The Sensitivity of the Phanerozoic Inorganic Carbon System to the Onset of Pelagic Sedimentation     

Rolf S. Arvidson  Fred T. Mackenzie  Robert A. Berner 《Aquatic Geochemistry》2014,20(2-3):343-362

The onset of pelagic sedimentation attending the radiation of pelagic calcifiers during the Mesozoic was an important divide in Earth history, shifting the locus of significant carbonate sedimentation from the shallow shelf environments of the Paleozoic to the deep sea. This shift would have impacted the CO₂ cycle, given that decarbonation of subducted pelagic carbonate is an important return flux of CO₂ to the atmosphere. Coupled with the fact that the mean residence time of continental platform and basin sedimentary carbonate exceeds that of the oceanic crust, it thus becomes unclear whether carbon cycling would have operated on a substantially different footing prior to the pelagic transition. Here, we examine this uncertainty with sensitivity analyses of the timing of this transition using a coupled model of the Phanerozoic atmosphere, ocean, and shallow lithosphere. For purposes of comparison, we establish an age of 250 Ma (i.e., after the Permo-Triassic extinctions) as the earliest opportunity for deposition of extensive biogenic pelagic carbonate on the deep seafloor, an age that predates known occurrences of pelagic calcifiers (and intact seafloor). Although an approximate boundary, we do show that attempts to shift this datum either significantly earlier or later in time produce model results that are inconsistent with observed trends in the mass–age distribution of the rock record and with accepted trends in seawater composition as constrained by proxy data. Significantly, we also conclude that regardless of the timing of the onset of biogenic pelagic carbonate sedimentation, a carbon sink involving seawater-derived dissolved inorganic carbon played a critical role in carbon cycling, particularly in the Paleozoic. This CaCO₃ sink may have been wholly abiogenic, involving calcium derived either directly from seawater (thus manifest as a direct seafloor deposit), or alternatively from basalt–seawater reactions (represented by precipitation of CaCO₃ in veins and fissures within the basalt). Despite the uncertainty in the source and magnitude of this abiogenic CaCO₃ flux, it is likely a basic and permanent feature of global carbon cycling. Subduction of this CaCO₃ would have acted as a basic return circuit for atmospheric CO₂ even in the absence of biogenically derived pelagic carbonate sedimentation. Lastly, model calculations of the ratio of dissolved calcium to carbonate ion (Ca²⁺/CO₃ ^2?) show this quantity underwent significant secular evolution over the Phanerozoic. As there is increasing recognition of this ratio’s role in CaCO₃ growth and dissolution reactions, this evolution, together with progressive increases in nutrient availability and saturation state, may have created a tipping point ultimately conducive to the appearance of pelagic calcifiers in the Mesozoic.  相似文献   

Beloc, Haiti, revisited: multiple events across the KT boundary in the Caribbean     

W. Stinnesbeck  G. Keller  T. Adatte  D. Stüben  U. Kramar  Z. Berner  C. Desremeaux  E. Molière 《地学学报》1999,11(6):303-310

Examination of new expanded K/T boundary sections near Beloc, Haiti, reveals deposition of a glass spherule-rich deposit (SRD) and two (PGE) anomalies (one Ir-dominated and one Pd-dominated) during the early Danian Parvularugoglobigerina eugubina Zone [Pla(l)]. The presence of the Haiti SRD within the early Danian is interpreted as being due to reworking. Ir is only slightly elevated within the SRD but forms an anomaly at the top of the SRD extending into the overlying pelagic limestones. It is unclear at present whether this Ir anomaly results from mechanical reworking of an impact at the K/T boundary, or an additional impact event in the early Danian. The second PGE anomaly upsection is dominated by Pd and Pt and is more compatible with a magmatic origin. This suggests a multi-event scenario consistent with one (and possibly two) impact(s), followed by a PGE-enriched volcanic event in the Caribbean.  相似文献   

Temporal variations in arsenic concentration in the groundwater of Murshidabad District,West Bengal,India   总被引：1，自引：0，他引：1  

S. H. Farooq  D. Chandrasekharam  S. Norra  Z. Berner  E. Eiche  P. Thambidurai  D. Stüben 《Environmental Earth Sciences》2011,62(2):223-232

Systematic investigations on seasonal variations in arsenic (As) concentrations in groundwater in both space and time are scarce for most parts of West Bengal (India). Hence, this study has been undertaken to investigate the extent of As pollution and its temporal variability in parts of Murshidabad district (West Bengal, India). Water samples from 35 wells were collected during pre-monsoon, monsoon and post-monsoon seasons and analyzed for various elements. Based on the Indian permissible limit for As (50 μg/L) in the drinking water, water samples were classified into contaminated and uncontaminated category. 18 wells were reported as uncontaminated (on average 12 μg/L As) and 12 wells were found contaminated (129 μg/L As) throughout the year, while 5 wells could be classified as either contaminated or uncontaminated depending on when they were sampled. Although the number of wells that alternate between the contaminated and uncontaminated classification is relatively small (14%), distinct seasonal variation in As concentrations occur in all wells. This suggests that investigations conducted within the study area for the purpose of assessing the health risk posed by As in groundwater should not rely on a single round of water samples. In comparison to other areas, As is mainly released to the groundwater due to reductive dissolution of Fe-oxyhydroxides, a process, which is probably enhanced by anthropogenic input of organic carbon. The seasonal variation in As concentrations appear to be caused mainly by dilution effects during monsoon and post-monsoon. The relatively high concentrations of Mn (mean 0.9 mg/L), well above the WHO limit (0.4 mg/L), also cause great concern and necessitate further investigations.  相似文献   

Arsenic in framboidal pyrite from recent sediments of a shallow water lagoon of the Baltic Sea     

Thomas Neumann  Florian Scholz  Utz Kramar  Michael Ostermaier  Nicole Rausch  Zsolt Berner 《Sedimentology》2013,60(6):1389-1404

Arsenic is a redox‐sensitive element of environmental relevance and often enriched in iron sulphides. Because sediments from the Achterwasser lagoon, a part of the estuarine system of the river Oder, south‐west Baltic Sea, show unexpectedly high pyrite concentrations of up to 7·5 wt% they were used to investigate the influence of authigenic pyrite on the mobility and burial of As in the coastal environment. Micro‐X‐ray‐fluorescence measurements of 106 micrometre‐sized pyrite framboids from the anoxic sediments show highly variable As concentrations ranging from 6 to 1142 μg g^?1. Even within a 1 cm thick layer, the As concentration of different framboids varies greatly and no clear depth trend is visible throughout the 50 cm long sediment core. Pyrite can account for 9 to 55% (average 22%) of the total As budget of the sediments and the degree of trace metalloid pyritization for As ranges from 26 to 61%, indicating that authigenic pyrite formation is an important process in the geochemical cycling of As in coastal sediments. High‐resolution micro‐X‐ray fluorescence mapping of single pyrite grains shows that As is distributed inhomogeneously within larger framboids, suggesting changing pore water composition during pyrite growth. X‐ray absorption near edge structure spectra indicate that As is usually present as As(‐I) substituting S in the pyrite lattice. However, in samples close to the sediment/water interface a considerable part of As is in higher valence states (+III/+V). This can be explained by frequent re‐suspension of the surficial sediments to the oxic water column due to wave action and subsequent re‐deposition, leading to the adsorption of As oxyanions onto pyrite. Although reduced As(‐I) becomes more important in the deeper samples, reflecting decreasing redox potential and a longer time since deposition, the occurrence of oxidized As species (AsIII/AsV) in pyrite in the anoxic part of the sediment suggests formation under dysoxic conditions.  相似文献   

An Earth Systems Diagram for the Global Cycles of Carbon and Phosphorus and Their Effects on Atmospheric CO2 and O2     

Robert A. Berner 《Aquatic Geochemistry》2013,19(5-6):565-568

A complex cause–effect type earth systems diagram is presented that represents the interrelation of the global carbon and phosphorus cycles over geological time. It demonstrates how a lot of information can be represented in an extremely compact manner and how relatively unrecognized positive and negative feedbacks are revealed by tracing paths on the diagram. Emphasis is on how the C and P cycles affect the levels of atmospheric CO₂ and O₂, often via rather indirect paths.  相似文献   

Characteristics of arsenic adsorption from aqueous solution: Effect of arsenic species and natural adsorbents     

Huaming Guo  Doris Stüben  Zsolt Berner  Qingchun Yu 《Applied Geochemistry》2009

Batch and column experiments were conducted on As adsorption from aqueous solution by natural solids to test the feasibility of these materials to act as adsorbents for As removal from groundwater and drinking water. The solids considered are natural hematite and natural siderite. The As species studied are As(V), As(III) and dimethylarsinic acid (DMA). Arsenic(III), As(V) and DMA were removed to different extents by the solids studied from water solutions containing these three As species, with the highest efficiency for As(V). In aqueous solutions with a mixture of As species, adsorption kinetics depend on the species. On both materials, As(V) was preferentially adsorbed in the batches and first reached equilibrium, followed by DMA and As(III). The As adsorption took place more slowly on natural hematite and natural siderite compared with ferrihydrite. The results demonstrate that the amount of As removed from As(III) batches was greater than that from As(V) batches due to a surface alteration of the solids caused by As(III) oxidation. Although the highest efficiency for As retention was observed on hematite HIO1 in the batch experiments, siderite used as column filling was more efficient in removing As from water containing the As species studied in comparison with hematite. The coating of fresh Fe(III)-oxides was much more intensive in the siderite-packed column than in the hematite-packed column. The combination of siderite and hematite would promote the column filling performance in removing As from aqueous solution.  相似文献   

Comments on “Molecular diffusion and the sedimentary environment: results from the in situ determination of whole sediment diffusion coefficients” by P. E. Kepkay,R. C. Cooke and A. J. Bowen     

Joseph T. Westrich  Michael D. Krom  Robert A. Berner 《Geochimica et cosmochimica acta》1982,46(11):2407

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Inclusion of adsorption in the modelling of early diagenesis     

Robert A. Berner 《Earth and Planetary Science Letters》1976,29(2):333-340

A general one-dimensional diagenetic equation is derived which expresses the effect of the following processes upon the depth and time distribution of a dissolved species in a modern subaqueous sediment: adsorptive or ion exchange equilibrium between pore water and grain surfaces; slower chemical or radiogenic reactions in the pore solution and on the grain surfaces; diffusion in solution and on grain surfaces; advection of grains due to depositional burial; and advection of water due both to burial and to flow past the grains. It is shown that the effects of equilibrium adsorption can be expressed in terms of a lowered diffusion coefficient only in the special case where there is negligible flow of water relative to grains, adsorption is described by a simple linear isotherm, and there is nochemical reaction occurring in the sediment (i.e. only radioactive decay or no reaction at all). Consideration of a commonly used special case of the general equation indicates that if equilibrium adsorption is strong, the depositional term in the resulting diagenetic equation may become quantitatively as important as the terms for diffusion and chemical reaction. Thus, when modelling diagenesis, deposition often cannot be ignored. A coupled pair of differential equations are also derived which express the steady state depth distribution for two ions exhibiting equilibrium ion exchange while undergoing chemical reaction, diffusion, and deposition.  相似文献   

Carbon isotope evidence implying high O₂/CO₂ ratios in the Permo-Carboniferous atmosphere     

D.J. Beerling  J.A. LakeR.A. Berner  L.J. HickeyD.W. Taylor  D.L. Royer 《Geochimica et cosmochimica acta》2002,66(21):3757-3767

Theoretical models predict a marked increase in atmospheric O₂ to ∼35% during the Permo-Carboniferous (∼300 Ma) occurring against a low (∼0.03%) CO₂ level. An upper O₂ value of 35%, however, remains disputed because ignition data indicate that excessive global forest fires would have ensued. This uncertainty limits interpretation of the role played by atmospheric oxygen in Late Paleozoic biotic evolution. Here, we describe new results from laboratory experiments with vascular land plants that establish that a rise in O₂ to 35% increases isotopic fractionation (Δ¹³C) during growth relative to control plants grown at 21% O₂. Despite some effect of the background atmospheric CO₂ level on the magnitude of the increase, we hypothesize that a substantial Permo-Carboniferous rise in O₂ could have imprinted a detectable geochemical signature in the plant fossil record. Over 50 carbon isotope measurements on intact carbon from four fossil plant clades with differing physiological ecologies and ranging in age from Devonian to Cretaceous reveal a substantial Δ¹³C anomaly (5‰) occurring between 300 and 250 Ma. The timing and direction of the Δ¹³C excursion is consistent with the effects of a high O₂ atmosphere on plants, as predicted from photosynthetic theory and observed in our experiments. Preliminary calibration of the fossil Δ¹³C record against experimental data yields a predicted O₂/CO₂ mixing ratio of the ancient atmosphere consistent with that calculated from long-term models of the global carbon and oxygen cycles. We conclude that further work on the effects of O₂ in the combustion of plant materials and the spread of wildfire is necessary before existing data can be used to reliably set the upper limit for paleo-O₂ levels.  相似文献   

S- and O-isotopic character of dissolved sulphate in the cover rock aquifers of a Zechstein salt dome     

Zsolt A. Berner  Doris Stüben  Markus A. Leosson  Hans Klinge 《Applied Geochemistry》2002,17(12):11

Sulfur and O isotope analyses of dissolved SO₄ were used to constrain a hydrogeological model for the area overlying the Gorleben–Rambow Salt Structure, Northern Germany. Samples were collected from 80 wells screened at different depth-intervals. The study area consists of a set of two vertically stacked aquifer systems. Generally, the isotope data show a good spatial correlation, outlining well-defined groundwater zones containing SO₄ of characteristic isotopic composition. Highly saline waters from deeper parts of the lower aquifer system are characterized by rather constant SO₄ isotopic compositions, which are typical of Permian Zechstein evaporites (δ³⁴S=9.6–11.9‰; δ¹⁸O=9.5–12.1‰). Above this is a transition zone containing ground waters of intermediate salinity and slightly higher isotopic values (average δ³⁴S=16.6‰; δ¹⁸O=15.3‰). The confined groundwater horizon on the top of the lower aquifer system below the low permeable Hamburg Clays is low in total dissolved solids and is characterized by an extreme ³⁴S enrichment (average δ³⁴S=39.1‰; δ¹⁸O=18.4‰), suggesting that bacterially mediated SO₄ reduction is a dominant geochemical process in this zone. Two areas of distinct isotopic composition can be identified in the shallow ground water horizons of the upper hydrogeological system. Sulfate in groundwaters adjacent to the river Elbe and Löcknitz has a typical meteoric isotopic signature (δ³⁴S=5.2‰; δ¹⁸O=8.2‰), whereas the central part of the area is characterized by more elevated isotopic ratios (δ³⁴S=12.7‰; δ¹⁸O=15.6‰). The two major SO₄ pools in the area are represented by Permian seawater SO₄ and a SO₄ of meteoric origin that has been mixed with SO₄ resulting from the oxidation of pyrite. It is suggested that the S-isotope compositions observed reflect the nature of the SO₄ source that have been modified to various extent by bacterial SO₄ reduction. Groundwaters with transitional salinity have resulted from mixing between brines and low-mineralized waters affected by bacterial SO₄ reduction.  相似文献