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471.
Dr. Shinsuke Nishida Dr. Junya Kawai Miki Moriguchi Tomohiro Ohba Naoki Haneda Dr. Kozo Fukui Prof. Akira Fuyuhiro Prof. Daisuke Shiomi Prof. Kazunobu Sato Prof. Takeji Takui Prof. Kazuhiro Nakasuji Prof. Yasushi Morita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(36):11904-11915
The tri‐tert‐butylphenalenyl (TBPLY) radical exists as a π dimer in the crystal form with perfect overlapping of the singly occupied molecular orbitals (SOMOs) causing strong antiferromagnetic exchange interactions. 2,5‐Di‐tert‐butyl‐6‐oxophenalenoxyl (6OPO) is a phenalenyl‐based air‐stable neutral π radical with extensive spin delocalization and is a counter analogue of phenalenyl in terms of the topological symmetry of the spin density distribution. X‐ray crystal structure analyses showed that 8‐tert‐butyl‐ and 8‐(p‐XC6H4)‐6OPOs (X=I, Br) also form π dimers in the crystalline state. The π‐dimeric structure of 8‐tert‐butyl‐6OPO is seemingly similar to that of TBPLY even though its SOMO–SOMO overlap is small compared with that of TBPLY. The 8‐(p‐XC6H4) derivatives form slipped stacking π dimers in which the SOMO–SOMO overlaps are greater than in 8‐tert‐butyl‐6OPO, but still smaller than in TBPLY. The solid‐state electronic spectra of the 6OPO derivatives show much weaker intradimer charge‐transfer bands, and SQUID measurements for 8‐(p‐BrC6H4)‐6OPO show a weak antiferromagnetic exchange interaction in the π dimer. These results demonstrate that the control of the spin distribution patterns of the phenalenyl skeleton switches the mode of exchange interaction within the phenalenyl‐based π dimer. The formation of the relevant multicenter–two‐electron bonds is discussed. 相似文献
472.
Masaaki Yoshifuji Kozo Toyota Naoki Inamoto Ken Hirotsu Taiichi Higuchi Shigeru Nagase 《Phosphorus, sulfur, and silicon and the related elements》2013,188(3):237-243
Abstract The X-ray analyses of sterically protected Z-2-t-butyldimethylsilyloxy-2-phenylphosphaethylene (Z-2) and 3,3-diphenyl-1-phosphaallene (3) were carried out and the structures of the parent compounds, HP[dbnd]CH2 and HP[dbnd]C[dbnd]CH2, were optimized by ab initio methods. 相似文献
473.
Masaaki Yoshifuji Kozo Toyota 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-4):589-592
Abstract: Sterically protected low-coordinated phosphorus-containing cyclobutenes were prepared and characterized as well as [4]radialenes. The reactions were studied involving E/Z isomerization, transition-metal complex formation, and coupling reactions catalyzed by some palladium complex ligated with diphosphacyclobutenes. 相似文献
474.
475.
Biomass gasification using supercritical water is a promising way to produce hydrogen gas. However, this method might release toxic heteroatomic compounds. It is therefore important to clarify reaction pathways for efficiently obtaining hydrogen gas and suppressing environmental burden. L-cysteine was adopted for a test reagent containing sulfur and determination of the sulfur compound reaction pathways was studied by Li+-ion attachment mass spectrometry. It was found that H2S, CO, CO2, SO, SO2 and SO3 gasses were released at high concentrations in the gas phase during the hydrothermal reaction. By adding Ca(OH)2 as alkali, the pathway of these gasses were, however, suppressed into the liquid phase so that the toxic emissions to the gas phase could be avoided. 相似文献
476.
Shigetaka Kawai Thijs Bouwhuis Yoshiaki Abe Aiko Yakeno Taku Nonomura Hikaru Aono Akira Oyama Harry W. M. Hoeijmakers Kozo Fujii 《Theoretical and Computational Fluid Dynamics》2018,32(6):805-820
This study investigates the relationship between body-force fields and maximum velocity induced in quiescent air for development of a simple body-force model of a plasma actuator. Numerical simulations are conducted with the body force near a wall. The spatial distribution and temporal variation of the body force are a Gaussian distribution and steady actuation, respectively. The dimensional analysis is performed to derive a reference velocity and Reynolds number based on the body-force distribution. It is found that the derived Reynolds number correlates well with the nondimensional maximum velocity induced in quiescent conditions when the center of the Gaussian distribution is fixed at the wall. Additionally, two flow regimes are identified in terms of the Reynolds number. Considering the variation of the center of gravity of force fields, another Reynolds number is defined by introducing a new reference length. The nondimensional maximum velocity is found to be scaled with the latter Reynolds number, i.e., the maximum induced velocity in quiescent conditions is determined from three key parameters of the force field: the total induced momentum per unit time, the height of the center of gravity, and the standard deviation from it. This scaling turns out to be applicable to existing body-force models of the plasma actuator, despite the force distributions different from the Gaussian distribution. Comparisons of velocity profiles with experimental data validate the results and show that the flow induced by a plasma actuator can be simulated with simple force distributions by adjustment of the key body-force parameters. 相似文献
477.