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81.
In strongly alkaline aqueous KOH solutions containing SiIV in large excess over AlIII, the kinetics of exchange of monomeric silicate with small acyclic aluminosilicate solute species is much more rapid than with either cyclic aluminosilicates or any all-silicate anions. Selective inversion recovery 29Si NMR studies of homogeneous solutions of stoichiometric composition 3.0 mol kg-1 of SiO2, 0.1 mol kg-1 of Al2O3, and 8.0 mol kg-1 of K2O in 60-75% D2O gave rate constants of 2.0 +/- 0.2 kg mol-1 s-1 and 17 +/- 4 s-1 for the forward and reverse reactions of monomeric silicate with (HO)3AlOSiOn(OH)(3-n)(n+1)- (n = 2 or 3) at 0 degree C. These rate constants are more than 10(4)-fold faster than those extrapolated from 60 to 90 degrees C for comparable reactions of silicate anions. The greater lability of acyclic aluminate centers relative to silicate is ascribed partly to the availability of HO- groups for condensation reactions on Al and mainly to the ease of expansion of the coordination number of AlIII beyond 4. The latter attribute is diminished when AlIII is constrained to be tetrahedral in cyclic structures. With respect to the mechanism of formation of zeolites from alkaline aqueous media, it is suggested that small, labile AlOSi units add rapidly to growing zeolitic structures "on demand", whereas the more kinetically inert cage or ring structures cannot. This would explain why a silicate or aluminosilicate structure that is dominant among solute species at equilibrium in the presence of a particular cation may bear little or no geometric relation to the zeolitic framework promoted kinetically by that same cation. 相似文献
82.
Donatella BantiMichael North 《Tetrahedron letters》2003,44(44):8157-8160
Norbornene derivatives 4 and 5 containing sidechains bearing an internal alkyne and either a terminal alkene or a terminal alkyne were found to undergo a cascade of metathesis reactions when treated with ruthenium based metathesis catalysts to form highly functionalised pentacyclic products. The reactions illustrate an interesting difference in reactivity between Grubbs’ catalyst and the second generation catalyst, with the former being more reactive for the early steps of the cascade. 相似文献
83.
Anton Deitmar School of Mathematical Sciences University of Exeter Laver Building North Park Road Exeter EX QE Devon UK 《数学物理学报(B辑英文版)》2001,(1)
0 IntroductionThe group of norm-1 ideles A1 over a global field lt acts by 1111lltip1ication on t11e additivegroup of adeIes A. Let G = A1 be A be tl1eir semidirect product. Let r be its arithnletic sub-group kx oc k. For the case k = Q Dorian Goldfeld gavc ill [2] a Schwartz kernel on rG whosegeometrical trace equals the prime 11un1ber side of the explicit fOr1llulas of A. Weil. A spectralillterpretatiou in the seuse of the Selberg trace formula is cal1ed for. In order that a geolllet… 相似文献
84.
Michael J. North 《Computational & Mathematical Organization Theory》2001,7(4):331-337
Complex Adaptive Systems (CAS) can be applied to investigate large-scale socio-cognitive-technical systems. Viewing such systems from a multi-agent social and organizational perspective allows innovative computational policy analysis. Argonne National Laboratory (ANL) has taken such a perspective to produce an integrated model of the electric power and natural gas markets. This model focuses on the organizational interdependencies between these markets. These organizational interdependencies are being strained by fundamental market transformations. 相似文献
85.
86.
CAO Gang WANG Mei-yi? WANG Ming-zhong WANG Su-hua LI Yong-hong LI Zheng-ming . State Key Laboratory of Elemento-Organic Chemistry Research Institute of Elemento-Organic Chemistry Nankai University Tianjin P. R. China . College of Chemistry Chemical Engineering North University for Ethnics Yinchuan 《高等学校化学研究》2011,27(1):60-65
Sulfonylurea herbicides have been applied worldwide in agriculture. Some sulfonylurea residues might exist in soil longer than that people expected. However, flupyrsulfuron-methyl-sodium which was firstly reported as a new 5-substituted sulfonylurea herbicide has less than one month residual life. Therefore, 5-substituted benzenesulfonylureas are potential molecules to regulate its residual situation. In order to develop new sulfonylurea derivatives, the substituent on the critical 5-posotion of the benzene... 相似文献
87.
Nicholas M. Musyoka Jianwei Ren Perushini Annamalai Henrietta W. Langmi Brian C. North Mkhulu Mathe Dmitri Bessarabov 《Research on Chemical Intermediates》2016,42(6):5299-5307
Metal–organic frameworks (MOFs) hybrid composites have recently attracted considerable attention in hydrogen storage applications. In this study a hybrid composite of zeolite templated carbon (ZTC) and Cr-based MOF (MIL-101) was synthesised by adding the templated carbon in situ during the synthesis of MIL-101(Cr). The obtained sample was fully characterized and hydrogen adsorption measurements performed at 77 K up to 1 bar. The results showed that the surface areas and the hydrogen uptake capacities of individual MIL-101 (2552 m2 g?1, 1.91 wt%) and zeolite templated carbon (2577 m2 g?1, 2.39 wt%) could be enhanced when a hybrid MIL-101(Cr)/ZTC composite (2957 m2 g?1, 2.55 wt%) was synthesized. The procedure presents a simple way for enhancement of hydrogen uptake capacity of the individual Cr-MOF and templated carbon samples. 相似文献
88.
Importance of Micropore–Mesopore Interfaces in Carbon Dioxide Capture by Carbon‐Based Materials 下载免费PDF全文
Dr. Gema Durá Dr. Vitaliy L. Budarin Dr. José A. Castro‐Osma Dr. Peter S. Shuttleworth Sophie C. Z. Quek Prof. James H. Clark Prof. Michael North 《Angewandte Chemie (International ed. in English)》2016,55(32):9173-9177
Mesoporous carbonaceous materials (Starbons®) derived from low‐value/waste bio‐resources separate CO2 from CO2/N2 mixtures. Compared to Norit activated charcoal (AC), Starbons® have much lower microporosities (8–32 % versus 73 %) yet adsorb up to 65 % more CO2. The presence of interconnected micropores and mesopores is responsible for the enhanced CO2 adsorption. The Starbons® also showed three–four times higher selectivity for CO2 adsorption rather than N2 adsorption compared to AC. 相似文献
89.
Rakvin B Zilić D North JM Dalal NS 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2003,165(2):260-264
We report on electron paramagnetic resonance (EPR) probing of magnetic fields and magnetic field gradients near the surface of a single crystal of the nanomagnet [Mn12O12(CH3COO)16(H2O)4].2CH3COOH.4H2O (Mn12-Ac). As the EPR probe, we utilized a 0.7 mm x 30 microm x 30 microm fibrous needle of the organic conductor N-methylphenazinium-tetracyanoquinodimethane (NMP-TCNQ), which yields an exceptionally sharp peak, with a 0.2 G (approximately 20 microT) width. In the presence of Mn12-Ac, the probe's peak exhibits splitting on temperature lowering, which depends on the orientation of the Zeeman field relative to the axis of easy magnetization of the employed Mn12-Ac crystal. The shifted peaks yield the magnitude of the magnetic field from Mn12-Ac crystal to which the various fibers of the probe are subjected. In conjunction with electron microscopy, the shifts yield the field gradient at the crystal surface and its change with temperature. For Mn12-Ac at 10 K, the surface magnetic field was measured to be in the mT range and its gradient on the order of 50 T/m. 相似文献
90.
The connection between the K-quantum number and product correlations in the barrierless unimolecular dissociation of symmetric-top molecules is explored to establish a qualitative diagnostic for the treatment of the K-rotor dynamics in unimolecular reaction theory. We find that fragment scalar and vector correlations can provide guidance in this matter, and the photodissociation dynamics of thermal NCNO to form CN and NO at several dissociation wavelengths are presented to demonstrate the utility of this approach. The "goodness" of the K-quantum number can be related to the amount of energy in the conserved vibrational modes at the inner transition state. On the basis of measured correlated vibrational distributions, the K-quantum number is found to be approximately conserved at the inner transition state for the photodissociation of NCNO at 514, 520, and 526 nm. The methodology, involving a comparison of product distributions from the photodissociation of jet and thermal ensembles at identical wavelengths, is general and may be applied to previously studied systems that dissociate along barrierless potential energy surfaces, CF(3)NO and CH(2)CO. In addition, vector correlations serve as a means to probe the K-mixing at the outer transition state, and measured v-j correlations in the photodissociation of thermal NCNO are presented. 相似文献