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排序方式: 共有224条查询结果,搜索用时 31 毫秒
81.
Kilgore UJ Roberts JA Pool DH Appel AM Stewart MP DuBois MR Dougherty WG Kassel WS Bullock RM DuBois DL 《Journal of the American Chemical Society》2011,133(15):5861-5872
A series of mononuclear nickel(II) bis(diphosphine) complexes [Ni(P(Ph)(2)N(C6H4X)(2))(2)](BF(4))(2) (P(Ph)(2)N(C6H4X)(2) = 1,5-di(para-X-phenyl)-3,7-diphenyl-1,5-diaza-3,7-diphosphacyclooctane; X = OMe, Me, CH(2)P(O)(OEt)(2), Br, and CF(3)) have been synthesized and characterized. X-ray diffraction studies reveal that [Ni(P(Ph)(2)N(C6H4Me)(2))(2)](BF(4))(2) and [Ni(P(Ph)(2)N(C6H4OMe)(2))(2)](BF(4))(2) are tetracoordinate with distorted square planar geometries. The Ni(II/I) and Ni(I/0) redox couples of each complex are electrochemically reversible in acetonitrile with potentials that are increasingly cathodic as the electron-donating character of X is increased. Each of these complexes is an efficient electrocatalyst for hydrogen production at the potential of the Ni(II/I) couple. The catalytic rates generally increase as the electron-donating character of X is decreased, and this electronic effect results in the favorable but unusual situation of obtaining higher catalytic rates as overpotentials are decreased. Catalytic studies using acids with a range of pK(a) values reveal that turnover frequencies do not correlate with substrate acid pK(a) values but are highly dependent on the acid structure, with this effect being related to substrate size. Addition of water is shown to dramatically increase catalytic rates for all catalysts. With [Ni(P(Ph)(2)N(C6H4CH2P(O)(OEt)2)(2))(2)](BF(4))(2) using [(DMF)H](+)OTf(-) as the acid and with added water, a turnover frequency of 1850 s(-1) was obtained. 相似文献
82.
We give a bound for codes over an arbitrary alphabet in a non-Hamming metric and define MDS codes as codes meeting this bound. We show that MDS codes are precisely those codes that are uniformly distributed and show that their weight enumerators based on this metric are uniquely determined. 相似文献
83.
A.L. Crosbie R.L. Dougherty 《Journal of Quantitative Spectroscopy & Radiative Transfer》1981,25(6):551-569
Exact integral equations are derived describing the source function and radiative flux in a two-dimensional, radially infinite cylindrical medium which scatters anisotropically. The problem is two-dimensional and cylindrical because of axisymmetric loading. Radially varying collimated radiation is incident normal to the upper surface while the lower boundary has no radiation incident upon it. The scattering phase function is represented by a spike in the forward direction plus a series of Legendre polynomials. The two-dimensional integral equations are reduced to a one-dimensional form by separating variables for the case when the radial variation of the incident radiation is a Bessel function. The one-dimensional form consists of a system of linear, singular Fredholm integral equations of second kind. Other more complex boundary conditions are shown to be solvable by a superposition of this basic Bessel function case. Diffusely incident radiation is also considered. 相似文献
84.
Thurston JH Dougherty MJ Swenson DC Messerle L 《Dalton transactions (Cambridge, England : 2003)》2008,(38):5146-5148
The novel tetrahedral [Bi(5)(dpd)(6) within CH(3)CN](ClO(4))(3).3CH(3)CN (dpd = di-2-pyridyl-gem-diolate) has been synthesized from [Bi(9)(mu(3)-O)(8)(mu(3)-OH)(6)](ClO(4))(5) and di-2-pyridyl ketone. The Bi(5) complex incorporates CH(3)CN via C-HO hydrogen bonding. 相似文献
85.
We present a novel approach to surface chemistry studies using scanning tunneling microscopy (STM), where dissociation of molecules adsorbed on metal surfaces is induced nonlocally in a 10-100 nm radius around the STM tip by hot electrons that originate from the STM tip and transport on the surface. Nonlocal molecular excitation eliminates the influence of the STM tip on the outcome of the electron-induced chemical reaction. The spatial attenuation of the nonlocal reaction is used as a direct measure of hot-electron transport on the surface. 相似文献
86.
Krishnamurthy VR Dougherty A Haller CA Chaikof EL 《The Journal of organic chemistry》2011,76(13):5433-5437
Resolvins are family of lipid mediators derived from omega-3 polyunsaturated fatty acids, which are generated during the resolution phase of acute inflammation. Resolvin E1 is biosynthesized from eicosapentaenoic acid via 18(R)-hydroxyeicosapentaenoic acid (18R-HEPE) in the Cox-2 and lipoxygenase mediated pathway and has proven to exhibit potent anti-inflammatory activity. We report herein the first total chemical synthesis of 18R-HEPE and demonstrate that this compound displays in vivo bioactivity by blocking neutrophil infiltration in a murine model of zymosan-induced peritonitis. 相似文献
87.
Kyle D. Reichl Chelsea L. Mandell William G. Dougherty Chip Nataro 《Journal of organometallic chemistry》2011,696(24):3882-3894
The electrochemistry of 1,1′-bis(diphenylphosphino)cobaltocenium hexafluorophosphate ([dppc][PF6]), 1,1′-bis(dicyclohexylphosphino)cobaltocenium hexafluorophosphate ([dcpc][PF6]), 1,1′-bis(di-iso-propylphosphino)cobaltocenium hexafluorophosphate ([dippc][PF6]), and 1-(di-tert-butylphosphino)cobaltocenium hexafluorophosphate ([1-dtbpc][PF6]) was examined in methylene chloride with tetrabutylammonium hexafluorophosphate as the supporting electrolyte. A reversible reductive wave followed by an irreversible wave at more negative potentials was observed. Ten new phosphinothioyl ([dppcS2][PF6], [dcpcS2][PF6], [dippcS2][PF6], [1-dtbpcS][PF6], and 1,1′-bis(dicyclohexylphosphinothioyl)ferrocene) and phosphinoselenoyl derivatives ([dppcSe2][PF6], [dcpcSe2][PF6], [dippcSe2][PF6], [1-dtbpcSe][PF6], and 1,1′-bis(dicyclohexylphosphinoselenoyl)ferrocene) were prepared and characterized, and the structures of eight of these compounds were determined. The electrochemistry of these phosphinochalcogenyl cobaltocenium compounds, as well as the previously prepared [dppcO2][PF6], displayed two reversible reductive waves at potentials less negative than that of the free phosphines. A correlation was found to exist between the Hammett substituent constant σp and the reduction potentials of these compounds. In addition, the phosphinoselenoyl [dppcSe2][PF6], [dcpcSe2][PF6], and [dippcSe2][PF6] displayed an electrochemically irreversible oxidative wave, potentially indicating an intramolecular Se-Se bonded trication. The electrochemistry of three new and five previously reported transition metal complexes of the general formula [MnCl2(P∩P)][PF6] (M = Pd or Pt, n = 1, P∩P = dppc, dcpc or dippc; M = Au, n = 2, P∩P = dppc or dcpc)) was also examined displaying at least two reductive waves at potentials less negative than that of the free phosphines. Comparison of the electrochemical data with that previously obtained for analogous ferrocenes indicates that a correlation exists between the reduction potentials of the cobaltocenium phosphines and the potentials at which oxidation of the ferrocene phosphines occurs. In addition, the structure of [Au2Cl2(dppc)][PF6] was determined. 相似文献
88.
Mock MT Chen S Rousseau R O'Hagan MJ Dougherty WG Kassel WS DuBois DL Bullock RM 《Chemical communications (Cambridge, England)》2011,47(44):12212-12214
Cis and trans-Cr-N(2) complexes supported by the diphosphine ligand P(Ph)(2)N(Bn)(2) have been prepared. Positioned pendant amines in the second coordination sphere influence the thermodynamically preferred geometric isomer. Electronic structure calculations indicate negligible Cr-N(2) back-bonding; rather, electronic polarization of N(2) ligand is thought to stabilize Cr-N(2) binding. 相似文献
89.
Steven T. Dougherty Suat Karadeniz Bahattin Yildiz 《Designs, Codes and Cryptography》2012,63(1):113-126
Cyclic codes over an infinite family of rings are defined. The general properties of cyclic codes over these rings are studied,
in particular nontrivial one-generator cyclic codes are characterized. It is also proved that the binary images of cyclic
codes over these rings under the natural Gray map are binary quasi-cyclic codes of index 2
k
. Further, several optimal or near optimal binary codes are obtained from cyclic codes over R
k
via this map. 相似文献
90.
Segmented polystyrene (PS) and poly-methyl methacrylate (PMMA) nanofibers were fabricated by wetting nanoporous alumina templates
with multilayered polymer thin films. The order and thickness of the polymers within the thin films affected the resulting
nanofiber morphology, PS and PMMA segment properties, and created unique core-shell structure in the PMMA segments. The core-shell
structure suggests a complex wetting phenomenon. Fabrication of polymer nanostructures by wetting of layered thin films opens
the arena of multifunctional, one-dimensional, polymer nanostructures with segments having individual and specific functionalities. 相似文献