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排序方式: 共有400条查询结果,搜索用时 31 毫秒
1.
Jnos Szanyi Ja Hun Kwak Sarah Burton Jose A. Rodriguez Charles H.F. Peden 《Journal of Electron Spectroscopy and Related Phenomena》2006,150(2-3):164-170
Adsorbed ionic NOx species formed upon the interaction of NO2 with dehydrated or hydrated Na- and Ba-Y, FAU zeolites were characterized using FT-IR/TPD, solid state NMR, and XANES techniques. NO2 disproportionates on both dehydrated catalyst materials forming NO+ and NO3− species. These ionic species are stabilized by their interactions with the negatively charged zeolite framework and the charge compensating cations (Na+ and Ba2+), respectively. Although the nature of the adsorbed NOx species formed on the two catalysts is similar, their thermal stabilities are strongly dependent on the charge compensating cations. In the presence of water in the channels of these zeolite materials new paths open for reactions between NO+ and H2O, and NO2 and H2O, resulting in significant changes in the adsorbed ionic species observed. These combined spectroscopic investigations afforded the understanding of the interactions between water and NO2 on these zeolite catalysts. 相似文献
2.
J. L. Gardea-Torresdey K. J. Tiemann J. R. Peralta-Videa J. G. Parsons M. Delgado 《Microchemical Journal》2004,76(1-2):65
Traditional treatment methods used to clean-up heavy metal contamination of soils and waters are cost intensive whereas more cost effective methods need to be developed. The use of plant materials to remediate heavy contamination has been studied for the past two decades. This technique has shown much promise for many of the common heavy metal contaminants, but few studies have focused on the lanthanide series elements. By investigating the binding and interactions of the lanthanide elements to alfalfa biomass, a more complete understanding of the binding mechanisms and the interactions of heavy metals with biomaterials can be obtained. Different chemical functional groups on the alfalfa biomass, carboxyl, amino, sulfur, and ester groups, were modified to investigate the binding mechanisms of erbium(III) and holmium(III). Batch experiments were performed with native and chemically modified alfalfa biomass suggesting that the carboxyl groups play a major role in the binding of erbium(III) and holmium(III) to the alfalfa biomass. In addition, X-ray absorption spectroscopy (XAS) studies corroborated the data obtained from the batch experiments. 相似文献
3.
Studies were performed to determine the effect of pH on chromium (Cr) binding by native, esterified, and hydrolyzed saltbush (Atriplex canescens) biomass. In addition, X-ray absorption spectroscopy studies were performed to determine the oxidation state of Cr atoms bound to the biomass. The amounts of Cr adsorbed by saltbush biomass were determined by inductively coupled plasma-optical emission spectroscopy (ICP-OES). For Cr(III), the results showed that the percentages bound by native stems, leaves, and flowers at pH 4.0 were 98%, 97%, and 91%, respectively. On the other hand, the Cr(VI) binding by the three tissues of the native and hydrolyzed saltbush biomass decreased as pH increased. At pH 2.0 the stems, leaves, and flowers of native biomass bound 31%, 49%, and 46%, of Cr(VI), respectively. The results of the XAS experiments showed that Cr(VI) was reduced in some extend to Cr(III) by saltbush biomass at both pH 2.0 and pH 5.0. The XANES analysis of the Cr(III) reaction with the saltbush biomass parts showed an octahedral arrangement of oxygen atoms around the central Cr(III) atom. The EXAFS studies of saltbush plant samples confirmed these results. 相似文献
4.
Arsenic (As) is a toxic trace element that occurs naturally in groundwater and soils. Understanding the reactions of arsenite
(As(III)) and arsenate (As(V)) with soil and mineral surfaces is critical for predicting the fate and transport of As in the
environment and developing better ways to remediate As-contaminated areas. This investigation uses X-ray absorption near edge
spectroscopy (XANES) to evaluate the solid phase oxidation state and mineral surface binding sites in three agricultural soil
samples from California, USA by fitting linear combinations of XANES spectra derived from several synthetic and well characterized
As(III)- and As(V)-treated model compounds (Fe and Al metal hydroxides and aluminosilicate illite clay mineral). The results
suggest that As(III) is either partially or completely oxidized to As(V) when reacted with soil in an aqueous, batch reaction.
The As(III)-treated Aiken soil was composed of 60% As(III) attached to surfaces similar to lepidocrocite (γ-FeOOH)) and 40%
As(V) attached to aluminosilicate (illite). The Fallbrook soil completely oxidized As(III) and the product was As(V) adsorbed
on Al hydroxide (gibbsite, γ-Al(OH)3) (62%), illite (16%), and lepidocrocite (γ-FeOOH) (22%). The reaction of As(III) with Wyo soil resulted in 42% As(III) adsorbed
on surface similar to goethite and 58% As(V) adsorbed on lepidocrocite. Arsenic(V) adsorption on soil resulted in stable As(V)
surface complexes that were well described by XANES spectra from As(V) adsorption complexes on gibbsite, illite, and lepidocrocite. 相似文献
5.
Feth MP Bolm C Hildebrand JP Köhler M Beckmann O Bauer M Ramamonjisoa R Bertagnolli H 《Chemistry (Weinheim an der Bergstrasse, Germany)》2003,9(6):1348-1359
XANES and EXAFS spectroscopic studies at the Mn-K- and Br-K-edge of reaction products of (S,S)-(+)-N,N'-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediaminomanganese(III) chloride ([(salen)Mn(III)Cl], 1) and (S,S)-(+)-N,N'-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediaminomanganese(III) bromide ([(salen)Mn(III)Br], 2) with 4-phenylpyridine N-oxide (4-PPNO) and 3-chloroperoxybenzoic acid (MCPBA) are reported. The reaction of the Mn(III) complexes with two equivalents of 4-PPNO leads to a hexacoordinated compound, in which the manganese atom is octahedrally coordinated by four oxygen/nitrogen atoms of the salen ligand at an average distance of approximately 1.90 A and two additional, axially bonded oxygen atoms of the 4-PPNO at 2.25 A. The oxidation state of this complex was determined as approximately +IV by a comparative study of Mn(III) and Mn(V) reference compounds. The green intermediate obtained in reactions of MCPBA and solutions of 1 or 2 in acetonitrile was investigated with XANES, EXAFS, UV/Vis, and Raman spectroscopy, and an increase of the coordination number of the manganese atoms from 4 to 5 and the complete abstraction of the halide was observed. A formal oxidation state of IV was deduced from the relative position of the pre-edge 1s-->3d feature of the X-ray absorption spectrum of the complex. The broad UV/Vis band of this complex in acetonitrile with lambda(max)=648 nm was consistent with a radical cation structure, in which a MCPBA molecule was bound to the Mn(IV) central atom. An oxomanganese(V) or a dimeric manganese(IV) species was not detected. 相似文献
6.
János Osán Szabina Török Bálint Alföldy Anita Alsecz Gerald Falkenberg Soo Yeun Baik René Van Grieken 《Spectrochimica Acta Part B: Atomic Spectroscopy》2007
The rivers in the Hungarian Upper Tisza Region are frequently polluted mainly due to mining activities in the catchment area. At the beginning of 2000, two major mining accidents occurred in the Romanian part of the catchment area due to the failure of a tailings dam releasing huge amounts of cyanide and heavy metals to the rivers. Surface sediment as well as water samples were collected at six sites in the years 2000–2003, from the northeast-Hungarian section of the Tisza, Szamos and Túr rivers. The sediment pollution of the rivers was compared based on measurements of bulk material and selected single particles, in order to relate the observed compositions and chemical states of metals to the possible sources and weathering of pollution. Non-destructive X-ray analytical methods were applied in order to obtain different kinds of information from the same samples or particles. In order to identify the pollution sources, their magnitude and fate, complementary analyses were carried out. Heterogeneous particulate samples were analyzed from a large geographical territory and a 4-year time period. Individual particles were analyzed only from the “hot” samples that showed elevated concentrations of heavy metals. Particles that were classified as anthropogenic were finally analyzed to identify trace concentrations and chemical states of heavy metals. 相似文献
7.
Stefan G Ebbinghaus 《Journal of solid state chemistry》2004,177(3):817-823
Single crystals of the new compound La1.2Sr2.4RuO7, an oxide related to the hexagonal perovskites, were grown from a BaCl2 flux. The structure was solved by single crystal X-ray diffraction. La1.2Sr2.4RuO7 crystallizes in the space group with a=5.760(1) Å and c=18.273(3) Å. It is one of the rare examples of oxides with isolated RuO6-octahedra. The structure consists of alternating layers of RuO6-octahedra and trigonal (La,Sr)O6-prisms. These prisms are capped by one additional oxygen ion, which occupies a distorted position within the (La,Sr)O6-layers. La1.2Sr2.4RuO7 is the second member of the general [A2O][AnBn−1O3n] family of hexagonal perovskites with n=2 and the first ruthenate possessing this structure. XANES investigations, bond valence sum calculations and magnetic measurements show that ruthenium takes the oxidation state +5. Although the ruthenium ions have quite long distances, a medium strong antiferromagnetic interaction between these paramagnetic centers was observed. 相似文献
8.
M. Karppinen Y. Morita I. Grigoraviciute R.S. Liu 《Journal of solid state chemistry》2005,178(11):3464-3470
Superconductivity characteristics have been systematically evaluated for a two-CuO2-plane copper oxide system, (Cu,Mo)-12s2, upon increasing the number of fluorite-structured layers, s, between the two CuO2 planes. Essentially single-phase samples of (Cu0.75Mo0.25)Sr2YCu2O7+δ (s=1), (Cu0.75Mo0.25)Sr2(Ce0.45Y0.55)2Cu2O9+δ (s=2) and (Cu0.75Mo0.25)Sr2(Ce0.67Y0.33)3Cu2O11+δ (s=3) were synthesized through a conventional solid-state route in air. To make the samples superconductive an additional high-pressure oxygenation (HPO) treatment was required. Such treatment (carried out at 5 GPa and 500 °C in the presence of 75 mol% Ag2O2 as an oxygen source to maximize the Tc) compressed the crystal lattice for the three members of the (Cu0.75Mo0.25)-12s2 series equally, i.e., by 0.01 Å for the a parameter and by 0.07 Å for the c parameter per formula unit. From both Cu L-edge and O K-edge XANES spectra the s=1 sample was found to possess the highest overall hole-doping level among the HPO samples. Accordingly it exhibited the best superconductivity characteristics. With increasing s, both the Tc (s=1: 88 K, s=2: 61 K, s=3: 53 K) and Hirr values got depressed, being well explained by the trend of decreasing CuO2-plane hole concentration with increasing s as revealed from O K-edge XANES spectra for the same samples. Hence, the present results do not suggest any significant (negative) impact on the superconductivity characteristics from the gradually thickened fluorite-structured block itself. 相似文献
9.
A. Kulińska M. Uhrmacher R. Dedryvère A. Lohstroh K.P. Lieb J.-C. Jumas 《Journal of solid state chemistry》2004,177(1):109-118
LixIn2S3 was electrochemically prepared with different small amounts x of lithium (0?x?0.13) in order to maintain the initial crystallographic structure of the thiospinel In2S3. About 1012 radioactive 111In ions have been implanted into these samples at 400 keV to perform PAC experiments in the temperature range from 10 to 773 K. The results are compared to previous experiments with undoped In2S3 samples. According to the structure of In2S3 in the β-phase, which belongs to the I41/amd space group having a unit cell with 32 In and 48 S atoms and the cell parameters α=7.61 Å and c=32.28 Å, three different electric field gradients were observed. Within two different temperature ranges dynamical EFGs occur, which are clearly influenced by the insertion of Lithium. The strong dependence of one EFG on the Li concentration x can be correlated to the effective charge of the In ions. This correlation is discussed with respect to XRD analyses of the LixIn2S3 samples and to XANES measurements on a similar sample. 相似文献
10.
G. Mountjoy M.A. Holland P. Gunawidjaja D.M. Pickup G.W. Wallidge M.E. Smith R.J. Newport 《Journal of Sol-Gel Science and Technology》2003,26(1-3):137-141
There has been much work on the binary TiO2-SiO2 and ZrO2-SiO2 materials prepared by sol-gel because of the beneficial properties resulting from incorporation of Ti and Zr. In contrast the ternary TiO2-ZrO2-SiO2 xerogels have been relatively little studied. We report the results of a study of those xerogels having Zr:Ti:Si ratios of 5:15:80, 10:10:80 and 15:5:80 heated to 750°C and to 1000°C. The study includes X-ray diffraction, small angle X-ray scattering, X-ray absorption spectroscopy at Ti and Zr K-edges, and 17O MAS-NMR. The study has benefited from close comparison with similar previous studies of the binary systems. The metal atoms in the ternary systems are shown to be predominantly homogeneously mixed in the silica network, as observed for the respective binary systems. The clear exception is for the sample with a minority of Zr, which after heat treatment at 750°C shows the presence of phase separation attributed to the formation of an amorphous precursor of ZrTiO4; at 1000°C this phase crystallises. In samples with higher Zr content the crystallisation of a ZrO2 tetragonal phase was observed. The data obtained illustrate well the strength of a research methodology in which a common batch of samples is studied using a coherent suite of modern structural probes. 相似文献