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41.
Jaap S. Sinninghe Damst Marcel M.M. Kuypers Richard D. Pancost Stefan Schouten 《Organic Geochemistry》2008,39(12):1703
The stable carbon isotopic compositions of free and sulfur (S)-bound biomarkers derived from algae, (cyano)bacteria, archaea and higher plants and total organic carbon (TOC) during the first phase of the late Cenomanian/Turonian oceanic anoxic event (OAE) were measured in black shales deposited in the southern proto-Atlantic Ocean in the Cape Verde basin (DSDP Site 367) to determine the response of these organisms to this major perturbation of the global carbon cycle resulting from widespread burial of marine organic matter. The average positive isotope excursions of TOC and biomarkers varied from 5.1‰ to 8.3‰. The δ13C values were cross correlated to infer potential common sources of biomarkers. This revealed common sources for C31 and C32 hopanes but no 1:1 relationship for pristane and phytane. The correlation of δ13CTOC with the δ13C value of sulfur (S)-bound phytane is the strongest. This is because S-bound phytane is derived from phytol that originates from all marine primary producers (algae and cyanobacteria) and thus represents a weighted average of their carbon isotopic compositions. The δ13C values of S-bound phytane and C35 hopane were also used to estimate pCO2 levels. Before the OAE burial event, pCO2 levels are estimated to be ca. 1300 ppmv using both biomarkers and the independent maximum Rubisco fractionation factors. At times of maximum organic carbon burial rates during the OAE, reconstructed pCO2 levels are estimated to be ca. 700 ppmv. However, compared to other C/T OAE sections the positive isotope excursion of S-bound phytane is also affected by an increased production during the OAE. When we compensate for this, we arrive at pCO2 levels around 1000 ppmv, a reduction of ca. 25%. This indicates that burial of organic matter can have a large effect on atmospheric CO2 levels. 相似文献
42.
Olivier Harifidy Ralison Alberto Vieira Borges Frank Dehairs J.J. Middelburg Steven Bouillon 《Organic Geochemistry》2008,39(12):1649
Madagascar’s largest estuary (Betsiboka) was sampled along the salinity gradient during the dry season to document the distribution and sources of particulate and dissolved organic carbon (POC, DOC) as well as dissolved inorganic carbon (DIC). The Betsiboka was characterized by a relatively high suspended matter load, and in line with this, low DOC/POC ratios (0.4–2.5). The partial pressure of CO2 (pCO2) was generally above atmospheric equilibrium (270–1530 ppm), but relatively low in comparison to other tropical and subtropical estuaries, resulting in low average CO2 emission to the atmosphere (9.1 ± 14.2 mmol m−2 d−1). Despite the fact that C4 vegetation is reported to cover >80% of the catchment area, stable isotope data on DOC and POC suggest that C4 derived material comprises only 30% of both pools in the freshwater zone, increasing to 60–70% and 50–60%, respectively, in the oligohaline zone due to additional lateral inputs. Sediments from intertidal mangroves in the estuary showed low organic carbon concentrations (<1%) and δ13C values (average −19.8‰) consistent with important inputs of riverine imported C4 material. This contribution was reflected in δ13C signatures of bacterial phospholipid derived fatty acids (i + a15:0), suggesting the potential importance of terrestrial organic matter sources for mineralization and secondary production in coastal ecosystems. 相似文献
43.
Supercritical gas sorption on moist coals 总被引:2,自引:1,他引:1
The effect of moisture on the CO2 and CH4 sorption capacity of three bituminous coals from Australia and China was investigated at 55 °C and at pressures up to 20 MPa. A gravimetric apparatus was used to measure the gas adsorption isotherms of coal with moisture contents ranging from 0 to about 8%. A modified Dubinin–Radushkevich (DR) adsorption model was found to fit the experimental data under all conditions. Moisture adsorption isotherms of these coals were measured at 21 °C. The Guggenheim–Anderson–de Boer (GAB) model was capable of accurately representing the moisture isotherms over the full range of relative pressures.Moist coal had a significantly lower maximum sorption capacity for both CO2 and CH4 than dry coal. However, the extent to which the capacity was reduced was dependent upon the rank of the coal. Higher rank coals were less affected by the presence of moisture than low rank coals. All coals exhibited a certain moisture content beyond which further moisture did not affect the sorption capacity. This limiting moisture content was dependent on the rank of the coal and the sorbate gas and, for these coals, corresponded approximately to the equilibrium moisture content that would be attained by exposing the coal to about 40–80% relative humidity. The experimental results indicate that the loss of sorption capacity by the coal in the presence of water can be simply explained by volumetric displacement of the CO2 and CH4 by the water. Below the limiting moisture content, the CO2 sorption capacity reduced by about 7.3 kg t− 1 for each 1% increase in moisture. For CH4, sorption capacity was reduced by about 1.8 kg t− 1 for each 1% increase in moisture.The heat of sorption calculated from the DR model decreased slightly on addition of moisture. One explanation is that water is preferentially attracted to high energy adsorption sites (that have high energy by virtue of their electrostatic nature), expelling CO2 and CH4 molecules. 相似文献
44.
This paper presents results of a small scale study that utilized particle-tracking techniques to evaluate transport of river
water through an alluvial aquifer in a bank infiltration testing site in El Paso, Texas, USA. The particle-tracking survey
was used to better define filtration parameters. Several simulations were generated to allow visualization of the effects
of well placement and pumping rate on flow paths, travel time, the size of the pumping influence zone, and proportion of river-derived
water and groundwater mixing in the pumping well. Simulations indicate that migration of river water into the aquifer is generally
slow. Most water does not arrive at the well by the end of an 18-day pumping period at 0.54 m3/min pumping rate for a well located 18 m from the river. Forty-four percent of the water pumped from the well was river water.
The models provided important information needed to design appropriate sampling schedules for bank filtration practices and
ensured meeting adequate soil-retention times. The pumping rate has more effect on river water travel time than the location
of the pumping well from the river. The examples presented in this paper indicate that operating the pumping well at a doubled
distance from the river increased the time required for the water to travel to the well, but did not greatly change the capture
zone. 相似文献
45.
Geneviève Bordeleau Richard Martel Dirk Schäfer Guy Ampleman Sonia Thiboutot 《Environmental Geology》2008,55(2):385-396
Numerical modelling was done at the Cold Lake Air Weapons Range, Canada, to test whether the dissolved RDX and nitrate detected
in groundwater come from the same sources, and to predict whether contamination poses a threat to the surface water receptors
near the site. Military live fire training activities may indeed pose a risk of contamination to groundwater resources, however
field investigations on military bases are quite recent, and little information is available on the long-term behaviour of
munition residues related contaminants. Very limited information was available about the contaminant source zones, which were
assigned based on our knowledge of current training activities. The RDX plume was well represented with the model, but the
heterogeneous distribution of nitrate concentrations was more difficult to reproduce. It was nonetheless determined that both
contaminants originate from the same areas. According to the model, both contaminants should reach the nearby river, but concentrations
in the river should remain very low if the source zone concentration does not change. Finally, the model allowed the recommendation
of a new location for the main bombing target, which would offer added protection to the river and the lake into which it
flows. 相似文献
46.
Pedro J. Marenco Frank A. Corsetti Douglas E. Hammond Alan J. Kaufman David J. Bottjer 《Chemical Geology》2008,247(1-2):124-132
The sulfur isotopic composition of carbonate associated sulfate (CAS) has been used to investigate the geochemistry of ancient seawater sulfate. However, few studies have quantified the reliability of δ34S of CAS as a seawater sulfate proxy, especially with respect to later diagenetic overprinting. Pyrite, which typically has depleted δ34S values due to authigenic fractionation associated with bacterial sulfate reduction, is a common constituent of marine sedimentary rocks. The oxidation of pyrite, whether during diagenesis or sample preparation, could thus adversely influence the sulfur isotopic composition of CAS. Here, we report the results of CAS extractions using HCl and acetic acid with samples spiked with varying amounts of pyrite. The results show a very strong linear relationship between the abundance of fine-grained pyrite added to the sample and the resultant abundance and δ34S value of CAS. This data represents the first unequivocal evidence that pyrite is oxidized during the CAS extraction process. Our mixing models indicate that in samples with much less than 1 wt.% pyrite and relatively high δ34Spyrite values, the isotopic offset imparted by oxidation of pyrite should be much less than ? 4‰. A wealth of literature exists on the oxidation of pyrite by Fe3+ and we believe this mechanism drives the oxidation of pyrite during CAS extraction, during which the oxygen used to form sulfate is taken from H2O, not O2. Consequently, extracting CAS under anaerobic conditions would only slow, but not halt, the oxidation of pyrite. Future studies of CAS should attempt to quantify pyrite abundance and isotopic composition. 相似文献
47.
Mercury vapor (Hg0) emission from plants contributes to the atmospheric Hg cycle. Young barley (Hordeum vulgare L.) plants grown on a hydroponic cultivation medium containing Hg(II) have previously been shown to increase their Hg0 emission significantly by reduction of Hg(II) with endogenous ascorbic acid. Regarding the potential contribution to the Hg cycle from the vast forest-covered areas, it was important to investigate this mechanism in trees. The increase in Hg0 emission from young European beech plants cultivated on a HgCl2 medium exceeded that from controls by ca. tenfold and was proportional to the Hg(II) concentration. From these experiments, a flux of 12.8 μg Hg0/h/m2 was estimated at an exposure of the roots to 20 μM Hg(II). Mercury vapor release from homogenates of Norway spruce needles exceeded that from European beech leaves by a factor of 2.3–4, i.e. in proportion to the reported AA concentrations; the reduction was maximal at alkaline pH which is typical for AA. The 8.4-fold difference in Hg0 release between homogenates from wild-type Arabidopsis thaliana and from its AA-deficient mutant vtc 1-1 also paralleled the reported difference in AA levels of both species. It is concluded that the phytoreduction and vaporization of Hg by AA is an important mechanism as much for Hg detoxification in trees as for Hg emission to the atmosphere. The efficiency of this process seems to result from the optimal coordination of transfer and biochemical transformation of mercuric ions and Hg vapor. There is no evidence for a relevant difference in the mechanisms of biogenic Hg(II) reduction between grass plants and trees. 相似文献
48.
In order to evaluate thermodynamic speciation calculations inherent in biotic ligand models, the speciation of dissolved Cd, Cu, Pb, and Zn in aquatic systems influenced by historical mining activities is examined using equilibrium computer models and the diffusive gradients in thin films (DGT) technique. Several metal/organic-matter complexation models, including WHAM VI, NICA-Donnan, and Stockholm Humic model (SHM), are used in combination with inorganic speciation models to calculate the thermodynamic speciation of dissolved metals and concentrations of metal associated with biotic ligands (e.g., fish gills). Maximum dynamic metal concentrations, determined from total dissolved metal concentrations and thermodynamic speciation calculations, are compared with labile metal concentrations measured by DGT to assess which metal/organic-matter complexation model best describes metal speciation and, thereby, biotic ligand speciation, in the studied systems. Results indicate that the choice of model that defines metal/organic-matter interactions does not affect calculated concentrations of Cd and Zn associated with biotic ligands for geochemical conditions in the study area, whereas concentrations of Cu and Pb associated with biotic ligands depend on whether the speciation calculations use WHAM VI, NICA-Donnan, or SHM. Agreement between labile metal concentrations and dynamic metal concentrations occurs when WHAM VI is used to calculate Cu speciation and SHM is used to calculate Pb speciation. Additional work in systems that contain wide ranges in concentrations of multiple metals should incorporate analytical speciation methods, such as DGT, to constrain the speciation component of biotic ligand models. 相似文献
49.
50.
Joseph F. Whelan Leonid A. Neymark Richard J. Moscati Brian D. Marshall Edwin Roedder 《Applied Geochemistry》2008
Secondary calcite, silica and minor amounts of fluorite deposited in fractures and cavities record the chemistry, temperatures, and timing of past fluid movement in the unsaturated zone at Yucca Mountain, Nevada, the proposed site of a high-level radioactive waste repository. The distribution and geochemistry of these deposits are consistent with low-temperature precipitation from meteoric waters that infiltrated at the surface and percolated down through the unsaturated zone. However, the discovery of fluid inclusions in calcite with homogenization temperatures (Th) up to ∼80 °C was construed by some scientists as strong evidence for hydrothermal deposition. This paper reports the results of investigations to test the hypothesis of hydrothermal deposition and to determine the temperature and timing of secondary mineral deposition. Mineral precipitation temperatures in the unsaturated zone are estimated from calcite- and fluorite-hosted fluid inclusions and calcite δ18O values, and depositional timing is constrained by the 207Pb/235U ages of chalcedony or opal in the deposits. Fluid inclusion Th from 50 samples of calcite and four samples of fluorite range from ∼35 to ∼90 °C. Calcite δ18O values range from ∼0 to ∼22‰ (SMOW) but most fall between 12 and 20‰. The highest Th and the lowest δ18O values are found in the older calcite. Calcite Th and δ18O values indicate that most calcite precipitated from water with δ18O values between −13 and −7‰, similar to modern meteoric waters. 相似文献