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91.
Hong Zhang Chenxu Zhao Jianxi Yao Wallace C. H. Choy 《Angewandte Chemie (International ed. in English)》2023,62(24):e202219307
Advancing inverted (p-i-n) perovskite solar cells (PSCs) is critical for commercial applications given their compatibility with different bottom cells for tandem photovoltaics, low-temperature processability (≤100 °C), and promising operational stability. Although inverted PSCs have achieved an efficiency of over 25 % using doped or expensive organic hole transport materials (HTMs), their synthesis cost and stability still cannot meet the requirements for their commercialization. Recently, dopant-free and low-cost non-stoichiometric nickel oxide nanocrystals (NiOx NCs) have been extensively studied as a low-cost and effective HTM in perovskite optoelectronics. In this minireview, we summarize the synthesis and surface-functionalization methods of NiOx NCs. Then, the applications of NiOx NCs in other perovskite optoelectronics beyond photovoltaics are discussed. Finally, we provide a perspective for the future development of NiOx NCs for the commercialization of perovskite optoelectronics. 相似文献
92.
Zuhao You Yanan Song Wenxu Liu Wenlong Wang Chenghao Zhu Yuxin Duan Yao Liu 《Angewandte Chemie (International ed. in English)》2023,62(23):e202302538
Electroactive ionenes combining caged-shaped diazabicyclic cations and aromatic diimides were developed as interlayers in organic solar cells (OSCs). These ionenes reduce the work-function of air-stable metal electrodes (e.g., Ag, Cu and Au) by generating strong interfacial dipoles, and their optoelectronic and morphological characters can be modulated by aromatic diimides, leading to high conductivity and good compatibility with active layers. The optimal ionene exhibits superior charge-transport, desirable crystallinity, and weak visible-absorption, boosting the efficiency of benchmark PM6 : Y6-based OSCs up to 17.44 %. The corresponding normal devices show excellent stability at maximum power point test under one sun illumination for 1000 h. Replacing Y6 with L8-BO promotes the efficiency to 18.43 %, one of the highest in binary OSCs. Notably, high efficiencies >16 % are maintained as the interlayer thickness increasing to 105 nm, the best result with interlayer-thickness over 100 nm. 相似文献
93.
Ye Qian Mi Wei Deng Chaohui He Prof. Dr. Osman Eksik Yi Ping Zheng De Kun Yao Dr. Xian Bin Liu Yan Hong Yin Ye Sheng Li Prof. Dr. Bao Yu Xia Prof. Dr. Zi Ping Wu 《Angewandte Chemie (International ed. in English)》2023,62(12):e202218621
Solid-state lithium batteries are promising and safe energy storage devices for mobile electronics and electric vehicles. In this work, we report a facile in situ polymerization of 1,3-dioxolane electrolytes to fabricate integrated solid-state lithium batteries. The in situ polymerization and formation of solid-state dioxolane electrolytes on interconnected carbon nanotubes (CNTs) and active materials is the key to realizing a high-performance battery with excellent interfacial contact among CNTs, active materials and electrolytes. Therefore, the electrodes could be tightly integrated into batteries through the CNTs and electrolyte. Electrons/ions enable full access to active materials in the whole electrode. Electrodes with a low resistance of 4.5 Ω □−1 and high lithium-ion diffusion efficiency of 2.5×10−11 cm2 s−1 can significantly improve the electrochemical kinetics. Subsequently, the batteries demonstrated high energy density, amazing charge/discharge rate and long cycle life. 相似文献
94.
Sai S. Patkar Yao Tang Arriana M. Bisram Tianren Zhang Jeffery G. Saven Darrin J. Pochan Kristi L. Kiick 《Angewandte Chemie (International ed. in English)》2023,62(25):e202301331
Thermoresponsive resilin-like polypeptides (RLPs) of various lengths were genetically fused to two different computationally designed coiled coil-forming peptides with distinct thermal stability, to develop new strategies to assemble coiled coil peptides via temperature-triggered phase separation of the RLP units. Their successful production in bacterial expression hosts was verified via gel electrophoresis, mass spectrometry, and amino acid analysis. Circular dichroism (CD) spectroscopy, ultraviolet-visible (UV/Vis) turbidimetry, and dynamic light scattering (DLS) measurements confirmed the stability of the coiled coils and showed that the thermosensitive phase behavior of the RLPs was preserved in the genetically fused hybrid polypeptides. Cryogenic-transmission electron microscopy and coarse-grained modeling revealed that functionalizing the coiled coils with thermoresponsive RLPs leads to their thermally triggered noncovalent assembly into nanofibrillar assemblies. 相似文献
95.
Dr. Zixuan Xu Zhaoyu Wang Dr. Wei Yao Yanhua Gao Yuxin Li Dr. Huifang Shi Prof. Wei Huang Prof. Zhongfu An 《Angewandte Chemie (International ed. in English)》2023,62(24):e202301564
Dynamic room temperature phosphorescence (RTP) materials have potential applications in optoelectronics, which inevitably suffer from poor processability, flexibility or stretchability. Herein, we report a concise strategy to develop supercooled liquids (SCLs) with dynamic RTP behavior using terminal hydroxyl engineering. The terminal hydroxyls effectively hinder the nucleation process of molecules for the formation of stable SCLs after thermal annealing. Impressively, the SCLs show reversible RTP emission via alternant stimulation by UV light and heat. Photoactivated SCLs have phosphorescent efficiency of 8.50 % and a lifetime of 31.54 ms under ambient conditions. Regarding the dynamic RTP behavior and stretchability of SCLs, we demonstrate the applications in erasable data encryption and patterns on flexible substrates. This finding provides a design principle for obtaining SCLs with RTP and expands the potential applications of RTP materials in flexible optoelectronics. 相似文献
96.
Zhiguo Sun Huijuan Zhang Linlin Cao Xiaokang Liu Dan Wu Xinyi Shen Xue Zhang Zihang Chen Sen Ru Xiangyu Zhu Zhiyuan Xia Qiquan Luo Faqiang Xu Prof. Tao Yao 《Angewandte Chemie (International ed. in English)》2023,62(13):e202217719
The construction and understanding of synergy in well-defined dual-atom active sites is an available avenue to promote multistep tandem catalytic reactions. Herein, we construct a dual-hetero-atom catalyst that comprises adjacent Cu-N4 and Se-C3 active sites for efficient oxygen reduction reaction (ORR) activity. Operando X-ray absorption spectroscopy coupled with theoretical calculations provide in-depth insights into this dual-atom synergy mechanism for ORR under realistic device operation conditions. The heteroatom Se modulator can efficiently polarize the charge distribution around symmetrical Cu-N4 moieties, and serve as synergistic site to facilitate the second oxygen reduction step simultaneously, in which the key OOH*-(Cu1-N4) transforms to O*-(Se1-C2) intermediate on the dual-atom sites. Therefore, this designed catalyst achieves satisfied alkaline ORR activity with a half-wave potential of 0.905 V vs. RHE and a maximum power density of 206.5 mW cm−2 in Zn-air battery. 相似文献
97.
Xiaotong Li Prof. Yuan Yao Chenxi Liu Xin Jia Jiahuang Jian Bao Guo Prof. Songtao Lu Prof. Wei Qin Prof. Qing Wang Prof. Xiaohong Wu 《Angewandte Chemie (International ed. in English)》2023,62(25):e202304667
Aqueous redox flow batteries (ARFBs) are a promising technology for grid-scale energy storage, however, their commercial success relies on redox-active materials (RAM) with high electron storage capacity and cost competitiveness. Herein, a redox-active material lithium ferrocyanide (Li4[Fe(CN)6]) is designed. Li+ ions not only greatly boost the solubility of [Fe(CN)6]4− to 2.32 M at room temperature due to weak intermolecular interactions, but also improves the electrochemical performance of [Fe(CN)6]4−/3−. By coupling with Zn, ZIRFBs were built, and the capacity of the batteries was as high as 61.64 Ah L−1 (pH-neutral) and 56.28 Ah L−1 (alkaline) at a [Fe(CN)6]4− concentration of 2.30 M and 2.10 M. These represent unprecedentedly high [Fe(CN)6]4− concentrations and battery energy densities reported to date. Moreover, benefiting from the low cost of Li4[Fe(CN)6], the overall chemical cost of alkaline ZIRFB is as low as $11 per kWh, which is one-twentieth that of the state-of-the-art VFB ($211.54 per kWh). This work breaks through the limitations of traditional electrolyte composition optimization and will strongly promote the development of economical [Fe(CN)6]4−/3−-based RFBs in the future. 相似文献
98.
Guangyue Xu Xiang Zhang Zhuoya Dong Wanying Liang Tianci Xiao Huiyong Chen Yanhang Ma Yang Pan Yao Fu 《Angewandte Chemie (International ed. in English)》2023,62(44):e202305915
Non-oxidative dehydrogenation of propane is a highly efficient approach for industrial preparation of propene that is commonly catalyzed by noble Pt or toxic Cr catalysts and suffers from coking. In this work, ferric catalyst confined in a zeolite framework was synthesized by a hydrothermal procedure. The isolated Fe in the framework formed distorted tetrahedra, which were beneficial for the selective dehydrogenation of propane and reached over 95 % propene selectivity and over 99 % total olefins selectivity. This catalyst had a silanol-free structure and was oxygen tolerant, hydrothermally stable, and coke free, with a deactivation constant of 0.01 h−1. This study provided guidance for the synthesis of structural heteroatomic zeolite and efficient propane non-oxidative dehydrogenation over early transition metals. 相似文献
99.
Qiuyu Li Yunchu Zhang Pengyun Liu Jing Zhong Baihui Gong Prof. Dr. Hequan Yao Prof. Dr. Aijun Lin 《Angewandte Chemie (International ed. in English)》2023,62(4):e202211988
We herein disclose a mild and efficient access to chiral 3-azabicyclo[3.1.0]hexanes via a Pd-catalyzed asymmetric 5-exo-trig cyclization/cyclopropanation/carbonylation of 1,6-enynes. Various nucleophiles, such as alcohols, phenols, amines and water, are well compatible with the reaction system. This reaction forms three C−C bonds, two rings, two adjacent quaternary carbon stereocenters as well as one C−O/C−N bond with excellent regio- and enantioselectivities. The products could be further functionalized to generate a library of 3-azabicyclo[3.1.0]hexane frameworks. 相似文献
100.
Yao Wu Cong Zhao Yanzhuang Su Prof. Dr. Sason Shaik Prof. Dr. Wenzhen Lai 《Angewandte Chemie (International ed. in English)》2023,62(7):e202212053
The copper-dependent formylglycine-generating enzyme (FGE) catalyzes the oxygen-dependent oxidation of specific peptidyl-cysteine residues to formylglycine. Our QM/MM calculations provide a very likely mechanism for this transformation. The reaction starts with dioxygen binding to the tris-thiolate CuI center to form a triplet CuII-superoxide complex. The rate-determining hydrogen atom abstraction involves a triplet-singlet crossing to form a CuII−OOH species that couples with the substrate radical, leading to a CuI-alkylperoxo intermediate. This is accompanied by proton transfer from the hydroperoxide to the S atom of the substrate via a nearby water molecule. The subsequent O−O bond cleavage is coupled with the C−S bond breaking that generates the formylglycine and a CuII-oxyl complex. Moreover, our results suggest that the aldehyde oxygen of the final product originates from O2, which will be useful for future experimental work. 相似文献