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Lanthanide Identity Governs Guest-Induced Dimerization in LnIII[15-MC
N(L-pheHA)-5])3+ Metallacrowns
Prof. Carmelo Sgarlata Bernadette L. Schneider Valeria Zito Dr. Rossella Migliore Prof. Matteo Tegoni Prof. Vincent L. Pecoraro Prof. Giuseppe Arena 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(70):17669-17675
Series of lanthanide-containing metallic coordination complexes are frequently presented as structurally analogous, due to the similar chemical and coordinative properties of the lanthanides. In the case of chiral (LnIII[15-MC N(L-pheHA)-5])3+ metallacrowns (MCs), which are well established supramolecular hosts, the formation of dimers templated by a dicarboxylate guest (muconate) in solution of neutral pH is herein shown to have a unique dependence on the identity of the MC's central lanthanide. Calorimetric data and nuclear magnetic resonance diffusion studies demonstrate that MCs containing larger or smaller lanthanides as the central metal only form monomeric host-guest complexes whereas analogues with intermediate lanthanides (for example, Eu, Gd, Dy) participate in formation of dimeric host-guest-host compartments. The driving force for the dimerization event across the series is thought to be a competition between formation of highly stable MCs (larger lanthanides) and optimally linked bridging guests (smaller lanthanides). 相似文献
168.
Shipeng Wu Yinghao Wang Prof. Qiue Cao Prof. Qihua Zhao Dr. Wenhao Fang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(9):3019-3028
High-surface-area mesoporous CeO2 (hsmCeO2) was prepared by a facile organic-template-induced homogeneous precipitation process and showed excellent catalytic activity in imine synthesis in the absence of base from primary alcohols and amines in air atmosphere at low temperature. For comparison, ordinary CeO2 and hsmCeO2 after different thermal treatments were also investigated. XRD, N2 physisorption, UV-Raman, H2 temperature-programmed reduction, O2 temperature-programmed desorption, EPR spectroscopy, and X-ray photoelectron spectroscopy were used to unravel the structural and redox properties. The hsmCeO2 calcined at 400 °C shows the highest specific surface area (158 m2 g−1), the highest fraction of surface coordinatively unsaturated Ce3+ ions (18.2 %), and the highest concentration of reactive oxygen vacancies (2.4×1015 spins g−1). In the model reaction of oxidative coupling of benzyl alcohol and aniline, such an exceptional redox property of the hsmCeO2 catalyst can boost benzylideneaniline formation (2.75 and 5.55 mmol h−1 based on >99 % yield at 60 and 80 °C, respectively) in air with no base additives. It can also work effectively at a temperature of 30 °C and in gram-scale synthesis. These are among the best results for all benchmark ceria catalysts in the literature. Moreover, the hsmCeO2 catalyst shows a wide scope towards primary alcohols and amines with good to excellent yield of imines. The influence of reaction parameters, the reusability of the catalyst, and the reaction mechanism were investigated. 相似文献
169.
Meng Liu Dr. Hao Fan Dr. Ou Zhuo Xiao Du Longqi Yang Prof. Peng Wang Lijun Yang Prof. Qiang Wu Prof. Xizhang Wang Prof. Zheng Hu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(15):3843-3848
Molybdenum disulfide (MoS2) is an intensively studied anode material for lithium-ion batteries (LIBs) owing to its high theoretical capacity, but it is still confronted by severe challenges of unsatisfactory rate capability and cycle life. Herein, few-layer MoS2 nanosheets, vertically grown on hierarchical carbon nanocages (hCNC) by a facile hydrothermal method, introduce pseudocapacitive lithium storage owing to the highly exposed MoS2 basal planes, enhanced conductivity, and facilitated electrolyte access arising from good hybridization with hCNC. Thus, the optimized MoS2/hCNC exhibits reversible capacities of 1670 mAh g−1 at 0.1 A g−1 after 50 cycles, 621 mAh g−1 at 5.0 A g−1 after 500 cycles, and 196 mAh g−1 at 50 A g−1 after 2500 cycles, which are among the best for MoS2-based anode materials. The specific power and specific energy, which can reach 16.1 kW and 252.8 Wh after 3000 cycles, respectively, indicate great potential in high-power and long-life LIBs. These findings suggest a promising strategy for exploring advanced anode materials with high reversible capacity, high-rate capability, and long-term recyclability. 相似文献
170.
We report the results of our investigation of magnetization and heat capacity on a series of compounds CeYxNiGe2 () under the influence of external magnetic field. Our studies of the thermodynamic quantity on these compounds indicate that magnetic frustration persists in Ce0.9Y0.1NiGe2, as also reported for the parent compound CeNiGe2. The weak signature of this frustration is also noted in Ce0.8Y0.2NiGe2, whereas, it is suppressed in Ce0.6Y0.4NiGe2. Heat capacity studies on Ce0.9Y0.1NiGe2 and Ce0.8Y0.2NiGe2 indicate the presence of a new magnetic anomaly at high field which indicates that quantum criticality is absent in these compounds. However, for Ce0.6Y0.4NiGe2 such an anomaly is not noted. For this later compound, the magnetic field (H) and temperature (T) dependence of heat capacity and magnetization obey scaling above critical fields. However, the obtained scaling critical parameter (δ) is 1.6, which is away from mean field value of 3. This deviation suggests the presence of unusual fluctuations and anomalous quantum criticality in these compounds. This unusual fluctuation may arise from disorderness induced by Y-substitution. 相似文献