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991.
Dr. Xi-Sha Zhang Yan-Ying Huang Jing Zhang Dr. Wei Meng Dr. Qian Peng Ruirui Kong Zhenwei Xiao Dr. Jie Liu Miaofei Huang Dr. Yuanping Yi Liangliang Chen Qingrui Fan Dr. Gaobo Lin Dr. Zitong Liu Dr. Guanxin Zhang Dr. Lang Jiang Prof. Dr. Deqing Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(9):3557-3561
Polycyclic aromatic hydrocarbons with hexagons/pentagons or hexagons/heptagons have been intensively investigated in recent years, but those with simultaneous presence of hexagons, pentagons and heptagons remain rare. In this paper, we report dicyclohepta[ijkl,uvwx]rubicene ( DHR ), a non-benzenoid isomer of dibenzo[bc,kl]coronene with two pentagons and two heptagons. We developed an efficient and scalable synthetic method for DHR by using Scholl reaction and dehydrogenation. Crystal structure of DHR shows that the benzenoid rings, two pentagons and two heptagons are coplanar. The bond lengths analysis and the ICSS(1)zz and LOL-π calculations indicate that the incorporation of two formal azulene moieties has an effect on the conjugated structure. The π-electrons of benzenoid and pentagon rings are more delocalized. Cyclic voltammetry studies indicate that DHR shows multiple oxidation and reduction potentials. Interestingly, DHR exhibits unusual S0 to S2 absorption and abnormal anti-Kasha S2 to S0 emission. Moreover, crystals of DHR exhibit semiconducting behaviour with hole mobility up to 0.082 cm2 V−1 s−1. 相似文献
992.
Prof. Shuaijun Yang Ping-An Yin Lin Li Prof. Qian Peng Prof. Xinggui Gu Prof. Ge Gao Prof. Jingsong You Prof. Ben Zhong Tang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(25):10222-10228
Squaraines (SQs) with tunable emission in the solid state is of great importance for various demands; however a remaining challenge is emission quenching upon aggregation. Herein, a unique SQ, named as CIEE-SQ, is designed to exhibit strong emission in crystal, undergoing crystallization-induced reverse from dark 1(n+σ,π*) to bright 1(π,π*) excited states. Such an excited state of CIEE-SQ can be subtly tuned by molecular conformation changes during the unexpected temperature-triggered single-crystal to single-crystal (SCSC) reversible transformation. Furthermore, co-crystallization between CIEE-SQ and chloroform largely stabilize the 1(π,π*) state, enhancing the transition dipole moment and decreasing the reorganization energy to boost the fluorescence, which is promising in data encryption and decryption. 相似文献
993.
Jiabin Zhang Ding Liu Varma Saikam Madhusudhan R. Gadi Christopher Gibbons Xuan Fu Heliang Song Jin Yu Shukkoor M. Kondengaden Prof. Dr. Peng G. Wang Prof. Dr. Liuqing Wen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):19997-20001
Historically, researchers have put considerable effort into developing automation systems to prepare natural biopolymers such as peptides and oligonucleotides. The availability of such mature systems has significantly advanced the development of natural science. Over the past twenty years, breakthroughs in automated synthesis of oligosaccharides have also been achieved. A machine-driven platform for glycopeptide synthesis by a reconstructed peptide synthesizer is described. The designed platform is based on the use of an amine-functionalized silica resin to facilitate the chemical synthesis of peptides in organic solvent as well as the enzymatic synthesis of glycan epitopes in the aqueous phase in a single reaction vessel. Both syntheses were performed by a peptide synthesizer in a semiautomated manner. 相似文献
994.
Yi-Fan Wang Yiyu Liang Yan-Fang Wu Jian Yang Xu Zhang Dr. Dandan Cai Dr. Xu Peng Dr. Mohamedally Kurmoo Prof. Dr. Ming-Hua Zeng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(32):13334-13339
The in situ tracking of the pyrolysis of a binary molecular cluster [Zn7(μ3-CH3O)6(L)6][ZnLCl2]2 is presented with one brucite disk and two mononuclear fragments (L=mmimp: 2-methoxy-6-((methylimino)-methyl)phenolate) to porous carbon using TG-MS from 30 to 900 °C. Following up the spilled gas product during the decomposed reaction of zinc cluster along the temperature rising, and in conjunction with XRD, SEM, BET and other materials characterization, where three key steps were observed: 1) cleavage of the bulky external ligand; 2) reduction of ZnO and 3) volatilization of Zn. The real-time-dependent phase-sequential evolution of the remaining products and the processing of pore forming template transformation are proposed simultaneously. The porous carbon structure featuring a uniform nano-sized pore distribution synthesized at 900 °C with the highest surface area of 1644 m2 g−1 and pore volume of 0.926 cm3 g−1 exhibits the best known capacitance of 662 F g−1 at 0.5 A g−1. 相似文献
995.
Bingjie Zhao Huiqin Wang Dr. Chunmiao Han Peng Ma Zhe Li Peng Chang Prof. Hui Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(43):19204-19209
Device simplification is of practical significance for organic light emitting diodes (OLEDs), and remains the great challenge for deep-red emitters. Herein, a deep-red thermally activated delayed fluorescence molecule ( p TPA-DPPZ ) is reported which features a T shaped structure containing two triphenylamine (TPA) donors, one either side of a planar dipyridophenazine (DPPZ) acceptor. The rational spatial arrangement of the functional groups leads to limited but sufficient molecular packing for effective carrier transport. The neat p TPA-DPPZ film achieves an around 90-fold improved radiation rate constant of 107 s−1 and the nearly unitary reverse intersystem crossing (RISC) efficiency, as well as accelerated emission decays for quenching suppression. The high radiation and RISC result in a photoluminescence quantum yield of 87 %. The bilayer OLED based on the p TPA-DPPZ emissive layer achieved the record external quantum efficiencies of 12.3 % for maximum and 10.4 % at 1000 nits, accompanied by the deep-red electroluminescence with the excellent color purity. 相似文献
996.
Luocai Yi Dr. Junxiang Chen Ping Shao Dr. Junheng Huang Xinxin Peng Junwei Li Dr. Genxiang Wang Chi Zhang Prof. Zhenhai Wen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20287-20294
Two-dimensional (2D) monometallic pnictogens (antimony or Sb, and bismuth or Bi) nanosheets demonstrate potential in a variety of fields, including quantum devices, catalysis, biomedicine and energy, because of their unique physical, chemical, electronic and optical properties. However, the development of general and high-efficiency preparative routes toward high-quality pnictogen nanosheets is challenging. A general method involving a molten-salt-assisted aluminothermic reduction process is reported for the synthesis of Sb and Bi nanosheets in high yields (>90 %). Electrocatalytic CO2 reduction was investigated on the Bi nanosheets, and high catalytic selectively to formate was demonstrated with a considerable current density at a low overpotential and an impressive stability. Bi nanosheets continuously convert CO2 into formate in a flow cell operating for one month, with a yield rate of 787.5 mmol cm−2 h−1. Theoretical results suggest that the edge sites of Bi are far more active than the terrace sites. 相似文献
997.
Feng-Xing Li Shu-Jian Ren Pei-Fang Li Peng Yang Prof. Jin Qu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(42):18631-18636
The rapid synthesis of marine ladder polyethers from polyepoxide precursors (in analogy with the biosynthetic pathway hypothesized by Nakanishi) is hampered by the fact that the exo-selective epoxide-opening cyclization cascade that gives THF-type polyethers is preferred over the endo-selective cascade that gives the desired products. We found that perfluoro-tert-butanol (PFTB) cooperating with 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM]BF4) can promote endo-selective epoxide-opening cyclization reactions of trisubstituted epoxy alcohols. Starting from readily accessible homochiral polyepoxy alcohols with a methyl group at all the endo-cyclization sites, we were able to construct polyethers up to five consecutive fused 6-, 7-, and/or 8-membered rings in one step. Notably, molecules with the 7/7/6/6 and 7/7/6/7/6 polyether frameworks of hemibrevetoxin B and brevenal, respectively, could be synthesized in 40 % and 17 % chemical yields. 相似文献
998.
Yun Liu Guangze Yang Song Jin Run Zhang Peng Chen Tengjisi Lianzhou Wang Dong Chen David A. Weitz Chun-Xia Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20240-20249
Understanding drug-release kinetics is critical for the development of drug-loaded nanoparticles. We developed a J-aggregate-based Förster-resonance energy-transfer (FRET) method to investigate the release of novel high-drug-loading (50 wt %) nanoparticles in comparison with low-drug-loading (0.5 wt %) nanoparticles. Single-dye-loaded nanoparticles form J-aggregates because of the high dye-loading (50 wt %), resulting in a large red-shift (≈110 nm) in the fluorescence spectrum. Dual-dye-loaded nanoparticles with high dye-loading using FRET pairs exhibited not only FRET but also a J-aggregate red-shift (116 nm). Using this J-aggregate-based FRET method, dye-core–polymer-shell nanoparticles showed two release processes intracellularly: the dissolution of the dye aggregates into dye molecules and the release of the dye molecules from the polymer shell. Also, the high-dye-loading nanoparticles (50 wt %) exhibited a slow release kinetics in serum and relatively quick release in cells, demonstrating their great potential in drug delivery. 相似文献
999.
Dr. Shaoguang Zhang Dr. Peng Cui Tianchang Liu Qiuran Wang Thomas J. Longo Laura M. Thierer Dr. Brian C. Manor Dr. Michael R. Gau Dr. Patrick J. Carroll Prof. Dr. Georgia C. Papaefthymiou Prof. Dr. Neil C. Tomson 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(35):15327-15331
Despite their connection to ammonia synthesis, little is known about the ability of iron-bound, bridging nitrides to form N−H bonds. Herein we report a linear diiron bridging nitride complex supported by a redox-active macrocycle. The unique ability of the ligand scaffold to adapt to the geometric preference of the bridging species was found to facilitate the formation of N−H bonds via proton-coupled electron transfer to generate a μ-amide product. The structurally analogous μ-silyl- and μ-borylamide complexes were shown to form from the net insertion of the nitride into the E−H bonds (E=B, Si). Protonation of the parent bridging amide produced ammonia in high yield, and treatment of the nitride with PhSH was found to liberate NH3 in high yield through a reaction that engages the redox-activity of the ligand during PCET. 相似文献
1000.
Meiling Chen Chenxi Peng Yaoquan Su Xue Chen Prof. Yuezhou Zhang Prof. Yu Wang Prof. Juanjuan Peng Dr. Qiang Sun Prof. Xiaowang Liu Prof. Wei Huang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(47):21174-21181
The ability to incorporate functional metal ions (Mn+) into metal–organic coordination complexes adds remarkable flexibility in the synthesis of multifunctional organic–inorganic hybrid materials with tailorable electronic, optical, and magnetic properties. We report the cation-exchanged synthesis of a diverse range of hollow Mn+-phytate (PA) micropolyhedra via the use of hollow Co2+-PA polyhedral networks as templates at room temperature. The attributes of the incoming Mn+, namely Lewis acidity and ionic radius, control the exchange of the parent Co2+ ions and the degree of morphological deformation of the resulting hollow micropolyhedra. New functions can be obtained for both completely and partially exchanged products, as supported by the observation of Ln3+ (Ln3+=Tb3+, Eu3+, and Sm3+) luminescence from as-prepared hollow Ln3+-PA micropolyhedra after surface modification with dipicolinic acid as an antenna. Moreover, Fe3+- and Mn2+-PA polyhedral complexes were employed as magnetic contrast agents. 相似文献