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661.
Wenyi Zhu Nathan Yee E. Danielle Rhine John R. Reinfelder 《Geochimica et cosmochimica acta》2008,72(21):5243-5250
We examined the hypothesis that sulfide drives arsenic mobilization from pyritic black shale by a sulfide-arsenide exchange and oxidation reaction in which sulfide replaces arsenic in arsenopyrite forming pyrite, and arsenide (As−1) is concurrently oxidized to soluble arsenite (As+3). This hypothesis was tested in a series of sulfide-arsenide exchange experiments with arsenopyrite (FeAsS), homogenized black shale from the Newark Basin (Lockatong formation), and pyrite isolated from Newark Basin black shale incubated under oxic (21% O2), hypoxic (2% O2, 98% N2), and anoxic (5% H2, 95% N2) conditions. The oxidation state of arsenic in Newark Basin black shale pyrite was determined using X-ray absorption-near edge structure spectroscopy (XANES). Incubation results show that sulfide (1 mM initial concentration) increases arsenic mobilization to the dissolved phase from all three solids under oxic and hypoxic, but not anoxic conditions. Indeed under oxic and hypoxic conditions, the presence of sulfide resulted in the mobilization in 48 h of 13-16 times more arsenic from arsenopyrite and 6-11 times more arsenic from isolated black shale pyrite than in sulfide-free controls. XANES results show that arsenic in Newark Basin black shale pyrite has the same oxidation state as that in FeAsS (−1) and thus extend the sulfide-arsenide exchange mechanism of arsenic mobilization to sedimentary rock, black shale pyrite. Biologically active incubations of whole black shale and its resident microorganisms under sulfate reducing conditions resulted in sevenfold higher mobilization of soluble arsenic than sterile controls. Taken together, our results indicate that sulfide-driven arsenic mobilization would be most important under conditions of redox disequilibrium, such as when sulfate-reducing bacteria release sulfide into oxic groundwater, and that microbial sulfide production is expected to enhance arsenic mobilization in sedimentary rock aquifers with major pyrite-bearing, black shale formations. 相似文献
662.
Microbial mass-dependent fractionation of chromium isotopes 总被引:1,自引:0,他引:1
Eric R. Sikora Thomas M. Johnson Thomas D. Bullen 《Geochimica et cosmochimica acta》2008,72(15):3631-3641
Mass-dependent fractionation of Cr isotopes occurs during dissimilatory Cr(VI) reduction by Shewanella oneidensis strain MR-1. Cells suspended in a simple buffer solution, with various concentrations of lactate or formate added as electron donor, reduced 5 or 10 μM Cr(VI) to Cr(III) over days to weeks. In all nine batch experiments, 53Cr/52Cr ratios of the unreacted Cr(VI) increased as reduction proceeded. In eight experiments covering a range of added donor concentrations up to 100 μM, isotopic fractionation factors were nearly invariant, ranging from 1.0040 to 1.0045, with a mean value somewhat larger than that previously reported for abiotic Cr(VI) reduction (1.0034). One experiment containing much greater donor concentration (10 mM lactate) reduced Cr(VI) much faster and exhibited a lesser fractionation factor (1.0018). These results indicate that 53Cr/52Cr measurements should be effective as indicators of Cr(VI) reduction, either bacterial or abiotic. However, variability in the fractionation factor is poorly constrained and should be studied for a variety of microbial and abiotic reduction pathways. 相似文献
663.
Adélie Delacour Gretchen L. Früh-Green Deborah S. Kelley 《Geochimica et cosmochimica acta》2008,72(20):5090-5110
Variations in sulfur mineralogy and chemistry of serpentinized peridotites and gabbros beneath the Lost City Hydrothermal Field at the southern face of the Atlantis Massif (Mid-Atlantic Ridge, 30°N) were examined to better understand serpentinization and alteration processes and to study fluid fluxes, redox conditions, and the influence of microbial activity in this active, peridotite-hosted hydrothermal system. The serpentinized peridotites are characterized by low total sulfur contents and high bulk δ34S values close to seawater composition. Low concentrations of 34S-enriched sulfide phases and the predominance of sulfate with seawater-like δ34S values indicate oxidation, loss of sulfide minerals and incorporation of seawater sulfate into the serpentinites. The predominance of pyrite in both serpentinites and gabbros indicates relatively high fO2 conditions during progressive serpentinization and alteration, which likely result from high fluid fluxes during hydrothermal circulation and evolution of the Lost City system from temperatures of ∼250 to 150 °C. Sulfate and sulfide minerals in samples from near the base of hydrothermal carbonate towers at Lost City show δ34S values that reflect the influence of microbial activity. Our study highlights the variations in sulfur chemistry of serpentinized peridotites in different marine environments and the influence of long-lived, moderate temperature peridotite-hosted hydrothermal system and high seawater fluxes on the global sulfur cycle. 相似文献
664.
Sulfur mineralogy and geochemistry of serpentinites and gabbros of the Atlantis Massif (IODP Site U1309) 总被引:3,自引:0,他引:3
In-situ uplifted portions of oceanic crust at the central dome of the Atlantis Massif (Mid-Atlantic Ridge, 30°N) were drilled during Expeditions 304 and 305 of the Integrated Ocean Drilling Program (IODP) and a 1.4 km section of predominantly gabbroic rocks with minor intercalated ultramafic rocks were recovered. Here we characterize variations in sulfur mineralogy and geochemistry of selected samples of serpentinized peridotites, olivine-rich troctolites and diverse gabbroic rocks recovered from Hole 1309D. These data are used to constrain alteration processes and redox conditions and are compared with the basement rocks of the southern wall of the Atlantis Massif, which hosts the Lost City Hydrothermal Field, 5 km to the south. The oceanic crust at the central dome is characterized by Ni-rich sulfides reflecting reducing conditions and limited seawater circulation. During uplift and exhumation, seawater interaction in gabbroic-dominated domains was limited, as indicated by homogeneous mantle-like sulfur contents and isotope compositions of gabbroic rocks and olivine-rich troctolites. Local variations from mantle compositions are related to magmatic variability or to interaction with seawater-derived fluids channeled along fault zones. The concomitant occurrence of mackinawite in olivine-rich troctolites and an anhydrite vein in a gabbro provide temperature constraints of 150-200 °C for late circulating fluids along local brittle faults below 700 m depth. In contrast, the ultramafic lithologies at the central dome represent domains with higher seawater fluxes and higher degrees of alteration and show distinct changes in sulfur geochemistry. The serpentinites in the upper part of the hole are characterized by high total sulfide contents, high δ34Ssulfide values and low δ34Ssulfate values, which reflect a multistage history primarily controlled by seawater-gabbro interaction and subsequent serpentinization. The basement rocks at the central dome record lower oxygen fugacities and more limited fluid fluxes compared with the serpentinites and gabbros of the Lost City hydrothermal system. Our studies are consistent with previous results and indicate that sulfur speciation and sulfur isotope compositions of altered oceanic mantle sequences commonly evolve over time. Heterogeneities in sulfur geochemistry reflect the fact that serpentinites are highly sensitive to local variations in fluid fluxes, temperature, oxygen and sulfur fugacities, and microbial activity. 相似文献
665.
A.K. Sokol V.A. Fernandes T. Schulz A. Bischoff R.N. Clayton K. Nishiizumi L. Schultz K. Mezger 《Geochimica et cosmochimica acta》2008,72(19):4845-4873
Kalahari 008 and 009 are two lunar meteorites that were found close to each other in Botswana. Kalahari 008 is a typical lunar anorthositic breccia; Kalahari 009 a monomict breccia with basaltic composition and mineralogy. Based on minor and trace elements Kalahari 009 is classified as VLT (very-low-Ti) mare basalt with extremely low contents of incompatible elements, including the REE. The Lu-Hf data define an age of 4286 ± 95 Ma indicating that Kalahari 009 is one of the oldest known basalt samples from the Moon. It provides evidence for lunar basalt volcanism prior to 4.1 Ga (pre-Nectarian) and may represent the first sample from a cryptomare. The very radiogenic initial 176Hf/177Hf (εHf = +12.9 ± 4.6), the low REE, Th and Ti concentrations indicate that Kalahari 009 formed from re-melting of mantle material that had undergone strong incompatible trace element depletion early in lunar history. This unusually depleted composition points toward a hitherto unsampled basalt source region for the lunar interior that may represent a new depleted endmember source for low-Ti mare basalt volcanism. Apparently, the Moon became chemically very heterogeneous at an early stage in its history and different cumulate sources are responsible for the diverse mare basalt types.Evidence that Kalahari 008 and 009 may be paired includes the similar fayalite content of their olivine, the identical initial Hf isotope composition, the exceptionally low exposure ages of both rocks and the fact that they were found close to each other. Since cryptomaria are covered by highland ejecta, it is possible that these rocks are from the boundary area, where basalt deposits are covered by highland ejecta. The concentrations of cosmogenic radionuclides and trapped noble gases are unusually low in both rocks, although Kalahari 008 contains slightly higher concentrations. A likely reason for this difference is that Kalahari 008 is a polymict breccia containing a briefly exposed regolith, while Kalahari 009 is a monomict brecciated rock that may never have been at the surface of the Moon.Altogether, the compositions of Kalahari 008 and 009 permit new insight into early lunar evolution, as both meteorites sample lunar reservoirs hitherto unsampled by spacecraft missions. The very low Th and REE content of Kalahari 009 as well as the depletion in Sm and the lack of a KREEP-like signature in Kalahari 008 point to a possible source far from the influence of the Procellarum-KREEP Terrane, possibly the lunar farside. 相似文献
666.
Thermodynamic model for arsenic speciation in sulfidic waters: A novel use of ab initio computations
Recent discoveries demonstrate that the chemistry of arsenic in sulfidic waters is much more complex that previously believed. One implication is that all earlier thermodynamic data on stabilities of As thioanions require revision. Previously used experimental approaches for determining As thioanion stabilities may be inadequate to deal with the full range of complexity. Here we use computational as well as empirical information to construct a provisional model for equilibrium As thioanion distributions in sulfidic waters. Whereas previous authors have argued for either As(III) or As(V) thioanions, the new model predicts that both are important and can occur simultaneously under commonly encountered pH and ΣS−II conditions. At the order of magnitude level, the model reasonably predicts the solubility of As2S3 in sulfidic solutions, provides tentative peak assignments for published Raman spectroscopic data and plausibly accounts for how sulfide modifies the bacterial toxicity of As. The model yields a thermodynamic justification for how sulfide, which is usually regarded as a reducing agent, can counter-intuitively drive oxidation of As(III) to As(V), as has been observed both in the laboratory and in the field. Despite its uncertain accuracy, the model serves as a useful source of new, testable hypotheses about As geochemistry and highlights crucial experimental data needs. 相似文献
667.
668.
Establishing the petrogenesis of volcanic and plutonic rocksis a key issue in unraveling the evolution of distinct subduction-relatedtectonic phases occurring along the South American margin. Thisis particularly true for Cenozoic times when large volumes ofmagma were produced in the Andean belt. In this study we havefocused on Oligo-Miocene magmatism in central Chile at 33°S.Our data include field and petrographic observations, whole-rockmajor and trace element analyses, U–Pb zircon dating,and Pb, Sr, and Hf isotope analyses of plagioclase, clinopyroxene,and zircon mineral separates. Combined with earlier dating resultsthe new zircon ages define a 28·8–5·2 Maperiod of plutonic and volcanic activity that ceased as a consequenceof flattening subduction of the Nazca–Farallon plate.Rare earth elements patterns are variable, with up to 92 timeschondrite concentrations for light rare earth elements yielding(La/Yb)N between 3·6 and 7·0, and an absence ofEu anomalies. Initial Pb isotope signatures are in the rangeof 18·358–19·023 for 206Pb/ 204Pb, 15·567–15·700for 207Pb/ 204Pb and 38·249–39·084 for 208Pb/204Pb. Initial 87Sr/ 86Sr are mostly in the range of 0·70369–0·70505,with two more radiogenic values at 0·7066. Initial Hfisotopic compositions of zircons yield exclusively positiveHfi ranging between + 6·9 and + 9·6. The newlydetermined initial isotope characteristics of the Oligo-Miocenemagmas suggest that the mantle source lithologies are differentfrom both those of Pacific mid-ocean ridge basalt and oceanisland basalt, plotting in the field of reference values forsubcontinental lithospheric mantle, characterized by moderatelarge ion lithophile element–high field strengh elementdepletion and high 238U/ 204Pb. A Hf model age of 2 Ga is estimatedfor the formation of the subcontinental mantle–continentalcrust assemblage in the region, suggesting that the initialSr and Pb isotope ratios inferred for the source of the Oligo-Mioceneparental magmas are the result of later Rb and U enrichmentcaused by mantle metasomatism. A time-integrated model Rb/Srof 0·039 and µ 16 are estimated for the sourceof the parental magmas, consistent with ratios measured in peridotitexenoliths from continental areas. Evolution from predominant(>90%) basaltic–gabbroic to andesitic–dioriticmagmas seems to involve a combination of (1) original traceelement differences in the metasomatized subcontinental mantle,(2) different degrees of partial melting and (3) fractionalcrystallization in the garnet- and spinel-peridotite stabilityfields. The genesis of more differentiated magmas reaching rhyolitic–graniticcompositions most probably also includes additional crystalfractionation at both shallow mantle depths and within the crust,possibly leading to some very minor assimilation of crustalmaterial. KEY WORDS: calc-alkaline magmatism; Oligo-Miocene; U–Pb dating; Sr–Pb–Hf isotopes; central Chile 相似文献
669.
The structure of anomalously uplifted areas in transverse ridges of the Vema, S o Paulo, and Romanche fracture zones is considered. It is concluded that their formation and eventual development in the present-day structure of the central Atlantic bottom proceeded during two stages. The first stage that corresponds to a short period at the Tortonian-Messinian transition (10 Ma ago) was marked by transportation of deep-seated rocks into the upper part of the lithosphere along thrust faults with mass motion in the meridional direction along the axis of the Mid-Atlantic Ridge. The second stage was characterized by contrasting highamplitude vertical movements from 10 to 3 Ma ago. It is suggested that near-meridional compression in the domains surrounding the Western Tethys in the Tortonian-Messinian resulted in deformation of the upper lithosphere within large transform fracture zones of the central Atlantic. The deformation that occurred 10 Ma ago was a manifestation of the global neotectonic epoch of the Earth. 相似文献
670.
A. van Geen K. Radloff Z. Aziz Z. Cheng M.R. Huq K.M. Ahmed B. Weinman S. Goodbred H.B. Jung Y. Zheng M. Berg P.T.K. Trang L. Charlet J. Metral D. Tisserand S. Guillot S. Chakraborty A.P. Gajurel B.N. Upreti 《Applied Geochemistry》2008
One of the reasons the processes resulting in As release to groundwater in southern Asia remain poorly understood is the high degree of spatial variability of physical and chemical properties in shallow aquifers. In an attempt to overcome this difficulty, a simple device that collects groundwater and sediment as a slurry from precisely the same interval was developed in Bangladesh. Recently published results from Bangladesh and India relying on the needle-sampler are augmented here with new data from 37 intervals of grey aquifer material of likely Holocene age in Vietnam and Nepal. A total of 145 samples of filtered groundwater ranging in depth from 3 to 36 m that were analyzed for As (1–1000 μg/L), Fe (0.01–40 mg/L), Mn (0.2–4 mg/L) and S (0.04–14 mg/L) are compared. The P-extractable (0.01–36 mg/kg) and HCl-extractable As (0.04–36 mg/kg) content of the particulate phase was determined in the same suite of samples, in addition to Fe(II)/Fe ratios (0.2–1.0) in the acid-leachable fraction of the particulate phase. Needle-sampler data from Bangladesh indicated a relationship between dissolved As in groundwater and P-extractable As in the particulate phase that was interpreted as an indication of adsorptive equilibrium, under sufficiently reducing conditions, across 3 orders of magnitude in concentrations according to a distribution coefficient of 4 mL/g. The more recent observations from India, Vietnam and Nepal show groundwater As concentrations that are often an order of magnitude lower at a given level of P-extractable As compared to Bangladesh, even if only the subset of particularly reducing intervals characterized by leachable Fe(II)/Fe >0.5 and dissolved Fe >0.2 mg/L are considered. Without attempting to explain why As appears to be particularly mobile in reducing aquifers of Bangladesh compared to the other regions, the consequences of increasing the distribution coefficient for As between the particulate and dissolved phase to 40 mL/g for the flushing of shallow aquifers of their initial As content are explored. 相似文献