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In laboratory experiments, the precipitation of dolomite at ambient temperature is virtually impossible due to strong solvation shells of magnesium ions in aqueous media and probably also due to the existence of a more intrinsic crystallization barrier that prevents the formation of long-range ordered crystallographic structures at ambient surface conditions. Conversely, dolomite can easily form at high temperature (>100 °C), but its precipitation and growth requires several days or weeks depending on experimental conditions. In the present study, experiments were performed to assess how a single heat-ageing step promotes the formation of dolomite under high-carbonate alkaline conditions via dissolution-precipitation reactions. This reaction pathway is relevant for the so-called hydrothermal dolomite frequently observed in carbonate platforms, but still ill-defined and understood. Our precipitation route is summarized by two main sequential reactions: (1) precipitation of Mg-calcite at low temperature (∼20 °C) by aqueous carbonation of synthetic portlandite (Ca(OH)2) in a highly alkaline medium (1 M of NaOH and 1 M of MgCl2), leading to precipitation of oriented nanoparticles of low- and high-Mg calcite (∼79 wt%) coexisting with aragonite (∼18 wt%) and brucite (∼3 wt%) after 24 h; (2) fast dolomitization process starting from 1 h of reaction by a single heat-ageing step from ∼20 to 200, 250 and 300 °C. Here, the Mg-calcite acts as a precursor that lowers the overall kinetics barrier for dolomite formation. Moreover, it is an important component in some bio-minerals (e.g. corals and seashells). Quantitative Rietveld refinements of XRD patterns, FESEM observations and FTIR measurements on the sequentially collected samples suggest fast dolomite precipitation coupled with dissolution of transient mineral phases such as low-Mg calcite (Mg < 4 mol%), high-Mg calcite (Mg > 4 mol%), proto-dolomite (or disordered dolomite; Mg > 40 mol%) and Ca-magnesite. In this case, the dolomite formation rate and the time-dependent mineral composition strongly depend on reaction temperature. For example, high-purity dolomitic material (87 wt% of dolomite mixed with 13 wt% of magnesite) was obtained at 300 °C after 48 h of reaction. Conversely, a lower proportion of dolomite (37 wt%), mixed with proto-dolomite (43 wt%), Ca-magnesite (16 wt%) and high-Mg calcite (4 wt%), was obtained at 200 °C after 72 h. The present experiments provide an additional mechanism for the massive dolomite formation in sedimentary environments (ex. deep sea organic-rich carbonate-sediments) if such sediments are subjected to significant temperature variations, for example by hot fluid circulations related to volcanic activity. In such systems, organic degradation increases the carbonate alkalinity (HCO3−) necessary to induce the dolomitization process at low and high temperature. 相似文献
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Rising atmospheric pCO2 and ocean acidification originating from human activities could result in increased dissolution of metastable carbonate minerals
in shallow-water marine sediments. In the present study, in situ dissolution of carbonate sedimentary particles in Devil’s
Hole, Bermuda, was observed during summer when thermally driven density stratification restricted mixing between the bottom
water and the surface mixed layer and microbial decomposition of organic matter in the subthermocline layer produced pCO2 levels similar to or higher than those levels anticipated by the end of the 21st century. Trends in both seawater chemistry
and the composition of sediments in Devil’s Hole indicate that Mg-calcite minerals are subject to selective dissolution under
conditions of elevated pCO2. The derived rates of dissolution based on observed changes in excess alkalinity and estimates of vertical eddy diffusion
ranged from 0.2 mmol to 0.8 mmol CaCO3 m−2 h−1. On a yearly basis, this range corresponds to 175–701 g CaCO3 m−2 year−1; the latter rate is close to 50% of the estimate of the current average global coral reef calcification rate of about 1,500 g
CaCO3 m−2 year−1. Considering a reduction in marine calcification of 40% by the year 2100, or 90% by 2300, as a result of surface ocean acidification,
the combination of high rates of carbonate dissolution and reduced rates of calcification implies that coral reefs and other
carbonate sediment environments within the 21st and following centuries could be subject to a net loss in carbonate material
as a result of increasing pCO2 arising from burning of fossil fuels. 相似文献
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Yifeng Chen Ryo Matsumoto Charles K. Paull William Ussler III Thomas Lorenson Patrick Hart William Winters 《Journal of Geochemical Exploration》2007,95(1-3):1
Authigenic carbonates were sampled in piston cores collected from both the Tunica Mound and the Mississippi Canyon area on the continental slope of the northern Gulf of Mexico during a Marion Dufresne cruise in July 2002. The carbonates are present as hardgrounds, porous crusts, concretions or nodules and shell fragments with or without carbonate cements. Carbonates occurred at gas venting sites which are likely to overlie gas hydrates bearing sediments. Electron microprobe, X-ray diffraction (XRD) and thinsection investigations show that these carbonates are high-Mg calcite (6–21 mol% MgCO3), with significant presence of framboidal pyrite. All carbonates are depleted in 13C (δ13C = − 61.9 to − 31.5‰ PDB) indicating that the carbon is derived mainly from anaerobic methane oxidation (AMO). Age estimates based on 14C dating of shell fragments and on regional sedimentation rates indicate that these authigenic carbonates formed within the last 1000 yr in the Mississippi Canyon and within 5500 yr at the Tunica Mound. The oxygen isotopic composition of carbonates ranges from + 3.4 to + 5.9‰ PDB. Oxygen isotopic compositions and Mg2+ contents of carbonates, and present in-situ temperatures of bottom seawater/sediments, show that some of these carbonates, especially from a core associated with underlying massive gas hydrates precipitated in or near equilibrium with bottom-water. On the other hand, those carbonates more enriched in 18O are interpreted to have precipitated from 18O-rich fluids which are thought to have been derived from the dissociation of gas hydrates. The dissociation of gas hydrates in the northern Gulf of Mexico within the last 5500 yr may be caused by nearby salt movement and related brines. 相似文献
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采用稳定加液一反应系统对5、15和25 ° C下镁方解石沉淀在海水中的形成过程进行了研究.结果表明镁方解石的沉淀速率(R)对过饱和度(Ω)的响应均可通过R=k(Ω-1)°或Log(R)=nLog(Ω-1)+Log(k)形式的动力学方程加以表达.pCO2的变化会显著改变过饱和度进而影响到镁方解石沉淀速率,但这一变化并不会对镁方解石沉淀形成过程的动力学表达产生影响.相比之下,不同温度下镁方解石沉淀形成的动力学方程存在明显差异,表明这一动力学过程同时还具有强烈的热力学相关性. 相似文献
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