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51.
For the purpose of utilizing ESDIAD as a real-time probe for surface processes, we have developed an instrument which can measure ESDIAD images and time of flight (TOF) spectra of desorbing ions in temperature-programmed surface processes. TOF measurements are carried out to identify the mass and to determine the kinetic energy distribution of the desorbed ions. This temperature-programmed (TP-) ESDIAD/TOF system was used to observe coadsorption layers of methylamine and CO on Ru(001) which have been previously studied by our group using LEED, TPD and HREELS, also drawing upon a comparison of findings with the coadsorption system of CO and ammonia. ESDIAD images acquired for temperature-programmed surface processes in real time were found to provide new insight into the dynamic behaviour of the coadsorption layers. As to the pure adsorption of ammonia and methylamine, the second and the first (chemisorbed) layers can be easily discriminated in their different ESD detection efficiency due to the difference in neutralization rate. The intensity change of H+ ions with temperature shows the process of the decomposition of methylamine to be dependent on CO coverage. The intensity of O+ originating from CO changes due to the change of CO adsorption site in the reaction process. The angular distribution of H+ ions which correspond to CH2=NH…Ru species appears at 250–300 K in the presence of high CO pre-coverage. 相似文献
52.
Dr. Kosuke Ono Shunsuke Shimo Dr. Kohei Takahashi Dr. Nobuhiro Yasuda Dr. Hidehiro Uekusa Prof. Nobuharu Iwasawa 《Angewandte Chemie (International ed. in English)》2018,57(12):3113-3117
Dynamic interconversion between large covalent organic cages was achieved simply by heating or acid/base treatment. A mixture of the boroxine cages 12‐mer and 15‐mer was cleanly converted into a pyridine adduct of the 9‐mer boroxine cage upon treatment with pyridine, and the geometry of N‐coordinated boron atoms changed from trigonal to tetrahedral. The reverse reaction was achieved by heating or acid treatment. In this process, the larger boroxine cages 12‐mer and 15‐mer were found to be entropically favored owing to the release of free pyridine molecules from 9‐mer ?6 Py. 相似文献
53.
Utilization of Donor–Acceptor Interactions for the Catalytic Acceleration of Nucleophilic Additions to Aromatic Carbonyl Compounds 下载免费PDF全文
Tatsuhiro Uchikura Dr. Kosuke Ono Dr. Kohei Takahashi Prof. Nobuharu Iwasawa 《Angewandte Chemie (International ed. in English)》2018,57(8):2130-2133
A conceptually new method for the catalytic electrophilic activation of aromatic carbonyl substrates, by utilizing donor–acceptor interactions between an electron‐deficient macrocyclic boronic ester host ( [2+2] BTH‐F ) and an aromatic carbonyl guest substrate, was realized. In the presence of a catalytic amount of [2+2] BTH‐F , dramatic acceleration of the nucleophilic addition of a ketene silyl acetal towards either electron‐rich aromatic aldehydes or ketones was achieved. Several control experiments confirmed that inclusion of the aromatic substrates within [2+2] BTH‐F , through efficient donor–acceptor interactions, is essential for the acceleration of the reaction. 相似文献
54.
[reaction: see text] Oligomerization of Pd(OAc)2(L)2 (L = pyridine derivatives), a catalyst for the air oxidation of alcohols, is studied with MALDI TOF mass, using dithranol as the matrix. The degree of the Pd oligomerization is influenced by the pyridine ligands, and this ligand effect is similar to one observed for Pd black formation in the catalysis. 相似文献
55.
56.
Tetsuo Iwasawa 《Tetrahedron letters》2008,49(36):5244-5246
A straightforward route to functionalized pentaarylbenzene derivatives is described, involving the effective lithiation method of 1-iodo-2,3,4,5,6-pentaarylbenzene. The activated pentaarylbenzene is a potential synton for producing organic materials. 相似文献
57.
Kazuhiro Ohashi Shigenori MiharaAkihiro H. Sato Masataka IdeTetsuo Iwasawa 《Tetrahedron letters》2014
A convenient synthesis of 1-haloethenamides has been achieved by utilizing halotrimethylsilane (TMSX, X = Cl, Br, I) and water. Halotrimethylsilane in 1 M CH2Cl2 solution functions as a halogen source of the in situ generated HX, and the HX added to the terminal triple bonds of ynamides in Markovnikov fashion. 相似文献
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59.
[reaction: see text] A concise method for the preparation of isochromene carboxylates has been developed by the regioselective 1,6-addition of various nucleophiles such as Grignard reagents, alkoxide, and cyanide onto benzopyranylidenetungsten(0) complexes, followed by iodine oxidation of the addition intermediates. 相似文献
60.
Rh-catalyzed direct carboxylation of unactivated aryl C-H bond under atmospheric pressure of carbon dioxide was realized via chelation-assisted C-H activation for the first time. Variously substituted and functionalized 2-arylpyridines and 1-arylpyrazoles underwent the carboxylation in the presence of the rhodium catalyst and a stoichiometric methylating reagent, AlMe(2)(OMe), to give carboxylated products in good yields. The catalysis is proposed to consist of methylrhodium(I) species as the key intermediate, which undergoes C-H activation to afford rhodium(III), followed by reductive elimination of methane to give nucleophilic arylrhodium(I). This approach demonstrates promising application of C-H bond activation strategy in the field of carbon dioxide fixation. 相似文献