edge have low δ13C, consistent with open marine DIC; 5 the rapid rise in sediment δ13C near the platform edge cap- tures the transition from the weak photosynthetic forcing (κp) characteristic of the open ocean to the strong photosynthetic forcing observed in shallow waters (Fig. 4); and 6 the lack of a significant cross- shelf δ13C gradient reflects the balancing isotopic effects of carbonate precipitation (depletes resid- ual DIC) and CO2 gas escape (enriches residual DIC) (Fig. 7). Carbon Model diurnal engine returns 100% of the carbon sequestered in organic To quantify the extent to which the temporal coupling between matter during the day back to the seawater each night (Fig. 3). photosynthesis and carbonate precipitation increases the δ13C of The only prescribed forcing in the engine model is the daily pho- carbonate, we develop a simple mass balance model of the diur- tosynthetic transfer of carbon between the inorganic and organic nal carbon engine (Fig. 3). To emphasize how the diurnal engine reservoirs (κp ). The gas exchange and carbonate fluxes are com- mechanism is distinct from the canonical treatment whereby net puted independently based on values of pCO2 and ΩA obtained primary production drives elevated δ13C in carbonates (3, 4), our in each time step using the carbonate-system calculation software 250 A Broecker & Takahashi (1966) C 37% B 26.0 14 C banktop water ages Eq/kg) Atm. Depth (m) 200 TA ( CaCO3 2000 Corg 25.6 -5 62% < 1%5 20 6 22 6 150 48 10 8 1800 0 = 6 12 A 71 5 25.2 100 56 1600 -10 4 73 66 Banktop water age (days) 96 56 3 Broecker & Takahashi (1966) 133 50 255 1400 (aragonite) 24.8 245 142 180 Atm. equilibrium: m = 1.26 150 1 Linear fit: m = 1.24 -15 0 -79.0 -78.6 -78.2 -77.8 1000 1200 1400 1600 1800 2000 CO ( mol/kg) 2 14 Fig. 2. Measurements of C, ΣCO2, and TA in seawater from the GBB (7) help to constrain the carbon fluxes in our model (Fig. 3). (A) Shallow waters and sluggish mixing on the GBB afford banktop residence times >250 days. Bathymetry from ref. 8. (B) ΣCO2 and TA measurements produce a slope of m = 1.24 in the Deffeyes diagram (9) (Fig.
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