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A.C. Fischer J.J. Kroon T.G. Verburg T. Teunissen H.Th. Wolterbeek 《Marine Chemistry》2007,107(4):533-546
Iron chemistry in seawater has been extensively studied in the laboratory, mostly in small-volume sample bottles. However, little has been reported about iron wall sorption in these bottles. In this paper, radio-iron 55Fe was used to assess iron wall adsorption, both in terms of capacity, affinity and kinetics. Various bottle materials were tested. Iron sorption increased from polyethylene/polycarbonate to polymethylmetacrylate (PMMA)/high-density polyethylene/polytetrafluoroethylene to glass/quartz, reaching equilibrium in a 25–70 h period. PMMA was studied in more detail: ferric iron (Fe(III)) adsorbed on the walls of the bottles, whereas ferrous iron (Fe(II)) did not. Considering that in seawater the inorganic iron pool mostly consists of ferric iron, the wall will be a factor that needs to be considered in bottle experiments.The present data indicate that for PMMA with specific surface (S)-to-volume (V) ratio S/V, both iron capacity (42 ± 16 × 10− 9 mol/m2 or 1.7 × 10− 9 mol/L recalculated for the S/V-specific PMMA bottles used) and affinity (log KFe'W = 11.0 ± 0.3 m2/mol or 12.4 ± 0.3 L/mol, recalculated for the S/V-specific PMMA bottles used) are of similar magnitude as the iron capacity and -affinity of the natural ligands in the presently used seawater and thus cannot be ignored.Calculation of rate constants for association and dissociation of both Fe'L (iron bound to natural occurring organic ligands) and Fe'W (iron adsorbed on the wall of vessels) suggests that the two iron complexes are also of rather similar kinetics, with rate constants for dissociation in the order of 10 −4–10− 5 L/s and rate constants for association in the order of 108 L/(mol s). This makes that iron wall sorption should be seriously considered in small-volume experiments, both in assessments of shorter-term dynamics and in end-point observations in equilibrium conditions. Therefore, the present data strongly advocate making use of iron mass balances throughout in experiments in smaller volume set-ups on marine iron (bio) chemistry. 相似文献
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库车坳陷侏罗系煤成气动力学模拟研究 总被引:1,自引:0,他引:1
应用黄金管—高压釜封闭体系热模拟实验与GC、GC-IRMS分析技术,结合KINETICS专用软件,对库车坳陷侏罗系煤成气进行了动力学模拟研究。库车坳陷侏罗系煤具有高的产气性,在高演化阶段主要产甲烷气;侏罗系煤热解气甲烷碳同位素为-36‰~-25‰,乙烷碳同位素为-28‰~-16‰;甲烷、C2-C5气态烃的生成活化能分别为(47~64k)calm/ol、(55~72k)calm/ol,频率因子各为5.265×1013s-1、5.388×1018s-1。在此基础上,进一步探讨了克拉2气田天然气的成因。研究认为,克拉2气田天然气属阶段捕获的煤成气,主要聚集了5~1Ma时期的天然气,其成熟度Ro分布范围为1.3%~2.5%。 相似文献
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Photobleaching of chromophoric dissolved organic matter in natural waters: kinetics and modeling 总被引:9,自引:0,他引:9
The effects of monochromatic and polychromatic UV and visible (VIS) radiation on the optical properties (absorption and fluorescence) of chromophoric dissolved organic matter (CDOM) were examined for a Suwannee River fulvic acid (SRFA) standard and for water from the Delaware and Chesapeake Bays. The primary (direct) loss of absorption and fluorescence occurred at the irradiation wavelength(s), with smaller secondary (indirect) losses occurring outside the irradiation wavelength(s). The efficiency of both direct and indirect photobleaching decreased monotonically with increasing wavelength. Exposure to polychromatic light increased the CDOM absorption spectral slope (S), consistent with previous field measurements. An analysis of the monochromatic photobleaching kinetics argues that a model based on a simple superposition of multiple chromophores undergoing independent photobleaching cannot apply; this conclusion further implies that the absorption spectrum of CDOM cannot arise solely from a simple superposition of the spectra of numerous independent chromophores. The kinetics of CDOM absorption loss with the monochromatic irradiation were employed to create a simple, heuristic model of photobleaching. This model allowed us to examine the importance of the indirect photobleaching losses in determining the overall photobleaching rates as well as to model the photobleaching of natural waters under polychromatic light fields. Application of this model to natural waters closely predicted the change in the CDOM spectral shape caused by photodegradation. The time scale of this process was consistent with field observations acquired during the summertime for coastal waters in the Middle Atlantic Bight (MAB). The results indicate that the ratio of the photodegradation depth to the mixed layer depth is a key parameter controlling the rate of the photobleaching in surface waters. 相似文献
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Models for petroleum generation used by the industry are often limited by (a) sub-optimal laboratory pyrolysis methods for studying hydrocarbon generation, (b) over-simple models of petroleum generation, (c) inappropriate mathematical methods to derive kinetic parameters by fitting laboratory data, (d) primitive models of primary migration/expulsion and its coupling with petroleum generation, and (e) insufficient use of subsurface data to constrain the models. Problems (a), (b) and (c) lead to forced compensation effects between the activation energies and frequency factors of reaction kinetics that are wholly artificial, and which yield poor extrapolations to geological conditions. Simple switch or adsorption models of expulsion are insufficient to describe the residence time of species in source rocks. Yet, the residence time controls the thermal stresses to which the species are subjected for cracking to lighter species. 相似文献
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Yoann Louis Cdric Garnier Vronique Lenoble Stphane Mounier Neven Cukrov Dario Omanovi Ivanka Pieta 《Marine Chemistry》2009,114(3-4):110-119
An interaction of dissolved natural organic matter (DNOM) with copper ions in the water column of the stratified Krka River estuary (Croatia) was studied. The experimental methodology was based on the differential pulse anodic stripping voltammetric (DPASV) determination of labile copper species by titrating the sample using increments of copper additions uniformly distributed on the logarithmic scale. A classical at-equilibrium approach (determination of copper complexing capacity, CuCC) and a kinetic approach (tracing of equilibrium reconstitution) of copper complexation were considered and compared. A model of discrete distribution of organic ligands forming inert copper complexes was applied. For both approaches, a home-written fitting program was used for the determination of apparent stability constants (Kiequ), total ligands concentration (LiT) and association/dissociation rate constants (ki1,ki- 1).A non-conservative behaviour of dissolved organic matter (DOC) and total copper concentration in a water column was registered. An enhanced biological activity at the freshwater–seawater interface (FSI) triggered an increase of total copper concentration and total ligand concentration in this water layer. The copper complexation in fresh water of Krka River was characterised by one type of binding ligands, while in most of the estuarine and marine samples two classes of ligands were identified. The distribution of apparent stability constants (log K1equ: 11.2–13.0, log K2equ:8.8–10.0) showed increasing trend towards higher salinities, indicating stronger copper complexation by autochthonous seawater organic matter.Copper complexation parameters (ligand concentrations and apparent stability constants) obtained by at-equilibrium model are in very good accordance with those of kinetic model. Calculated association rate constants (k11:6.1–20 × 103 (M s)− 1, k21: 1.3–6.3 × 103 (M s)− 1) indicate that copper complexation by DNOM takes place relatively slowly. The time needed to achieve a new pseudo-equilibrium induced by an increase of copper concentration (which is common for Krka River estuary during summer period due to the nautical traffic), is estimated to be from 2 to 4 h.It is found that in such oligotrophic environment (dissolved organic carbon content under 83 µMC, i.e. 1 mgCL− 1) an increase of the total copper concentration above 12 nM could enhance a free copper concentration exceeding the level considered as potentially toxic for microorganisms (10 pM). 相似文献
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We report on the use of X-ray diffractometry under controlled conditions of temperature and relative humidity (RH-XRD) for
the investigation of NaCl deliquescence in the pore space of glass filter frits, which were used as model substrates. The
study confirms that RH-XRD is an appropriate experimental technique for the in situ observation of phase transformation in
porous materials. It is used for an investigation of both the deliquescence kinetics and the deliquescence humidity within
pores of different median pore diameter. Several major influences affecting deliquescence rates in the pore space close to
the surface of a porous material are discussed. It appears that quite short-term variation of ambient relative humidity, e.g.,
typical daily fluctuations, might induce damaging deliquescence–crystallization cycles within the pore space of building materials.
In agreement with theoretical considerations it was found that confinement of NaCl crystals in pores with median diameters
in the range 1.4–70 μm does not affect the deliquescence humidity of the salt. 相似文献
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The effects of oxygen supply rate and the presence or absence of nutrients on the kinetics of phenol degradation and oxygen consumption by a mixed microbial population were tested in a model system. The values for the maximum specific rate of phenol degradation (qSmax), the saturation constant (KS), and the inhibition concentration (SCR) were determined for unlimited growth (KLa = 340 h?1, growth medium) with 1.7 mmol g?1 h?1, 65 mg L?1, and 190 mg L?1. Under limitation conditions, alterations occur depending on the type of limitation. Nutrient limitations lead to values of 0.8 mmol g?1 h?1, 45 mg L?1, and 160 mg L?1, and oxygen limitations lead to 1.2 mmol g?1 h?1. 30 mg L?1, and 120 mg L?1, respectively. The results suggest that with excess oxygen, the rate of phenol degradation was higher and the inhibition effect of phenol was suppressed to some extent. Under the same high oxygen supply rate, the presence of nutrients in the model water significantly supported the phenol degradation rate. 相似文献