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191.
The kinetics of the aqueous phase reactions of NO3 radicals with HCOOH/HCOO– and CH3COOH/CH3COO– have been investigated using a laser photolysis/long-path laser absorption technique. NO3 was produced via excimer laser photolysis of peroxodisulfate anions (S2O
8
2–
) at 351 nm followed by the reactions of sulfate radicals (SO
4
–
) with excess nitrate. The time-resolved detection of NO3 was achieved by long-path laser absorption at 632.8 nm. For the reactions of NO3 with formic acid (1) and formate (2) rate coefficients ofk
1=(3.3±1.0)×105 l mol–1 s–1 andk
2=(5.0±0.4)×107 l mol–1 s–1 were found atT=298 K andI=0.19 mol/l. The following Arrhenius expressions were derived:k
1(T)=(3.4±0.3)×1010 exp[–(3400±600)/T] l mol–1 s–1 andk
2(T)=(8.2±0.8)×1010 exp[–(2200±700)/T] l mol–1 s–1. The rate coefficients for the reactions of NO3 with acetic acid (3) and acetate (4) atT=298 K andI=0.19 mol/l were determined as:k
3=(1.3±0.3)×104 l mol–1 s–1 andk
4=(2.3±0.4)×106 l mol–1 s–1. The temperature dependences for these reactions are described by:k
3(T)=(4.9±0.5)×109 exp[–(3800±700)/T] l mol–1 s–1 andk
4(T)=(1.0±0.2)×1012 exp[–(3800±1200)/T] l mol–1 s–1. The differences in reactivity of the anions HCOO– and CH3COO– compared to their corresponding acids HCOOH and CH3COOH are explained by the higher reactivity of NO3 in charge transfer processes compared to H atom abstraction. From a comparison of NO3 reactions with various droplets constituents it is concluded that the reaction of NO3 with HCOO– may present a dominant loss reaction of NO3 in atmospheric droplets. 相似文献
192.
Xue Xi Tie Guy Brasseur Xing Lin Pierre Friedlingstein Claire Granier Philip Rasch 《Journal of Atmospheric Chemistry》1994,18(2):103-128
The paper discusses the potential effects on the ozone layer of gases released by the engines of proposed high altitude supersonic aircraft. The major problem arises from the emissions of nitrogen oxides which have the potential to destroy significant quantities of ozone in the stratosphere. The magnitude of the perturbation is highly dependent on the cruise altitude of the aircraft. Furthermore, the depletion of ozone is substantially reduced when heterogeneous conversion of nitrogen oxides into nitric acid on sulfate aerosol particles is taken into account in the calculation. The sensitivity of the aerosol load on stratospheric ozone is investigated. First, the model indicates that the aerosol load induced by the SO2 released by aircraft is increased by about 10–20% above the background aerosols at mid-high latitude of the Northern Hemisphere at 15 km for the NASA emission scenario A (the NASA emission scenarios are explained in Tables I to III). This increase in aerosol has small effects on stratospheric ozone. Second, when the aerosol load is increased following a volcanic eruption similar to the eruption of El Chichon (Mexico, April 1982), the ozone column in spring increases by as much as 9% in response to the injection of NO
x
from the aircraft with the NASA emission scenario A. Finally, the modeled suggests that significant ozone depletion could result from the formation of additional polar stratospheric clouds produced by the injection of H2O and HNO3 by the aircraft engines. 相似文献
193.
194.
Diana Rodriguez Ana Rodriguez Amparo Soto Alfonso Aranda Yolanda Diaz-de-Mera Alberto Notario 《Journal of Atmospheric Chemistry》2008,59(3):187-197
The reactions of three structurally similar unsaturated alcohols, 2-buten-1-ol (crotyl alcohol), 2-methyl-2-propen-1-ol (MPO221)
and 3-methyl-2-buten-1-ol (MBO321) with Cl atoms, have been investigated for the first time, using a 400 l Teflon reaction
chamber coupled with gas chromatograph-coupled with flame-ionization detection (GC-FID). The experiments were performed at
atmospheric pressure and at temperatures between 255 and 298 K, in air or nitrogen as the bath gas. The obtained kinetic data
were used to derive the Arrhenius expressions , , (in units of cm3 molecule−1 s−1). Finally, atmospheric lifetimes of those unsaturated alcohols with respect to OH, NO3, O3 and Cl have been calculated. 相似文献
195.
利用一个三维的冰雹云模式与化学组分输送模块耦合,得到云输送引起大气光化学组分的再分布,然后用一个包含详细气相化学反应机制的箱模式研究了云输送引起的气相体积分数的变化及其对大气化学系统产生的影响。结果表明,云输送后O3体积分数大于无云个例,但其后两天内两者的变化趋势相差不大;HNO3、NO2、NO3、PAN等的体积分数均明显高于无云个例,分别增长了87%、70%、62%和49%,其中NO2体积分数的增加主要由于云输送造成,而NO3、HNO3、PAN主要是输送对化学扰动的结果。两天内OH和HO2自由基体积分数比无云个例平均增长了13%和11%。 相似文献
196.
Measurements were performed in spring 2001 and 2002 to determine the characteristics of soil dust in the Chinese desert region of Dunhuang, one of the ground sites of the Asia-Pacific Regional Aerosol Characterization Experiment (ACE-Asia). The mean mass concentrations of total suspended particle matter during the spring of 2001 and 2002 were 317 μg m?3 and 307 μg m?3, respectively. Eleven dust storm events were observed with a mean aerosol concentration of 1095 μg m?3, while the non-dusty days with calm or weak wind speed had a background aerosol loading of 196 μgm?3 on average in the springtime. The main minerals detected in the aerosol samples by X-ray diffraction were illite, kaolinite, chlorite, quartz, feldspar, calcite and dolomite. Gypsum, halite and amphibole were also detected in a few samples. The mineralogical data also show that Asian dust is characterized by a kaolinite to chlorite (K/C) ratio lower than 1 whereas Saharan dust exhibits a K/C ratio larger than 2. Air mass back-trajectory analysis show that three families of pathways are associated with the aerosol particle transport to Dunhuang, but these have similar K/C ratios, which further demonstrates that the mineralogical characteristics of Asian dust are different from African dust. 相似文献
197.
Cloud droplet chemistry is modelled for the first 150 m of rise in a wintertime, mid-latitude, marine stratus cloud using observations made at and near the Cape Grim Baseline Station as a source of input parameters. The emphasis in this work was to study the variation in droplet chemistry as a function of both droplet size and nucleus composition, with a particular focus on the way in which oxidation of dissolved sulfur dioxide varied.At 150 m above the condensation level, solute concentration as a function of droplet size was found to increase by as much as 2 to 3 orders of magnitude for only a factor of 2 increase in droplet radius, primarily as a consequence of the 1/r dependence in the droplet growth equation. This type of size dependence exists at all levels in the model cloud, and has a significant influence on oxidation rate of sulfur dioxide in droplets growing on sulfate nuclei, oxidation by ozone being favoured in the smallest droplets, but oxidation by hydrogen peroxide being favoured in the larger droplets. Oxidation by ozone is favoured at all sizes in droplets formed on sea-salt nuclei as a result of the initially high alkalinity of these droplets, and in the cloud overall is calculated to be the more important oxidation pathway. Although based on a simplified chemical scheme, these results suggest that both size-dependent and nucleus-dependent chemistry of cloud droplets may need to be considered explicitly in cloud modelling work.Volume-weighted mean pH values in the range 5 to 6 were predicted from sensitivity studies in which input variables were varied over reasonable ranges, in agreement with two sets of bulk cloud-water pH data obtained by aircraft near Cape Grim. 相似文献
198.
M.?Steinbacher J.?Dommen C.?Ordonez S.?Reimann F.?C.?Grüebler J.?Staehelin S.?Andreani-Aksoyoglu A.?S.?H.?PrevotEmail author 《Journal of Atmospheric Chemistry》2005,51(3):293-315
Measurements of volatile organic compounds (VOCs) were performed in the Po Basin, northern Italy in early summer 1998, summer 2002, and autumn 2003. During the three campaigns, trace gases and meteorological parameters were measured at a semi-rural station, around 35 km north of the city center of Milan. Bimodal diurnal cycles of isoprene with highest concentrations in the morning and evening were found and could be explained by the interaction of emissions, chemical reactions, and vertical mixing. The diurnal cycle could be qualitatively reproduced by a three-dimensional Eulerian model. The nighttime decay of isoprene could be attributed mostly to reactions with NO3, while the decay of the isoprene oxidation products could not be explained with the considered chemical reactions. Methanol reached very high mixing ratios, up to 150 ppb. High concentrations with considerable variability occurred during nights with high relative humidities and low wind speeds. The origin of these nighttime methanol concentrations is most likely local and biogenic but the specific source could not be identified. 相似文献
199.
A global two-dimensional chemistry model is developed to study long-term trends of CH_4 sinceindustrial revolution.The sources of CH_4,CO and NO_x are parameterized as functions of latitudeand time.With two long-term emission scenarios,long-term trends of CH_4 are simulated.The resultshave a good agreement with observation from ice cores.The modeled CH_4 increased from 760 ppbvin 1840 to 1611.9 ppbv in 1991, while the modeled number concentration of tropospheric OHdecreased from 7.17×10~5 cm~(-3)in 1840 to 5.79×10~5 cm~(-3) in 1991.The increase of atmosphericCH_4 can be explained by the increase of emission of CH_4 and build-up because of decrease of OHradicals that remove CH_4 from the atmosphere.The model is also used to simulate the distribution of CH_4.Comparisons between the modelresults and observations show that the model can simulate both latitudinal distribution and seasonalvariation of CH_4 well. 相似文献
200.
A global two-dimensional chemistry model is developed to study long-term trends of CH4 since industrial revolution.The sources of CH4,CO and NOx are parameterized as functions of latitude and time.With two long-term emission scenarios,long-term trends of CH4 are simulated.The results have a good agreement with observation from ice cores.The modeled CH4 increased from 760 ppbv in 1840 to 1611.9 ppbv in 1991, while the modeled number concentration of tropospheric OH decreased from 7.17×105 cm-3 in 1840 to 5.79×105 cm-3 in 1991.The increase of atmospheric CH4 can be explained by the increase of emission of CH4 and build-up because of decrease of OH radicals that remove CH4 from the atmosphere.The model is also used to simulate the distribution of CH4.Comparisons between the model results and observations show that the model can simulate both latitudinal distribution and seasonal variation of CH4 well. 相似文献