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91.
The time-dependent energy distribution of solvation dynamics is studied by molecular dynamics simulations of a Lennard-Jones mixture. We calculate the response functions of the average and the variance which correspond to the spectral peak shift and bandwidth. Our calculation shows that the variance relaxation is slower than that of the average. The result agrees qualitatively with the experimental results. Dividing the obtained response functions into subcomponents caused by each solvent, we find that the relaxation is dominated by that solvent which strongly interacts with the solute. Extracting the redistribution component from the response functions, we find that it causes the slower relaxation of the response function. Thus, we conclude that the difference of the slower relaxations between the average and variance is caused by the redistribution process. 相似文献
92.
Sato K Tamura M Tamoto K Omote M Ando A Kumadaki I 《Chemical & pharmaceutical bulletin》2000,48(7):1023-1025
We have reported that the reaction of ethyl bromodifluoroacetate (1) with alkenyl iodides in the presence of copper powder gives ethyl alkenyldifluoroacetates. As an extension of this reaction, reaction of 1 with Michael acceptors in the presence of copper powder was examined and found to give 1,4-addition products selectively, unless the acceptor has a group stabilizing a radical intermediate, such as a phenyl group. 相似文献
93.
“Truncated” [1.1.1.1] pagodanes like the [1.1.0.0] and [0.0.0.0] homologues3 and 4 (EStr = 146.1 – 171.5 kcal mol?1, MM2) are potential precursors of unusual unsaturated homoconjugated radical cations and σ-bishomoaromatic dications. Attempts are presented toward the synthesis of 3 - starting out from [1.1.1.1] pagodane-4,9-dione 9 and diaza [2.2.1.1] pagodadiene 11 by cycloelimination (unsuccessful) and by Favorskii-type ring contraction methodologies. Control experiments with the model diketone 19 documented the limitations for α,α′-difunctionalization of 9 as the prerequisite for one-pot double Favorskii-type ring contraction. A de novo synthesis for such α,α′-disubstituted derivatives of 9(54) was not sufficiently expeditious to open a practical access to 3. Sequential double bridgehead hydroxylation of 9, successfully practized with model 19, similarly suffered from inherent cage effects and allowed only limited yields of [1.1.1.0] pagodanone 10, the intermediate on the way to 3. 相似文献
94.
Photochemical behaviors of the pyrazinone derivatives 5,6,7,8-tetrahydroquinoxalin-2(1H)-ones 1a – c and 1,5,6,7,8,9-hexahydro-2H-cyclohepta[b]pyrazin-2-one 1d were investigated. Dye-sensitized photo-oxygenation of 1a-c gave the 1:1 adducts 5a – c of the corresponding 3,8a-epidioxy-3,5,6,7,8,8a-hexahydroquinoxalin-2(1H)-one 4 and H2O, whereas 1d gave 3,9a-epidioxy-1,3,5,6,7,8,9,9a-octahydro-2H-cyclohepta[b]pyrazin-2-one 4d (Scheme 2). The different kind of products was interpreted as being the result of the ring strain and steric hindrance of endoperoxides produced from 1a – d with singlet oxygen. Irradiation of 1a – b in the presence of alkenes gave tricyclic azetidine derivatives 9 by [2 + 2] cycloaddition of the C?N bond of 1 to the alkene. 相似文献
95.
1-Aryl-2(1H)pyrimidinones I reacted with α-haloesters in the presence of zinc to give mainly 3,4-dihydro-4-alkoxycarbonylmethyl-1-aryl-2(1H)pyrimidinones IV in addition to the minor products of 3,6-dihydro-6-alkoxycarbonylmethyl-1-aryl-2(1H)pyrimidinones V. Further, 3,4-dihydro derivatives IVa-c were successfully converted into the corresponding exomethylene compounds Vla-c in high yields. 相似文献
96.
The NMR spectra of the benzohexahelicenes have been analyzed. The conformation of the helical structure is not changed to a large extent by the benzo-groups. Some flattening of a part of the helix results in a small downfield shift of the protons on the terminal rings and in a larger upfield shift of proton A in II ascribed to a change in the ring current in the pitch of the helix. A gradual upfield shift is found for protons of the terminal rings by an increase in overcrowding of the benzo-groups. 相似文献
97.
Choji Kashima Akira Katoh Nobutoshi Yoshiwara Yoshimori Omote 《Journal of heterocyclic chemistry》1981,18(8):1595-1596
1-Aryl-3,4,5,6-tetrahydro-2-(1H)pyrimidinones (I) underwent reductive ring opening reaction with lithium aluminum hydride to afford N-aryl-2,4-diaminopentanes (II) in good yields. On the other hand, 3,4,5,6-tetrahydro-3,4,6-trimethyl-1-phenyl-2-(1H)-pyrimidinone (V) gave only cyclic diamine, 3,4,6-trimethyl-1-phenylhexahydropyrimidine (VI), in 60% yield. 相似文献
98.
Yoshimori Omote Yasuomi Takizawa Shunichi Mochida Yoshihiko Tsuda Noboru Sugiyama 《Journal of heterocyclic chemistry》1977,14(8):1361-1363
The oxidative coupling of indole with three naphthols, 2-naphthol, 2,3-dihydroxynaphthalene and 2,7-dihydroxynaphthalene gave 1,1-bis(3′-indolyl)-2(1H)naphthalenone, 1,1-bis(3′-indolyl)-3-hydroxy-2(1H)naphthalenone and 1,1-bis(3′-indolyl)-7-hydroxy-2(1H)naphthalenone, respectively. The coupling of indole with protocatechuic aldehyde gave bis-(3-indolyl)-(3′,4′-di-hydroxyphenyl)methane and that of indole with homocatechol gave 3-(2′-methyl-3′,4′-di-hydroxyphenyl)indole. 相似文献
99.
We have synthesized novel axially chiral ligand with two chiral centers, (R)-(R)(2)- and (S)-(S)(2)-2,2'-bis(2,2,2-trifluoro-1-hydroxyethyl)biphenyl (1), which showed a high asymmetric induction when used as ligand. Here, another new approach to 1 by kinetic and thermodynamic resolution is presented which gave these ligands in a much shorter steps, in a higher yield, and in a higher enantiomeric excess. 相似文献
100.
Takehiko Nishio Tatsuhiro Tokunaga Yoshimori Omote 《Journal of heterocyclic chemistry》1985,22(2):405-407
β-Sulfenyl α, β-unsaturated ketones 1a-c reacted with guanidine or amidines to give pyrimidine derivatives 3 in 14-76% yields. Treatment of ketones 1 with diamines such as ethylenediamine and o -phenylenediamine afforded the seven-membered heterocycles, 2,3-dihydro-1,4-diazepine 5 and 2,3-benzo-1,4-diazepines 8a-c . 相似文献