全文获取类型
收费全文 | 144篇 |
免费 | 0篇 |
国内免费 | 13篇 |
专业分类
化学 | 135篇 |
力学 | 1篇 |
数学 | 9篇 |
物理学 | 12篇 |
出版年
2019年 | 3篇 |
2018年 | 2篇 |
2017年 | 1篇 |
2016年 | 1篇 |
2015年 | 2篇 |
2014年 | 1篇 |
2013年 | 8篇 |
2012年 | 3篇 |
2011年 | 3篇 |
2010年 | 6篇 |
2009年 | 5篇 |
2008年 | 13篇 |
2007年 | 14篇 |
2006年 | 21篇 |
2005年 | 24篇 |
2004年 | 15篇 |
2003年 | 11篇 |
2002年 | 5篇 |
2000年 | 2篇 |
1999年 | 1篇 |
1998年 | 1篇 |
1997年 | 1篇 |
1996年 | 4篇 |
1995年 | 2篇 |
1994年 | 1篇 |
1992年 | 2篇 |
1990年 | 1篇 |
1988年 | 1篇 |
1984年 | 1篇 |
1977年 | 1篇 |
1975年 | 1篇 |
排序方式: 共有157条查询结果,搜索用时 15 毫秒
71.
Kanamori D Furukawa A Okamura TA Yamamoto H Ueyama N 《Organic & biomolecular chemistry》2005,3(8):1453-1459
Intramolecularly OHO[double bond, length as m-dash]C hydrogen bonded phenols, 2-HO-C6H2-3,5-(t-Bu)2-CONH-t-Bu (1-OH), 2-HO-C6H2-5-t-Bu-1,3-(CONH-t-Bu)2 (2-OH) and 2-HO-C6H2-3,5-(t-Bu)2-NHCO-t-Bu (4-OH), were synthesized and their phenolate anions were prepared as tetraethylammonium salts (-1O-(NEt4+), 2-O-(NEt4+) and 4-O-(NEt4+)) with intramolecular NHO(oxyanion) hydrogen bonds. 4-HO-C(6)H(2)-3,5-t-Bu(2)-CONH-t-Bu (3-OH) and its phenolate anion, 3-O-(NEt4+), were synthesized as non-hydrogen bonded references. The presence of intramolecular hydrogen bonds was established through the crystallographic analysis and/or (1)H NMR spectroscopic results. Intramolecular NHO(phenol) hydrogen bonds shift the pK(a) of the phenol to a more acidic value. The results of cyclic voltammetry show that the intramolecular OH...O=C hydrogen bond negatively shifts the oxidation potential of the phenol. In contrast, the intramolecular NHO(oxyanion) hydrogen bond positively shifts the oxidation potential of the phenolate anion, preventing oxidation. These contributions of the hydrogen bond to the pKa value and the oxidation potentials probably play an important role in the formation of a tyrosyl radical in photosystem II. 相似文献
72.
Kato M Kojima K Okamura TA Yamamoto H Yamamura T Ueyama N 《Inorganic chemistry》2005,44(11):4037-4044
A novel series of bis(carbamoylthiophenolato)mercury(II) complexes, [Hg(S-RNHCOC6H4)2] (1, R = 2-t-Bu; 2, R = 2-CH3; 3, R = 2-C6H5CH2; 4, R = 4-t-Bu), and a tetrakis(carbamoylthiophenolato)mercury(II) complex, (NEt4)2[Hg-(S-2-CH3NHCOC6H4)4] (5), were synthesized and characterized by 1H NMR, IR, 199Hg NMR, and crystallographic analyses. The bis(carbamoylthiophenolato)mercury complexes 1-3 do not have intramolecular NH...S hydrogen bonds between the amide NH group and the sulfur atom coordinated to mercury, whereas the tetrakis(thiophenolato)mercury complex 5 does have an intramolecular NH...S hydrogen bond. A relatively weak NH...S hydrogen bond in 5 can be seen in the 1H NMR spectra and the IR spectra in chloroform and in the solid state. The 199Hg NMR spectra in bis(carbamoylthiophenolato)mercury complexes 1-4 show a downfield shift, with an increase in the flow of electrons to mercury(II) from the oxygen atom due to the intramolecular Hg...O bonding interaction. Conversely, the 199Hg NMR spectra in 5 show a high-field shift with a decrease in the flow of electrons to mercury(II) from the sulfur atom due to the intramolecular NH...S hydrogen bond. 相似文献
73.
Mononuclear Zn, Cd, and Hg 1,2-benzenedithiolates with intramolecular NH...S hydrogen bonds, [M(II){1,2-S2-3,6-(RCONH)2C6H2}2](2-) (R = CH 3, t-Bu; M = Zn, Cd, Hg), were synthesized and characterized by X-ray analysis and spectral measurements. The presence of intramolecular NH...S hydrogen bonds was established by the IR spectra. (199)Hg and (113)Cd nuclear magnetic resonance showed a stabilized four-thiolate coordinated structure and suggested the influence of the NH...S hydrogen bonds to ppi(Hg)-ppi(S) interactions. The NH stretching bands show that the NH...S hydrogen bonds in Cd and Hg complexes are stronger than those in the corresponding Zn complex. These results are supported by theoretical calculations. The experimental and theoretical results suggested that the NH...S hydrogen bond influences the efficient capture of toxic Cd and Hg ions by metallothioneins. 相似文献
74.
A new and reliable procedure for constructing five- to seven-membered carbocycles via an endo-mode ring-closing reaction of 1-phenylsulfonylallenes with a substituent that has a terminal active methine moiety at the C1-position has been developed. Trisubstituted 1-phenylsulfonylallenes underwent a similar endo-mode ring-closing reaction to produce the corresponding five- to seven-membered carbocycles, while the formation of six- and seven-membered carbocycles from the corresponding tetrasubstituted allene was not realized. In addition, the introduction of an aromatic ring to the alkyl side chain of the starting allenes made possible the construction not only of normal-sized carbocycles but also an eight-membered framework. 相似文献
75.
76.
Zheng‐Hua Zhang Shuang‐Yi Wan Taka‐aki Okamura Wei‐Yin Sun Norikazu Ueyama 《无机化学与普通化学杂志》2006,632(4):679-683
Two novel lanthanide coordination polymers, [La(tpaa)3(H2O)2] ( 1 ) and [Eu2(BDC)3(DMF)2(H2O)2] ( 2 ) (Htpaa = terephthalamic acid, H2BDC = 1,4‐benzenedicarboxylic acid, DMF = N,N‐dimethylformamide), were hydro(solvo)thermally synthesized by reactions of the corresponding lanthanide nitrate salts with 1,3,5‐triazine‐2,4,6‐tri(4‐benzenecarboxylate) ( L ), in which a simultaneous hydrolysis of the ligand L occurred. Single‐crystal X‐ray analysis revealed that complex 1 comprises one‐dimensional chains that are further interlinked via hydrogen bonds, resulting in a two‐dimensional network; while complex 2 is a three‐dimensional interpenetrated coordination architecture. 相似文献
77.
We propose a new outflow boundary condition, a unilateral condition of Signorini’s type, for the incompressible Navier–Stokes equations. The condition is a generalization of the standard free-traction condition. Its variational formulation is given by a variational inequality. We also consider a penalty approximation, a kind of the Robin condition, to deduce a suitable formulation for numerical computations. Under those conditions, we can obtain energy inequalities that are key features for numerical computations. The main contribution of this paper is to establish the well-posedness of the Navier–Stokes equations under those boundary conditions. Particularly, we prove the unique existence of strong solutions of Ladyzhenskaya’s class using the standard Galerkin’s method. For the proof of the existence of pressures, however, we offer a new method of analysis. 相似文献
78.
79.
Matsuhira T Yamamoto H Onoda A Okamura TA Ueyama N 《Organic & biomolecular chemistry》2006,4(7):1338-1342
In this study, we synthesized two novel carboxylic acid and carboxylate compounds, both of which had an amide group linked with an azomethine moiety to introduce photoinduced switching of the intramolecular NH...O hydrogen bond. We suggest that the cis-carboxylate compound forms a stronger intramolecular NH...O hydrogen bond than the cis-carboxylic acid compound. 相似文献
80.
Gang Wu Xiao-Feng Wang Min Chen Norikazu Ueyama 《Journal of solid state chemistry》2010,183(9):2174-2182
Five new silver(I) complexes [Ag2(L2)2](BF4)2·CH3CN·CH3OH (1), [Ag(L2)(CF3SO3)] (2), [Ag(L3)]ClO4·CH3OH (3), [Ag2(L3)2](CF3SO3)2·CH3CN·CH3OH·H2O (4) and [Ag(L3)]PF6·2CH3CN (5) [L2=1,3,5-tris(2-pyridylmethoxyl)benzene, L3=1,3,5-tris(3-pyridylmethoxyl)benzene] were synthesized and characterized by single crystal X-ray diffraction analyses. In complexes 1-5, ligands L2 and L3 show different conformations and act as three-connectors, while the Ag(I) atom serves as three-connecting node to result in the formation of 2D and 3D frameworks. Complexes 1 and 2 with different counteranions have similar 2D network structure with the same (4,82) topology. Complex 3 has a 3D structure with (10,3)-a topology while complexes 4 and 5 have the same 2D (6,3) topological structure. The results showed that the structure of organic ligands and counteranions play subtle but important role in determining the structure of the complexes. In addition, the photoluminescence and anion-exchange properties of the complexes were investigated in the solid state at room temperature. 相似文献