Dissolution of Carbonate Sediments Under Rising <Emphasis Type="Italic">p</Emphasis>CO<Subscript>2</Subscript> and Ocean Acidification: Observations from Devil’s Hole,Bermuda     

Andreas J. Andersson  Nicholas R. Bates  Fred T. Mackenzie 《Aquatic Geochemistry》2007,13(3):237-264

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   

Low-temperature heat capacities of MgAl<Subscript>2</Subscript>O<Subscript>4</Subscript> and spinels of the MgCr<Subscript>2</Subscript>O<Subscript>4</Subscript>–MgAl<Subscript>2</Subscript>O<Subscript>4</Subscript> solid solution     

Stephan Klemme  Martin Ahrens 《Physics and Chemistry of Minerals》2007,34(2):59-72

We present results from low-temperature heat capacity measurements of spinels along the solid solution between MgAl₂O₄ and MgCr₂O₄. The data also include new low-temperature heat capacity measurements for MgAl₂O₄ spinel. Heat capacities were measured between 1.5 and 300 K, and thermochemical functions were derived from the results. No heat capacity anomaly was observed for MgAl₂O₄ spinel; however, we observe a low-temperature heat capacity anomaly for Cr-bearing spinels at temperatures below 15 K. From our data we calculate standard entropies (298.15 K) for Mg(Cr,Al)₂O₄ spinels. We suggest a standard entropy for MgAl₂O₄ of 80.9 ± 0.6 J mol⁻¹ K⁻¹. For the solid solution between MgAl₂O₄ and MgCr₂O₄, we observe a linear increase of the standard entropies from 80.9 J mol⁻¹ K⁻¹ for MgAl₂O₄ to 118.3 J mol⁻¹ K⁻¹ for MgCr₂O₄.  相似文献   

CO<Subscript>2</Subscript> absorption by alkaline soils and its implication to the global carbon cycle   总被引：2，自引：0，他引：2  

Jingxia Xie  Yan Li  Cuixia Zhai  Chenhua Li  Zhongdong Lan 《Environmental Geology》2009,56(5):953-961

Motivated by the rapid increase in atmospheric CO₂ due to human activities since the Industrial Revolution, and the climate changes it produced, the world’s concerned scientific community has made a huge effort to investigate the global carbon cycle. However, the results reveal that the global CO₂ budget cannot be balanced, unless a “missing sink” is invoked. Although numerous studies claimed to find the “missing sink”, none of those claims has been widely accepted. This current study showed that alkaline soil on land are absorbing CO₂ at a rate of 0.3–3.0 μmol m⁻² s⁻¹ with an inorganic, non-biological process. The intensity of this CO₂ absorption is determined by the salinity, alkalinity, temperature and water content of the saline/alkaline soils, which are widely distributed on land. Further studies revealed that high salinity or alkalinity positively affected the CO₂ absorbing intensity, while high temperature and water content had a negative effect on the CO₂ absorbing intensity of these soils. This inorganic, non-biological process of CO₂ absorption by alkaline soils might have significant implications to the global carbon budget accounting.  相似文献   

Respiration and Calcification of <Emphasis Type="Italic">Crassostrea gigas</Emphasis>: Contribution of an Intertidal Invasive Species to Coastal Ecosystem CO<Subscript>2</Subscript> Fluxes     

Morgane Lejart  Jacques Clavier  Laurent Chauvaud  Christian Hily 《Estuaries and Coasts》2012,35(2):622-632

Respiration and calcification rates of the Pacific oyster Crassostrea gigas were measured in a laboratory experiment in the air and underwater, accounting for seasonal variations and individual size, to estimate the effects of this exotic species on annual carbon budgets in the Bay of Brest, France. Respiration and calcification rates changed significantly with season and size. Mean underwater respiration rates, deducted from changes in dissolved inorganic carbon (DIC), were 11.4 μmol DIC g⁻¹ ash-free dry weight (AFDW) h⁻¹ (standard deviation (SD), 4.6) and 32.3 μmol DIC g⁻¹ AFDW h⁻¹ (SD 4.1) for adults (80–110 mm shell length) and juveniles (30–60 mm), respectively. The mean daily contribution of C. gigas underwater respiration (with 14 h per day of immersion on average) to DIC averaged over the Bay of Brest population was 7.0 mmol DIC m⁻² day⁻¹ (SD 8.1). Mean aerial CO₂ respiration rate, estimated using an infrared gas analyzer, was 0.7 μmol CO₂ g⁻¹ AFDW h⁻¹ (SD 0.1) for adults and 1.1 μmol CO₂ g⁻¹ AFDW h⁻¹ (SD 0.2) for juveniles, corresponding to a mean daily contribution of 0.4 mmol CO₂ m⁻² day⁻¹ (SD 0.50) averaged over the Bay of Brest population (with 10 h per day of emersion on average). Mean CaCO₃ uptake rates for adults and juveniles were 4.5 μmol CaCO₃ g⁻¹ AFDW h⁻¹ (SD 1.7) and 46.9 μmol CaCO₃ g⁻¹ AFDW h⁻¹ (SD 29.2), respectively. The mean daily contribution of net calcification in the Bay of Brest C. gigas population to CO₂ fluxes during immersion was estimated to be 2.5 mmol CO₂ m⁻² day⁻¹ (SD 2.9). Total carbon release by this C. gigas population was 39 g C m⁻² year⁻¹ and reached 334 g C m⁻² year⁻¹ for densely colonized areas with relative contributions by underwater respiration, net calcification, and aerial respiration of 71%, 25%, and 4%, respectively. These observations emphasize the substantial influence of this invasive species on the carbon cycle, including biogenic carbonate production, in coastal ecosystems.  相似文献   

Analysis of the spatial and temporal changes in soil CO<Subscript>2</Subscript> flux in alpine meadow of Qilian Mountain     

Zongqiang Chang  Qi Feng  Jianhua Si  Yonghong Su  Haiyang Xi  Jianlin Li 《Environmental Geology》2009,58(3):483-490

Field experiments on the CO₂ flux of alpine meadow soil in the Qilian Mountain were conducted along the elevation gradient during the growing season of 2004 and 2005. The soil CO₂ flux was measured using the Li-6400-09 soil respiration chamber attached to the Li-6400 portable photosynthesis system. The effects of water and heat and roots on the soil CO₂ flux were statistically analyzed. The results show that soil CO₂ flux along the elevation gradient gradually decreases. The soil CO₂ flux was low at night, with lowest value occurring between 0200 and 0600 hours, started to rise rapidly during 0700–0830 hours, and then descend during 1600–1830 hours. The peak CO₂ efflux appears during 1100–1600 hours. The diurnal average of soil CO₂ efflux was between 0.56 ± 0.32 and 2.53 ± 0.76 μmol m⁻² s⁻¹. Seasonally, soil CO₂ fluxes are relatively high in summer and autumn and low in spring and winter. The soil CO₂ efflux, from the highest to the lowest in the ranking order, occurred in July and August (4.736 μmol m⁻² s⁻¹), June and September, and May and October, respectively. The soil CO₂ efflux during the growing season is positively correlated with soil temperature, root biomass and soil water content.  相似文献   

Contribution of a Dense Population of the Brittle Star <Emphasis Type="Italic">Acrocnida brachiata</Emphasis> (Montagu) to the Biogeochemical Fluxes of CO<Subscript>2</Subscript> in a Temperate Coastal Ecosystem     

Dominique Davoult  Jérôme Harlay  Franck Gentil 《Estuaries and Coasts》2009,32(6):1103-1110

The production of organic matter and calcium carbonate by a dense population of the brittle star Acrocnida brachiata (Echinodermata) was calculated using demographic structure, population density, and relations between the size (disk diameter) and the ash-free dry weight (AFDW) or the calcimass. During a 2-year survey in the Bay of Seine (Eastern English Channel, France), organic production varied from 29 to 50 g_AFDW m⁻² year⁻¹ and CaCO₃ production from 69 to 104 g_CaCO3 m⁻² year⁻¹. Respiration was estimated between 1.7 and 2.0 mol_CO2 m⁻² year⁻¹. Using the molar ratio (ψ) of CO₂ released: CaCO₃ precipitated, this biogenic precipitation of calcium carbonate would result in an additional release between 0.5 and 0.7 mol_CO2 m⁻² year⁻¹ that represented 23% and 26% of total CO₂ fluxes (sum of calcification and respiration). The results of the present study suggest that calcification in temperate shallow environments should be considered as a significant source of CO₂ to seawater and thus a potential source of CO₂ to the atmosphere, emphasizing the important role of the biomineralization (estimated here) and dissolution (endoskeletons of dead individuals) in the carbon budget of temperate coastal ecosystems.  相似文献   

Vibrational states of H<Subscript>2</Subscript>O in beryl: physical aspects     

Boris Kolesov 《Physics and Chemistry of Minerals》2008,35(5):271-278

Single-crystal polarized Raman spectra (3,000–4,000 cm⁻¹ at 3 ≤ T ≤ 300 K) were measured for synthetic alkali-free and natural beryl, Be₂Al₃Si₆O₁₈·xH₂O, to determine the behavior of H₂O molecules of both Type I and Type II in the cavities. At low temperature, the H₂O molecules of Type I displace from the center of cavity and give rise to very weak hydrogen bonding with the host lattice. The H₂O Type I translational motion is characterized by substantial anharmonicity and looks like a motion of “a particle in the box” with a frequency of 6.3 cm⁻¹. Water Type II is characterized by a free rotation with respect to the C ₂ molecule axis, and it makes possible the water nuclear isomers (i.e. ortho- and para-) to be observed at low temperature.

Boris KolesovEmail:

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Superdense CO2 inclusions in Cretaceous quartz–stibnite veins hosted in low-grade Variscan basement of the Western Carpathians, Slovakia     

Márian Urban  Rainer Thomas  Vratislav Hurai  Patrik Koneèný  Martin Chovan 《Mineralium Deposita》2006,40(8):867-873

CO₂ inclusions with density up to 1,197 kg m⁻³ occur in quartz–stibnite veins hosted in the low-grade Palaeozoic basement of the Gemericum tectonic unit in the Western Carpathians. Raman microanalysis corroborated CO₂ as dominant gas species accompanied by small amounts of nitrogen (<7.3 mol%) and methane (<2.5 mol%). The superdense CO₂ phase exsolved from an aqueous bulk fluid at temperatures of 183–237°C and pressures between 1.6 and 3.5 kbar, possibly up to 4.5 kbar. Low thermal gradients (∼12–13°C km⁻¹) and the CO₂–CH₄–N₂ fluid composition rule out a genetic link with the subjacent Permian granites and indicate an external, either metamorphogenic (oxidation of siderite, dedolomitization) or lower crustal/mantle, source of the ore-forming fluids.According to microprobe U–Pb–Th dating of monazite, the stibnite-bearing veins formed during early Cretaceous thrusting of the Gemeric basement over the adjacent Veporic unit. The 15- to 18-km depth of burial estimated from the fluid inclusion trapping PT parameters indicates a 8- to 11-km-thick Upper Palaeozoic–Jurassic accretionary complex overlying the Gemeric basement and its Permo-Triassic autochthonous cover.  相似文献   

Low-temperature heat capacities,entropies and enthalpies of Mg<Subscript>2</Subscript>SiO<Subscript>4</Subscript> polymorphs,and α−β−γ and post-spinel phase relations at high pressure     

M. Akaogi  H. Takayama  H. Kojitani  H. Kawaji  T. Atake 《Physics and Chemistry of Minerals》2007,34(3):169-183

The low-temperature isobaric heat capacities (C _p) of β- and γ-Mg₂SiO₄ were measured at the range of 1.8–304.7 K with a thermal relaxation method using the Physical Property Measurement System. The obtained standard entropies (S°₂₉₈) of β- and γ-Mg₂SiO₄ are 86.4 ± 0.4 and 82.7 ± 0.5 J/mol K, respectively. Enthalpies of transitions among α-, β- and γ-Mg₂SiO₄ were measured by high-temperature drop-solution calorimetry with gas-bubbling technique. The enthalpies of the α−β and β−γ transitions at 298 K (ΔH°₂₉₈) in Mg₂SiO₄ are 27.2 ± 3.6 and 12.9 ± 3.3 kJ/mol, respectively. Calculated α−β and β−γ transition boundaries were generally consistent with those determined by high-pressure experiments within the errors. Combining the measured ΔH°₂₉₈ and ΔS°₂₉₈ with selected data of in situ X-ray diffraction experiments at high pressure, the ΔH°₂₉₈ and ΔS°₂₉₈ of the α−β and β−γ transitions were optimized. Calculation using the optimized data tightly constrained the α−β and β−γ transition boundaries in the P, T space. The slope of α−β transition boundary is 3.1 MPa/K at 13.4 GPa and 1,400 K, and that of β−γ boundary 5.2 MPa/K at 18.7 GPa and 1,600 K. The post-spinel transition boundary of γ-Mg₂SiO₄ to MgSiO₃ perovskite plus MgO was also calculated, using the optimized data on γ-Mg₂SiO₄ and available enthalpy and entropy data on MgSiO₃ perovskite and MgO. The calculated post-spinel boundary with a Clapeyron slope of −2.6 ± 0.2 MPa/K is located at pressure consistent with the 660 km discontinuity, considering the error of the thermodynamic data.  相似文献   

Fine structure in photoluminescence spectrum of S<Subscript>2</Subscript><Superscript>−</Superscript> center in sodalite     

Aierken Sidike  Alifu Sawuti  Xiang-Ming Wang  Heng-Jiang Zhu  S. Kobayashi  I. Kusachi  N. Yamashita 《Physics and Chemistry of Minerals》2007,34(7):477-484

The photoluminescence and excitation spectra of sodalites from Greenland, Canada and Xinjiang (China) are observed at 300 and 10 K in detail. The features of the emission and excitation spectra of the orange-yellow fluorescence of these sodalites are independent of the locality. The emission spectra at 300 and 10 K consist of a broad band with a series of peaks and a maximum peak at 648 and 645.9 nm, respectively. The excitation spectra obtained by monitoring the orange-yellow fluorescence at 300 and 10 K consist of a main band with a peak at 392 nm. The luminescence efficiency of the heat-treated sodalite from Xinjiang is about seven times as high as that of untreated natural sodalite. The emission spectrum of the S₂ ⁻ center in sodalite at 10 K consists of a band with a clearly resolved structure with a series of maxima spaced about 560 cm⁻¹ (20–25 nm) apart. Each narrow band at 10 K shows a fine structure consisting of a small peak due to the stretching vibration of the isotopic species of ³²S³⁴S⁻, a main peak due to that of the isotopic species of ³²S₂ ⁻ and five peaks due to phonon sidebands of the main peak.  相似文献   

CO<Subscript>2</Subscript> emissions from a municipal site for final disposal of solid waste in Gualeguaychu,Entre Rios Province,Argentina     

Romina Sanci  Héctor O. Panarello  Héctor A. Ostera 《Environmental Earth Sciences》2012,66(2):519-528

This paper estimates CO₂ fluxes in a municipal site for final disposal of solid waste, located in Gualeguaychu, Argentina. Estimations were made using the accumulation chamber methods, which had been calibrated previously in laboratory. CO₂ fluxes ranged from 31 to 331 g m⁻² day⁻¹. Three different populations were identified: background soil gases averaging 46 g m⁻² day⁻¹, intermediate anomalous values averaging 110 g m⁻² day⁻¹ and high anomalous values averaging 270 g m⁻² day⁻¹. Gas samples to a depth of 20 cm were also taken. Gas fractions, XCO₂ < 0.1, XCH₄ < 0.01, XN₂ ~0.71 and XO₂ ~0.21, δ¹³C of CO₂ (−34 to −18‰), as well as age of waste emplacement, suggest that the study site may be at the final stage of aerobic biodegradation. In a first approach, and following the downstream direction of groundwater flow, alkalinity and δ¹³C of dissolved inorganic carbon (−15 to 4‰) were observed to increase when groundwater passed through the disposal site. This suggests that the CO₂ generated by waste biodegradation dissolves or that dissolved organic matter appears as a result of leachate degradation.  相似文献   

Potential protonation sites in the Al<Subscript>2</Subscript>SiO<Subscript>5</Subscript> polymorphs based on polarized FTIR spectroscopy and properties of the electron density distribution     

Jason B. Burt  Nancy L. Ross  G. V. Gibbs  George R. Rossman  Kevin M. Rosso 《Physics and Chemistry of Minerals》2007,34(5):295-306

Potential protonation sites for, kyanite, sillimanite, and andalusite, located in a mapping of the (3, −3) critical points displayed by their L(r) = −∇²ρ(r) distributions, are compared with polarized single-crystal FTIR spectra of kyanite and sillimanite determined earlier and with andalusite measured in this study. For andalusite, seven peaks were observed when the electric vector, E, is parallel to [100]: four intense ones at 3,440, 3,460, 3,526, and 3,597 cm⁻¹ and three weaker ones at 3,480, 3,520, and 3,653 cm⁻¹. Six peaks, three intense ones at 3,440, 3,460, and 3,526 cm⁻¹ and three weaker ones at 3,480, 3,520, and 3,653 cm⁻¹ when E parallels [010]. No peaks were observed when E is parallel to [001]. The concentration of water in andalusite varies between 110 and 168 ppm by weight % H₂O. Polarized FTIR spectra indicate that the OH vector is parallel to (001) in andalusite and sillimanite and in kyanite. Examination of the L(r) (3, −3) critical points in comparison with the polarized FTIR indicates that H prefers to bond to the oxygen atoms O1 and O2 in andalusite and O2 and O4 in sillimanite which correspond to the underbonded oxygen atoms and those with the largest L(r) maxima. In kyanite, comparison of the FTIR spectrum and the critical points indicates that H will preferentially bond to the two 4-coordinated O2 and O6 atoms.  相似文献   

Statistical evaluation of PM<Subscript>10</Subscript> and distribution of PM<Subscript>1</Subscript>, PM<Subscript>2.5</Subscript>, and PM<Subscript>10</Subscript> in ambient air due to extreme fireworks episodes (Deepawali festivals) in megacity Delhi     

S. Tiwari  D. M. Chate  M. K. Srivastava  P. D. Safai  A. K. Srivastava  D. S. Bisht  B. Padmanabhamurty 《Natural Hazards》2012,61(2):521-531

Temporal variation of PM₁₀ using 2-year data (January, 2007–December, 2008) of Delhi is presented. PM₁₀ varied from 42 to 200 μg m⁻³ over January to December, with an average 114.1 ± 81.1 μg m⁻³. They are comparable with the data collected by Central Pollution Control Board (National Agency which monitors data over the entire country in India) and are lower than National Ambient Air Quality (NAAQ) standard during monsoon, close to NAAQ during summer but higher in winter. Among CO, NO₂, SO₂, rainfall, temperature, and wind speed, PM₁₀ shows good correlation with CO. Also, PM₁₀, PM_2.5, and PM₁ levels on Deepawali days when fireworks were displayed are presented. In these festive days, PM₁₀, PM_2.5, and PM₁ levels were 723, 588, and 536 μg m⁻³ in 2007 and 501, 389, and 346 μg m⁻³ in 2008. PM₁₀, PM_2.5, and PM₁ levels in 2008 were 1.5 times lower than those in 2007 probably due to higher mixing height (446 m), temperature (23.8°C), and winds (0.36 ms⁻¹).  相似文献   

The influence of degradation of the swamp and alpine meadows on CH<Subscript>4</Subscript> and CO<Subscript>2</Subscript> fluxes on the Qinghai-Tibetan Plateau     

Junfeng Wang  Genxu Wang  Hongchang Hu  Qingbai Wu 《Environmental Earth Sciences》2010,60(3):537-548

CH₄ and CO₂ fluxes from a high-cold swamp meadow and an alpine meadow on the Qinghai-Tibetan Plateau, subject to different degrees of degradation, were measured over a 12-month period. Air temperature, soil temperature and moisture, and the depths of the water table and thawing-freezing layer were determined. For swamp meadows, the greater the degradation, the lesser the carbon efflux. CH₄ emissions at the nondegraded swamp meadow site were 1.09–3.5 and 2.5–11.27 times greater, and CO₂ emissions 1.08–1.69 and 1.41–4.43 times greater, respectively, than those from moderately and severely degraded sites. For alpine meadows, the greater the degradation, the greater the CH₄ consumption and CO₂ emissions. CH₄ consumption at the severely degraded alpine meadow site was 6.6–21 and 1.1–5.25 times greater, and CO₂ emissions 1.05–78.5 and 1.04–6.28 times greater, respectively, than those from the nondegraded and moderately degraded sites. The CH₄ and CO₂ fluxes at both sites were significantly correlated (R ² > 0.59, P < 0.05) with air temperature, soil temperature, and topsoil (0–5 cm depth) moisture, indicating these to be the main environmental factors affecting such fluxes.  相似文献   

Nitrous oxide (N<Subscript>2</Subscript>O) emissions from a mesotrophic reservoir on the Wujiang River,southwest China     

Xiaolong Liu  Siliang Li  Zhongliang Wang  Guilin Han  Jun Li  Baoli Wang  Fushun Wang  Li Bai 《中国地球化学学报》2017,36(4):667-679

Aquatic ecosystems have been identified as a globally significant source of nitrous oxide (N₂O) due to continuous active nitrogen involvement, but the processes and influencing factors that control N₂O production are still poorly understood, especially in reservoirs. For that, monthly N₂O variations were monitored in Dongfeng reservoir (DFR) with a mesotrophic condition. The dissolved N₂O concentration in DFR displayed a distinct spatial–temporal pattern but lower than that in the eutrophic reservoirs. During the whole sampling year, N₂O saturation ranging from 144% to 640%, indicating that reservoir acted as source of atmospheric N₂O. N₂O production is induced by the introduction of nitrogen (NO₃ ^?, NH₄ ⁺) in mesotrophic reservoirs, and is also affected by oxygen level and water temperature. Nitrification was the predominate process for N₂O production in DFR due to well-oxygenated longitudinal water layers. Mean values of estimated N₂O flux from the air–water interface averaged 0.19 µmol m^?2 h^?1 with a range of 0.01–0.61 µmol m^?2 h^?1. DFR exhibited less N₂O emission flux than that reported in a nearby eutrophic reservoir, but still acted as a moderate N₂O source compared with other reservoirs and lakes worldwide. Annual emissions from the water–air interface of DFR were estimated to be 0.32 × 10⁵ mol N–N₂O, while N₂O degassing from releasing water behind the dam during power generation was nearly five times greater. Hence, N₂O degassing behind the dam should be taken into account for estimation of N₂O emissions from artificial reservoirs, an omission that historically has probably resulted in underestimates. IPCC methodology should consider more specifically N₂O emission estimation in aquatic ecosystems, especially in reservoirs, the default EF5 model will lead to an overestimation.  相似文献   

Inorganic nitrogen dynamics in intertidal rocky biofilms and sediments of the Douro River estuary (Portugal)   总被引：1，自引：0，他引：1  

Catarina M. Magalhäes  William J. Wiebe  Samantha B. Joye  Adriano A. Bordalo 《Estuaries and Coasts》2005,28(4):592-607

In this study rates of oxygen, ammonium (NH₄ ⁺), nitrate (NO₃ ⁻), nitrite (NO₂ ⁻), and nitrous oxide (N₂O) fluxes, nitrogen (N) fixation, nitrification, and denitrification were compared between two intertidal sites for which there is an abundant global literature, muddy and sandy sediments, and two sites representing the rocky intertidal zone where biogeochemical processes have scarcely been investigated. In almost all sites oxygen production rates greatly exceeded oxygen consumption rates. During daylight, NH₄ ⁺ and NO₃ ⁻ uptake rates together with ammonification could supply the different N requirements of the primary producer communities at all four sites; N assimilation by benthic or epilithic primary producers was the major process of dissolved inorganic nitrogen (DIN) removal; N fixation, nitrification, and denitrification were minor processes in the overall light DIN cycle. At night, distinct DIN cycling processes took place in the four environments, denitrification rates ranged from 9 ± 2 to 360 ± 30 μmol N₂ m⁻² h⁻¹, accounting for 10–48% of the water column NO₃ ⁻ uptake; nitrification rates varied from 0 to 1712 ± 666 μmol NH₄ ⁺ m⁻² h⁻¹. A conceptual model of N cycle dynamics showed major differences between intertidal sediment and rocky sites in terms of the mean rates of DIN net fluxes and the processes involved, with rocky biofilm showing generally higher fluxes. Of particular significance, the intertidal rocky biofilms released 10 times the amount of N₂O produced in intertidal sediments (up to 17 ± 6 μmol N₂O m⁻² h⁻¹), representing the highest N₂O release rates ever recorded for marine systems. The biogeochemical contributions of intertidal rocky substrata to estuarine and coastal processes warrant future detailed investigation.  相似文献   

Diel Aquatic CO<Subscript>2</Subscript> System Dynamics of a Bermudian Mangrove Environment     

John A. Zablocki  Andreas J. Andersson  Nicholas R. Bates 《Aquatic Geochemistry》2011,17(6):841-859

Mangrove ecosystems play an important, but understudied, role in the cycling of carbon in tropical and subtropical coastal ocean environments. In the present study, we examined the diel dynamics of seawater carbon dioxide (CO₂) and dissolved oxygen (DO) for a mangrove-dominated marine ecosystem (Mangrove Bay) and an adjacent intracoastal waterway (Ferry Reach) on the island of Bermuda. Spatial and temporal trends in seawater carbonate chemistry and associated variables were assessed from direct measurements of dissolved inorganic carbon, total alkalinity, dissolved oxygen (DO), temperature, and salinity. Diel pCO₂ variability was interpolated across hourly wind speed measurements to determine variability in daily CO₂ fluxes for the month of October 2007 in Bermuda. From these observations, we estimated rates of net sea to air CO₂ exchange for these two coastal ecosystems at 59.8 ± 17.3 in Mangrove Bay and 5.5 ± 1.3 mmol m⁻² d⁻¹ in Ferry Reach. These results highlight the potential for large differences in carbonate system functioning and sea-air CO₂ flux in adjacent coastal environments. In addition, observation of large diel variability in CO₂ system parameters (e.g., mean pCO₂: 390–2,841 μatm; mean pH_T: 8.05–7.34) underscores the need for careful consideration of diel cycles in long-term sampling regimes and flux estimates.  相似文献   

LiFeSi<Subscript>2</Subscript>O<Subscript>6</Subscript> and NaFeSi<Subscript>2</Subscript>O<Subscript>6</Subscript> at low temperatures: an infrared spectroscopic study     

M. Zhang  G. J. Redhammer  E. K. H. Salje  M. Mookherjee 《Physics and Chemistry of Minerals》2002,29(9):609-616

 Synthetic aegirine LiFeSi₂O₆ and NaFeSi₂O₆ were characterized using infrared spectroscopy in the frequency range 50–2000 cm⁻¹, and at temperatures between 20 and 300 K. For the C2/c phase of LiFeSi₂O₆, 25 of the 27 predicted infrared bands and 26 of 30 predicted Raman bands are recorded at room temperature. NaFeSi₂O₆ (with symmetry C2/c) shows 25 infrared and 26 Raman bands. On cooling, the C2/c–P2₁/c structural phase transition of LiFeSi₂O₆ is characterized by the appearance of 13 additional recorded peaks. This observation indicates the enlargement of the unit cell at the transition point. The appearance of an extra band near 688 cm⁻¹ in the monoclinic P2₁/c phase, which is due to the Si–O–Si vibration in the Si₂O₆ chains, indicates that there are two non-equivalent Si sites with different Si–O bond lengths. Most significant spectral changes appear in the far-infrared region, where Li–O and Fe–O vibrations are mainly located. Infrared bands between 300 and 330 cm⁻¹ show unusually dramatic changes at temperatures far below the transition. Compared with the infrared data of NaFeSi₂O₆ measured at low temperatures, the change in LiFeSi₂O₆ is interpreted as the consequence of mode crossing in the frequency region. A generalized Landau theory was used to analyze the order parameter of the C2/c–P2₁/c phase transition, and the results suggest that the transition is close to tricritical. Received: 21 January 2002 / Accepted: 22 July 2002  相似文献   

Denitrification and the stoichiometry of nutrient regeneration in Waquoit Bay, Massachusetts     

Michael G. LaMontagne  Valeria Astorga  Anne E. Giblin  Ivan Valiela 《Estuaries and Coasts》2002,25(2):272-281

To determine the removal of regenerated nitrogen by estuarine sediments, we compared sediment N₂ fluxes to the stoichiometry of nutrient and O₂ fluxes in cores collected in the Childs River, Cape Cod, Massachusetts. The difference between the annual PO₄ ³⁻ (0.2 mol P m⁻² yr⁻¹) and NH₄ ⁺ (1.6 mol N m⁻² yr⁻¹) flux and the Redfield N∶P ratio of 16 suggested an annual deficit of 1.5 mol N m⁻² yr⁻¹. Denitrification predicted from O₂∶NH₄ ⁺ flux ratios and measured as N₂ flux suggested a nitrogen sink of roughly the same magnitude (1.4 mol N m⁻² yr⁻¹). Denitrification accounted for low N∶P ratios of benthic flux and removed 32–37% of nitrogen inputs entering the relatively highly nutrient loaded Childs River, despite a relatively brief residence time for freshwater in this system. Uptake of bottom water nitrate could only supply a fraction of the observed N₂ flux. Removal of regenerated nitrogen by denitrification in this system appears to vary seasonally. Denitrification efficiency was inversely correlated with oxygen and ammonium flux and was lowest in summer. We investigated the effect of organic matter on denitrification by simulating phytoplankton deposition to cores incubated in the lab and by deploying chambers on bare and macroaglae covered sediments in the field. Organic matter addition to sediments increased N₂ flux and did not alter denitrification efficiency. Increased N₂ flux co-varied with O₂ and NH₄ ⁺ fluxes. N₂ flux (261±60 μmol m⁻² h⁻¹) was lower in chambers deployed on macroalgal beds than deployed on bare sediments (458±70 μmol m⁻² h⁻¹), and O₂ uptake rate was higher in chambers deployed on macroalgal beds (14.6±2.2 mmol m⁻² h⁻¹) than on bare sediments (9.6±1.5 mmol m⁻² h⁻¹). Macroalgal cover, which can retain nitrogen in the system, is a link between nutrient loading and denitrification. Decreased denitrification due to increasing macroalgal cover could create a positive feedback because decreasing denitrification would increase nitrogen availability and could increase macroalgae cover.  相似文献   

CO<Subscript>2</Subscript>-rich fluid inclusions with chalcopyrite daughter mineral from the Fenghuangshan Cu–Fe–Au deposit,China: implications for metal transport in vapor     

Jianqing Lai  Guoxiang Chi 《Mineralium Deposita》2007,42(3):293-299

CO₂-rich fluid inclusions containing opaque mineral crystals were found in the Fenghuangshan skarn-porphyry Cu–Fe–Au deposit in Tongling, Anhui, China. These inclusions show variable CO₂ contents and are accompanied by aqueous inclusions, both occurring as secondary inclusions in quartz and being locally associated with chalcopyrite mineralization. Laser Raman microspectroscopic analyses confirm the predominance of CO₂ in the vapor and the presence of H₂S as high as 8 mol%, and identify the opaque mineral with yellow reflectance color in the inclusions as chalcopyrite. More than half of the CO₂-bearing inclusions contains chalcopyrite, whereas few of the associated aqueous inclusions do so. The chalcopyrite, occupying less than 1% (volume) of the inclusions, is interpreted to be a daughter mineral, and calculated Cu concentrations in the inclusions range from 0.1 to 3.4 wt%. Copper is inferred to have been transported in CO₂-dominated fluids as HS⁻ complexes. The occurrence of chalcopyrite daughter crystals in CO₂-rich fluid inclusions indicates that CO₂-rich vapor has the capacity of transporting large amounts of Cu, and possibly Au. This finding has significant implications for metal transport and mineralization in hydrothermal systems enriched in CO₂, such as orogenic-type and granitic intrusion-related gold deposits.  相似文献