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101.
Jianbo Yu Aidaer Muhetaer Xiaowen Gao Zhenzhen Zhang Yuying Yang Prof. Qi Li Prof. Langxing Chen Prof. Haichao Liu Prof. Dongsheng Xu 《Angewandte Chemie (International ed. in English)》2023,62(28):e202303135
Photo-assisted reverse water gas shift (RWGS) reaction is regarded green and promising in controlling the reaction gas ratio in Fischer Tropsch synthesis. But it is inclined to produce more byproducts in high H2 concentration condition. Herein, LaInO3 loaded with Ni-nanoparticles (Ni NPs) was designed to obtain an efficient photothermal RWGS reaction rate, where LaInO3 was enriched with oxygen vacancies to roundly adsorbing CO2 and the strong interaction with Ni NPs endowed the catalysts with powerful H2 activity. The optimized catalyst performed a large CO yield rate (1314 mmol gNi−1 h−1) and ≈100 % selectivity. In situ characterizations demonstrated a COOH* pathway of the reaction and photoinduced charge transfer process for reducing the RWGS reaction active energy. Our work provides valuable insights on the construction of catalysts concerning products selectivity and photoelectronic activating mechanism on CO2 hydrogenation. 相似文献
102.
Dr. Jin-Bo Pan Bing-Hao Wang Dr. Sheng Shen Dr. Lang Chen Prof. Dr. Shuang-Feng Yin 《Angewandte Chemie (International ed. in English)》2023,62(38):e202307246
Core-shell photoanodes have shown great potential for photoelectrochemical (PEC) water oxidation. However, the construction of a high-quality interface between the core and shell, as well as a highly catalytic surface, remains a challenge. Herein, guided by computation, we present a BiVO4 photoanode coated with ZnCoFe polyphthalocyanine using pyrazine as a coordination agent. The bidirectional axial coordination of pyrazine plays a dual role by facilitating intimate interfacial contact between BiVO4 and ZnCoFe polyphthalocyanine, as well as regulating the electron density and spin configuration of metal sites in ZnCoFe phthalocyanine, thereby promoting the potential-limiting step of *OOH desorption. The resulting photoanode displayed a high photocurrent density of 5.7±0.1 mA cm−2 at 1.23 VRHE. This study introduces a new approach for constructing core–shell photoanodes, and uncovers the key role of pyrazine axial coordination in modulating the catalytic activity of metal phthalocyanine. 相似文献
103.
Jiaqian Zhou Peiran Xie Chao Wang Tieyuan Bian Dr. Jian Chen Dr. Yang Liu Zhu Guo Congcong Chen Xin Pan Prof. Dr. Min Luo Prof. Dr. Jun Yin Prof. Dr. Lingling Mao 《Angewandte Chemie (International ed. in English)》2023,62(35):e202307646
Double perovskites (DP) have attracted extensive attention due to their rich structures and wide application prospects in the field of optoelectronics. Here, we report 15 new Bi-based double perovskite derived halides with the general formula of A2BBiX6 (A=organic cationic ligand, B=K or Rb, X=Br or I). These materials are synthesized using organic ligands to coordinate with metal ions with a sp3 oxygen, and diverse structure types have been obtained with distinct dimensionalities and connectivity modes. The optical band gaps of these phases can be tuned by changing the halide, the organic ligand and the alkali metal, varying from 2.0 to 2.9 eV. The bromide phases exhibit increasing photoluminescence (PL) intensity with decreasing temperature, while the PL intensity of iodide phases changes nonmonotonically with temperature. Because the majority of these phases are non-centrosymmetric, second harmonic generation (SHG) responses are also measured for selected non-centrosymmetric materials, showing different particle-size-dependent trends. Our findings give rise to a series of new structural types to the DP family, and provide a powerful synthetic handle for symmetry breaking. 相似文献
104.
Hui Luo Dr. Kejun Bu Dr. Yanfeng Yin Dong Wang Cuimi Shi Songhao Guo Tonghuan Fu Jiayuan Liang Bingyan Liu Dr. Dongzhou Zhang Prof. Liang-Jin Xu Prof. Qingyang Hu Prof. Yang Ding Prof. Shengye Jin Prof. Wenge Yang Prof. Biwu Ma Prof. Xujie Lü 《Angewandte Chemie (International ed. in English)》2023,62(37):e202304494
Low-dimensional (low-D) organic metal halide hybrids (OMHHs) have emerged as fascinating candidates for optoelectronics due to their integrated properties from both organic and inorganic components. However, for most of low-D OMHHs, especially the zero-D (0D) compounds, the inferior electronic coupling between organic ligands and inorganic metal halides prevents efficient charge transfer at the hybrid interfaces and thus limits their further tunability of optical and electronic properties. Here, using pressure to regulate the interfacial interactions, efficient charge transfer from organic ligands to metal halides is achieved, which leads to a near-unity photoluminescence quantum yield (PLQY) at around 6.0 GPa in a 0D OMHH, [(C6H5)4P]2SbCl5. In situ experimental characterizations and theoretical simulations reveal that the pressure-induced electronic coupling between the lone-pair electrons of Sb3+ and the π electrons of benzene ring (lp-π interaction) serves as an unexpected “bridge” for the charge transfer. Our work opens a versatile strategy for the new materials design by manipulating the lp-π interactions in organic–inorganic hybrid systems. 相似文献
105.
Si-Yong Yin Qiansujia Zhou Dr. Chen-Xu Liu Prof. Dr. Qing Gu Prof. Dr. Shu-Li You 《Angewandte Chemie (International ed. in English)》2023,62(37):e202305067
Enantioselective synthesis of N−N biaryl atropisomers is an emerging area but remains underexplored. The development of efficient synthesis of N−N biaryl atropisomers is in great demand. Herein, the construction of N−N biaryl atropisomers through iridium-catalyzed asymmetric C−H alkylation is reported for the first time. In the presence of readily available Ir precursor and Xyl-BINAP, a variety of axially chiral molecules based on indole-pyrrole skeleton were obtained in good yields (up to 98 %) with excellent enantioselectivity (up to 99 % ee). In addition, N−N bispyrrole atropisomers could also be synthesized in excellent yields and enantioselectivity. This method features perfect atom economy, wide substrate scope, and multifunctionalized products allowing diverse transformations. 相似文献
106.
Xiaoyang Cheng Xiaotian Jiang Shuhu Yin Lifei Ji Yani Yan Guang Li Rui Huang Prof. Chongtai Wang Prof. Honggang Liao Prof. Yanxia Jiang Prof. Shigang Sun 《Angewandte Chemie (International ed. in English)》2023,62(34):e202306166
To achieve the Fe−N−C materials with both high activity and durability in proton exchange membrane fuel cells, the attack of free radicals on Fe−N4 sites must be overcome. Herein, we report a strategy to effectively eliminate radicals at the source to mitigate the degradation by anchoring CeO2 nanoparticles as radicals scavengers adjacent (Scaad-CeO2) to the Fe−N4 sites. Radicals such as ⋅OH and HO2⋅ that form at Fe−N4 sites can be instantaneously eliminated by adjacent CeO2, which shortens the survival time of radicals and the regional space of their damage. As a result, the CeO2 scavengers in Fe−NC/Scaad-CeO2 achieved ∼80 % elimination of the radicals generated at the Fe−N4 sites. A fuel cell prepared with the Fe−NC/Scaad-CeO2 showed a smaller peak power density decay after 30,000 cycles determined with US DOE PGM-relevant AST, increasing the decay of Fe−NCPhen from 69 % to 28 % decay. 相似文献
107.
Dr. Yunqin Zhang Leilei Wang Qingli Zhou Zuoshan Li Dan Li Caixia Yin Prof. Xiufang Wang Prof. Guozhi Xiao 《Angewandte Chemie (International ed. in English)》2023,62(22):e202301351
Lipopolysaccharides from Bacteroides vulgatus represent interesting targets for the treatment of inflammatory bowel diseases. However, efficient access to long, branched and complex lipopolysaccharides remains challenging. Herein, we report the modular synthesis of a tridecasaccharide from Bacteroides vulgates through an orthogonal one-pot glycosylation strategy based on glycosyl ortho-(1-phenylvinyl)benzoates, which avoids the issues of thioglycoside-based one-pot synthesis. Our approach also features: 1) 5,7-O-di-tert-butylsilylene-directed glycosylation for stereoselective construction of the α-Kdo linkage; 2) hydrogen-bond-mediated aglycone delivery for the stereoselective formation of β-mannosidic bonds; 3) remote anchimeric assistance for stereoselective assembly of the α-fucosyl linkage; 4) several orthogonal one-pot synthetic steps and strategic use of orthogonal protecting groups to streamline oligosaccharide assembly; 5) convergent [1+6+6] one-pot synthesis of the target. 相似文献
108.
Prof. Dr. Dengrong Sun Lok Wing Wong Hok Yin Wong Ka Hei Lai Dr. Lin Ye Xinyao Xv Prof. Dr. Thuc Hue Ly Prof. Dr. Qingming Deng Prof. Dr. Jiong Zhao 《Angewandte Chemie (International ed. in English)》2023,62(4):e202216008
The direct utilization of metal–organic frameworks (MOFs) for electrocatalytic oxygen evolution reaction (OER) has attracted increasing interests. Herein, we employ the low-dose integrated differential phase contrast-scanning transmission electron microscopy (iDPC-STEM) technique to visualize the atomic structure of multivariate MOFs (MTV-MOFs) for guiding the structural design of bulk MOFs for efficient OER. The iDPC-STEM images revealed that incorporating Fe3+ or 2-aminoterephthalate (ATA) into Ni-BDC (BDC: benzenedicarboxylate) can introduce inhomogeneous lattice strain that weaken the coordination bonds, which can be selectively cleaved via a mild heat treatment to simultaneously generate coordinatively unsaturated metal sites, conductive Ni@C and hierarchical porous structure. Thus, excellent OER activity with current densities of 10 and 100 mA cm−2 are achieved over the defective MOFs at small overpotentials of 286 mV and 365 mV, respectively, which is superior to the commercial RuO2 catalyst and most of the bulk MOFs. 相似文献
109.
Dr. Ligang Wang Dr. Hui Su Zhuang Zhang Junjie Xin Hai Liu Dr. Xiaoge Wang Dr. Chenyu Yang Xiao Liang Dr. Shunwu Wang Dr. Huan Liu Yanfei Yin Taiyan Zhang Prof. Yang Tian Dr. Yaping Li Prof. Qinghua Liu Prof. Xiaoming Sun Prof. Junliang Sun Prof. Dingsheng Wang Prof. Yadong Li 《Angewandte Chemie (International ed. in English)》2023,62(49):e202314185
Developing cost-effective and sustainable acidic water oxidation catalysts requires significant advances in material design and in-depth mechanism understanding for proton exchange membrane water electrolysis. Herein, we developed a single atom regulatory strategy to construct Co−Co dinuclear active sites (DASs) catalysts that atomically dispersed zirconium doped Co9S8/Co3O4 heterostructure. The X-ray absorption fine structure elucidated the incorporation of Zr greatly facilitated the generation of Co−Co DASs layer with stretching of cobalt oxygen bond and S−Co−O heterogeneous grain boundaries interfaces, engineering attractive activity of significantly reduced overpotential of 75 mV at 10 mA cm−2, a breakthrough of 500 mA cm−2 high current density, and water splitting stability of 500 hours in acid, making it one of the best-performing acid-stable OER non-noble metal materials. The optimized catalyst with interatomic Co−Co distance (ca. 2.80 Å) followed oxo-oxo coupling mechanism that involved obvious oxygen bridges on dinuclear Co sites (1,090 cm−1), confirmed by in situ SR-FTIR, XAFS and theoretical simulations. Furthermore, a major breakthrough of 120,000 mA g−1 high mass current density using the first reported noble metal-free cobalt anode catalyst of Co−Co DASs/ZCC in PEM-WE at 2.14 V was recorded. 相似文献
110.
Hongwu Jiang Kaiwen Li Shuangfeng Dong Prof. Zhuqi Chen Prof. Guochuan Yin 《European journal of organic chemistry》2023,26(35):e202300598
Transition-metal-catalyzed oxidative C−H amination reactions are among the most attractive topics in organic synthesis to construct nitrogen-containing motifs. The challenge is that most of these reactions employed stoichiometric oxidants to achieve satisfied catalytic efficiencies. Herein, we report a Pd(II)/LA-catalyzed (LA: Lewis acid) oxidative C−H amination reaction of 2-acetaminobiphenyls to construct carbazoles by using dioxygen balloon as the sole oxidant source, and the presence of LA sharply improved the catalytic efficiency of Pd(OAc)2. Remarkably, in certain cases, the deacetylation of the annulation product happened under standard conditions to afford free carbazoles as the final product. The H/D exchange studies confirmed the reversibility of C−H activation and also disclosed multiple C−H activation sites by using −NAc and −NTs as the directing groups. In addition, the palladacycle compound was identified through 1H NMR characterizations and proved to be the intermediate prior to the carbazole formation. 相似文献