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1.
Multiple sulfur isotope system is a powerful new tracer for atmospheric, volcanic, and biological influences on sulfur cycles in the anoxic early Earth. Here, we report high-precision quadruple sulfur isotope analyses (32S/33S/34S/36S) of barite, pyrite in barite, and sulfides in related hydrothermal and igneous rocks occurring in the ca. 3.5 Ga Dresser Formation, Western Australia. Our results indicate that observed isotopic variations are mainly controlled by mixing of mass-dependently (MD) and non-mass-dependently fractionated (non-MD) sulfur reservoirs. Based on the quadruple sulfur isotope systematics (δ34S-Δ33S-Δ36S) for these minerals, four end-member sulfur reservoirs have been recognized: (1) non-MD sulfate (δ34S = −5 ± 2‰; Δ33S = −3 ± 1‰); (2) MD sulfate (δ34S = +10 ± 3‰); (3) non-MD sulfur (δ34S > +6‰; Δ33S > +4‰); and (4) igneous MD sulfur (δ34S = Δ33S = 0‰). The first and third components show a clear non-MD signatures, thus probably represent sulfate and sulfur aerosol inputs. The MD sulfate component (2) is enriched in 34S (+10 ± 3‰) and may have originated from microbial and/or abiotic disproportionation of volcanic S or SO2. Our results reconfirm that the Dresser barites contain small amounts of pyrite depleted in 34S by 15-22‰ relative to the host barite. These barite-pyrite pairs exhibit a mass-dependent relationship of δ33S/δ34S with slope less than 0.512, which is consistent with that expected for microbial sulfate reduction and is significantly different from that of equilibrium fractionation (0.515). The barite-pyrite pairs also show up to 1‰ difference in Δ36S values and steep Δ36S/Δ33S slopes, which deviate from the main Archean array (Δ36S/Δ33S = −0.9) and are comparable to isotope effects exhibited by sulfate reducing microbes (Δ36S/Δ33S = −5 to −11). These new lines of evidence support the existence of sulfate reducers at ca. 3.5 Ga, whereas microbial sulfur disproportionation may have been more limited than recently suggested.  相似文献   
2.
Radiocarbon and total carbonate data were obtained near the 1973 GEOSECS stations in the North Pacific along 30°N and along 175°E between 1993 and 1994. In these stations, we estimated radiocarbon originating from atomic bomb tests using tritium, trichlorofluoromethane and silicate contents. The average penetration depth of bomb radiocarbon during the two decades has deepened from 900 m to 1300 m. Bomb radiocarbon inventories above the average value for the whole North Pacific were found widely in the western subtropical region around 30°N both in the 1970s and 1990s, and its area in the 1990s was broader than that in the 1970s. In most of the North Pacific, while the bomb radiocarbon has decreased above 25.4, the bomb radiocarbon flux below 25.4 was over 1 × 1012 atom m-2yr-1 in the subtropical region around 30°N. In the tropical area south of 20°N, the bomb radiocarbon inventory below 25.4 increased from zero to over 10 × 1012 atom m-2 during the last three decades. These distributions suggest that the bomb radiocarbon removed from the surface is currently accumulated with bomb 14C flux of over 1 × 1012 atom m-2yr-1 below 25.4 in the subtropical region, mainly by advection from the higher latitude, and that part of the accumulated bomb 14C gradually spread southward with about 30 years.  相似文献   
3.
Sea water samples were collected from various depths in the North Pacific (40–21°N) along 165°E in 1991. Their total carbonate (total dissolved carbonate species) contents were determined with random errors less than 0.2% by a coulometric method. The preformed carbonate contents defined by Chen (1982) were calculated from the obtained data and other observed data including potential temperature, salinity, dissolved oxygen and total alkalinity. The same calculation was done for the GEOSECS data obtained in nearly the same region in 1973. The difference between the two data sets reveals that the preformed carbonate has increased by 180±41 gC/m2 during the last 18 years. This value is comparable or somewhat larger than 150 gC/m2 obtained in the case that the ocean uptakes 3 GtC/yr for 18 years and distributes it equally among the world oceans. Based on the results, a hypothesis on the missing sink for the anthropogenic carbon dioxide is presented, in that the missing sink is the intermediate waters formed in the northern North Pacific and the Southern Ocean besides the deep waters formed in the North Atlantic and the Southern Ocean.  相似文献   
4.
A preliminary study of carbon system in the East China Sea   总被引:1,自引:0,他引:1  
In the central part of the East China Sea, the activity of CO2 in the surface water and total carbonate, pH and alkalinity in the water column were determined in winter and autumn of 1993. The activity of CO2 in the continental shelf water was about 50 ppm lower than that of surface air. This decrease corresponds to the absorption of about 40 gC/m2/yr of atmospheric CO2 in the coastal zone or 1 GtC/yr in the global continental shelf, if this rate is applicable to entire coastal seas. The normalized total carbonate contents were higher in the water near the coast and near the bottom. This increase toward the bottom may be due to the organic matter deposited on the bottom. This conclusion is supported by the distribution of pH. The normalized alkalinity distribution also showed higher values in the near-coast water, but in the surface water, indicating the supply of bicarbonate from river water. The residence time of the East China Sea water, including the Yellow Sea water, has been calculated to be about 0.8 yr from the excess alkalinity and the alkalinity input. Using this residence time and the excess carbonate, we can estimate that the amount of dissolved carbonate transported from the coastal zone to the oceanic basin is about 70 gC/m2/yr or 2 GtC/yr/area-of-global-continental-shelf. This also means that the rivers transport carbon to the oceans at a rate of 30 gC/m2/yr of the coastal sea or 0.8 GtC/yr/ area-of-global shelf, the carbon consisting of dissolved inorganic carbonate and terrestrial organic carbon decomposed on the continental shelf.  相似文献   
5.
Vertical distribution of anthropogenic carbon content of the water (exDIC) in the Oyashio area just outside of the Kuroshio/Oyashio Interfrontal Zone (K/O Zone) was estimated by the simple 1-D advection-diffusion model calibrated by the distribution of chlorofluorocarbons (CFCs). The average concentration of exDIC for = 26.60–27.00 is multiplied by the volume transport of Oyashio water into the North Pacific Intermediate Water (NPIW) to estimate the annual transport of exDIC into NPIW through K/O Zone. The estimated transport of exDIC was 0.018–0.020 GtC/y, which corresponds to 15% of the whole total exDIC accumulation in the temperate North Pacific. A simple assessment using the NPIW 1-box model indicates that the current study explains at least 70% of the total annual transport of exDIC into NPIW, and that small exDIC sources for NPIW still exists in addition to K/O Zone.  相似文献   
6.
We proposed an empirical equation of sea surface dimethylsulfide (DMS, nM) using sea surface temperature (SST, K), sea surface nitrate (SSN, μM) and latitude (L, °N) to reconstruct the sea surface flux of DMS over the North Pacific between 25°N and 55°N: ln DMS = 0.06346 · SST  0.1210 · SSN  14.11 · cos(L)  6.278 (R2 = 0.63, p < 0.0001). Applying our algorithm to climatological hydrographic data in the North Pacific, we reconstructed the climatological distributions of DMS and its flux between 25 °N and 55 °N. DMS generally increased eastward and northward, and DMS in the northeastern region became to 2–5 times as large as that in the southwestern region. DMS in the later half of the year was 2–4 times as large as that in the first half of the year. Moreover, applying our algorithm to hydrographic time series datasets in the western North Pacific from 1971 to 2000, we found that DMS in the last three decades has shown linear increasing trends of 0.03 ± 0.01 nM year− 1 in the subpolar region, and 0.01 ± 0.001 nM year− 1 in the subtropical region, indicating that the annual flux of DMS from sea to air has increased by 1.9–4.8 μmol m− 2 year− 1. The linear increase was consistent with the annual rate of increase of 1% of the climatological averaged flux in the western North Pacific in the last three decades.  相似文献   
7.
An ASCA observation of the Jovian impact of the comet Shoemaker-Levy 9 is reported. Four impacts of H, L, Q1 and R were observed and four impacts of B, C, G, and Q2 were observed within 60 minutes after their impacts. No significant flaring of X-ray emission was observed. Upper limit X-ray fluxes of 90 % confidence level, averaged 5 minutes just after the impacts, were 2.4 × 10–13 erg sec–1 cm–2, 3.5 × 10–13 erg sec–1 cm–2, 1.6 × 10–13 erg sec–1 cm–2 and 2.9 × 10–13 erg sec–1 cm–2 for the impacts of H, L, Q1 and R, respectively, in the 0.5(0.7 for H and Q1)–10 keV energy range. However, a hint of X-ray enhancement around Jupiter from July 17 to July 19 was detected with about 2 6 × 10–14 erg sec–1 cm–2 in the 0.5–10 keV energy range.  相似文献   
8.
Sulfur isotope studies of post-Archean terrestrial materials have focused on the ratio 34S/32S because additional isotopes, 33S and 36S, were thought to carry little information beyond the well-known mass-dependent relationship among multiple-isotope ratios. We report high-precision analyses of Δ33S and Δ36S values, defined as deviations of 33S and 36S from ideal mass-dependent relationships, for international reference materials and sedimentary sulfides of Phanerozoic age by using a fluorination technique with a dual-inlet isotope ratio mass spectrometer. Measured variations in Δ33S and Δ36S are explained as resulting from processes involve branching reactions (two or more reservoirs formed) or mixing. Irreversible processes in closed systems (Rayleigh distillation) amplify the isotope effect. We outline how this new isotope proxy can be used to gain new insights into fundamental aspects of the sulfur biogeochemical cycle, including additional constraints on seawater sulfate budget and processes in sedimentary sulfide formation. The isotope systematics discussed here cannot explain the much larger variation of Δ33S and Δ36S observed in Archean rock records. Furthermore, Phanerozoic samples we have studied show a characteristic Δ33S and Δ36S relationship that differs from those measured in Archean rocks and laboratory photolysis experiments. Thus, high precision analysis of Δ33S and Δ36S can be used to distinguish small non-zero Δ33S and Δ36S produced by mass-dependent processes from those produced by mass-independent processes in Archean rocks and extraterrestrial materials.  相似文献   
9.
We studied the temporal behavior of the background shallow seismicity rate in 700 circular areas across inland Japan. To search for and test the significance of the possible rate changes in background seismicity, we developed an efficient computational method that applies the space–time ETAS model proposed by Ogata in 1998 to the areas. Also, we conducted Monte Carlo tests using a simulated catalog to validate the model we applied. Our first finding was that the activation anomalies were found so frequently that the constant background seismicity hypothesis may not be appropriate and/or the triggered event model with constraints on the parameters may not adequately describe the observed seismicity. However, quiescence occasionally occurs merely by chance. Another outcome of our study was that we could automatically find several anomalous background seismicity rate changes associated with the occurrence of large earthquakes. Very significant seismic activation was found before the M6.1 Mt. Iwate earthquake of 1998. Also, possible seismic quiescence was found in an area 150 km southwest of the focal region of the M7.3 Western Tottori earthquake of 2000. The seismicity rate in the area recovered after the mainshock.  相似文献   
10.
Abstract. Oxidation and reduction processes can influence extent of leaching of elements from solid waste. Three samples of municipal solid waste combustion fly ash were subjected to oxidizing and reducing conditions in order to evaluate leaching of elements in the Milli-Q water and fly ash (liquid to solid ratio, 100) mixtures. Although the oxidizing and reducing conditions were applied for 6 hours only, elements like Cs, Li, Mg, Sb, Tl and V leached more under oxidizing condition than under reducing condition in the case of all three ash samples. Cadmium, Pb and Zn leached more from all samples under reducing condition than under oxidizing condition. Leaching of other elements like Al, Ba, Cr, Cu, Ni and Rb was inconsistent with oxidizing or reducing conditions and varied from sample to sample, suggesting that factors other than redox may be more important in controlling leaching of these elements. Strong acid neutralization capacity of the fly ash samples let the pH vary within a narrow range, and thus severely limited the extent of leaching during the course of the experiment. Lead and Zn were the most sensitive while K and Na were the least sensitive to changes in redox conditions.  相似文献   
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