Du, J. ; Haley, B. A. ; Mix, A. C. ; Abbott, A. N. ; McManus, J. ; Vance, D. Reactive-Transport Modeling of Neodymium and Its Radiogenic Isotope in Deep-Sea Sediments: The Roles of Authigenesis, Marine Silicate Weathering and Reverse Weathering.
Earth and Planetary Science Letters 2022,
596, 117792.
访问链接AbstractDissolved Rare Earth Elements (REE) and radiogenic neodymium (Nd) isotope composition (εNd) of seawater are widely used geochemical tools in studying marine processes, but their modern ocean budgets are poorly understood. Recent discoveries of large benthic fluxes of REE with unique εNd signatures from marine sediments, particularly in the deep-sea, have led to a “bottom-up” hypothesis, which suggests that early diagenesis below the sediment-water interface (SWI) controls the ocean's REE and εNd budgets. To investigate such sedimentary processes, we created a reactive-transport model for the biogeochemical cycling of Nd and εNd in marine sediments. Here, we attempt to quantify the roles of authigenesis, marine silicate weathering and reverse weathering in the diagenetic cycling of Nd and εNd at a deep-sea (3000 m) site on the Oregon margin. Our model predicts that, at this site, Nd carried by Fe/Mn oxides into sediments eventually transforms to authigenic Nd-phosphate, during which ∼9% of the incoming solid Nd flux is released as a dissolved benthic flux back to the overlying bottom water. We also find that the classic reversible scavenging formulation applied to Nd co-cycling with Fe/Mn oxides is inconsistent with the data. Rather, a co-precipitation formulation, assuming Nd is structurally incorporated into Fe/Mn oxides, successfully simulates the data. The model also shows that authigenesis alone cannot explain the pore water and authigenic εNd, which are both more radiogenic than bottom water at this site. However, the weathering of volcanic silicates sourced from the local subduction zone can successfully explain εNd. We suggest that, because reverse weathering by authigenic clay formation maintains the under-saturation of primary silicates in pore water, marine silicate weathering can proceed. The processes we model likely affect the sedimentary cycling of many other trace elements and isotopes, with much broader implications for the understanding of ocean biogeochemistry.
Deng, K. ; Yang, S. ; Du, J. ; Lian, E. ; Vance, D. Dominance of Benthic Flux of Rees on Continental Shelves: Implications for Oceanic Budgets.
Geochemical Perspectives Letters 2022,
22, 26–30.
访问链接AbstractRare earth elements (REEs) are powerful tools to track oceanic biogeochemical proc-esses. However, our understanding of REE sources is incomplete, leading to contro-versial interpretations regarding their oceanic cycling. Continental margin sediments are often assumed to be a major source, but the sediment pore water data required to understand the processes controlling that potential source are scarce. Here, we mea-sure and compile pore water and estuarine REE data from the Changjiang (Yangtze) estuary-East China Sea shelf. We show that release of REEs, from shallow pore water to overlying seawater, is coupled to Mn reduction. In contrast, REEs are removed in deep pore water, perhaps via formation of an authigenic REE-bearing phase. This sedimentary source can potentially explain REE addition in the estuary at mid-high salinity. Our calculations suggest that the benthic flux is the largest Nd source (similar to 40 %) on the East China Sea shelf. Globally, however, despite a higher benthic Nd flux on the advection-dominated shelf, the much more extensive deep ocean still domi-nates the total area-integrated benthic flux. Our results call for a more extensive investigation of the magnitude of the benthic flux of REEs to the oceans.
Du, J. ; Mix, A. C. ; Haley, B. A. ; Belanger, C. L. ; Sharon,.
Volcanic Trigger of Ocean Deoxygenation During Cordilleran Ice Sheet Retreat.
Nature 2022,
611, 74–80.
访问链接AbstractNorth Pacific deoxygenation events during the last deglaciation were sustained over millennia by high export productivity, but the triggering mechanisms and their links to deglacial warming remain uncertain1–3. Here we find that initial deoxygenation in the North Pacific immediately after the Cordilleran ice sheet (CIS) retreat4 was associated with increased volcanic ash in seafloor sediments. Timing of volcanic inputs relative to CIS retreat suggests that regional explosive volcanism was initiated by ice unloading5,6. We posit that iron fertilization by volcanic ash7–9 during CIS retreat fuelled ocean productivity in this otherwise iron-limited region, and tipped the marine system towards sustained deoxygenation. We also identify older deoxygenation events linked to CIS retreat over the past approximately 50,000 years (ref. 4). Our findings suggest that the apparent coupling between the atmosphere, ocean, cryosphere and solid-Earth systems occurs on relatively short timescales and can act as an important driver for ocean biogeochemical change.
Abbott, A. N. ; Löhr, S. C. ; Payne, A. ; Kumar, H. ; Du, J. Widespread Lithogenic Control of Marine Authigenic Neodymium Isotope Records? Implications for Paleoceanographic Reconstructions.
Geochimica et Cosmochimica Acta 2022,
319, 318–336.
访问链接AbstractOur understanding of past ocean-climate dynamics is informed by multiple paleocirculation proxies including δ13C, 231Pa/230Th, and radiogenic neodymium isotopes (εNd). Of these, the εNd signature of marine authigenic phases is of particular importance as it is considered a robust circulation proxy applicable across timescales, permitting circulation reconstructions during periods of rapid, climatically-induced biological or chemical change (e.g. productivity, pH). However, growing evidence of non-conservative behavior and a widespread sedimentary source (benthic flux via pore water) of Nd to the global ocean suggests that authigenic εNd records do not strictly record a water mass signature, highlighting the need to reconsider interpretations of the authigenic record. To examine the impact of a sedimentary influence on the authigenic record, here we compile paired authigenic and detrital neodymium records from every major ocean basin and from 80 Ma to present. We then focus on just the North Atlantic Ocean basin to examine if this relationship holds up regionally and how authigenic εNd changes relate to sediment composition changes from two scientific ocean drill cores spanning the past 25 ka. We present a new conceptual framework to guide our discussion that examines the coupling or decoupling of authigenic and detrital εNd in terms of the relative importance of each of the three major potential controls as defined in the existing literature (bottom water, pore water, sediments) on the authigenic record. Our compilation reveals a strong linear relationship between detrital εNd and authigenic εNd (correlation coefficient = 0.86, n = 871), demonstrating a widespread influence of lithogenically sourced neodymium on authigenic εNd. We find the same is true within the North Atlantic, with the authigenic records at both locations strongly influenced by the sediments and likely not recording bottom water neodymium values. Emerging evidence for a lithogenic or benthic flux influence on the budgets of a wide range of trace elements suggests that our interpretative framework will be broadly useful for understanding the behavior of trace elements and their isotopes at the sediment-water interface.
Lemaitre, N. ; Du, J. ; de Souza, G. F. ; Archer, C. ; Vance, D. The Essential Bioactive Role of Nickel in the Oceans: Evidence from Nickel Isotopes.
Earth and Planetary Science Letters 2022,
584, 117513.
访问链接AbstractThe role of nickel (Ni) in ocean biogeochemical cycles is both under-studied and controversial. Strong correlations between Ni and organic carbon in modern and ancient marine sediments suggest a prominent biogeochemical role over a substantial portion of Earth history. Addition of Ni to culturing and seawater incubation experiments produces strong responses in terms of cell growth, particularly of nitrogen-fixing organisms. But the implied limiting role for phytoplankton growth is inconsistent with observations in the real ocean, specifically that photic zone Ni concentrations never descend to the very low values that characterise other bioactive, and often bio-limiting, metals like iron. These two observations can be reconciled if a large portion of the total dissolved Ni present in open-ocean surface waters is not bio-available on short timescales. Here we present new Ni concentration and stable isotope data from the GEOVIDE transect in the North Atlantic. We interpret these new data in the light of the growing database for Ni stable isotopes in the modern ocean, with implications for the biogeochemical importance of Ni. In the new North Atlantic dataset, the lowest Ni concentrations (1.8-2.6 nmol/L) and highest δ60Ni (up to +1.67‰) are associated with low nitrate, south of the subarctic front (SAF). By contrast, stations at latitudes north of the SAF, with higher surface nitrate, show very subdued variation in Ni concentrations throughout the entire depth of the water column (3.6±0.3 nmol/L, mean and 2SD), and no variation in δ60Ni beyond the narrow global deep-ocean range (+1.33±0.13 ‰). These North Atlantic Ni isotope data also show relationships with nitrogen isotope effects, observed in the same samples, that are suggestive of a link between Ni utilisation, isotope fractionation and nitrogen fixation. The global dataset, including the new data presented here, reveals a biogeochemical divide with Ni isotope fractionation only occurring in low latitude surface waters. A simple observationally constrained three-dimensional model of Ni cycling suggests that the creation of this isotopically heavy, Ni-poor, end-member, together with the physical circulation and remineralisation at depth, can explain the global Ni-δ60Ni systematics. Taken together, these findings hint at Ni-N co-limitation in the modern ocean. We advocate for more extensive and detailed culturing/incubation studies of this neglected metal in order to elucidate its potentially crucial biogeochemical role.