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991.
Prof. Xiaona Li Yang Xu Prof. Changtai Zhao Duojie Wu Dr. Limin Wang Matthew Zheng Xu Han Dr. Simeng Zhang Junyi Yue Prof. Biwei Xiao Dr. Wei Xiao Dr. Ligen Wang Prof. Tao Mei Prof. Meng Gu Prof. Jianwen Liang Prof. Xueliang Sun 《Angewandte Chemie (International ed. in English)》2023,62(48):e202306433
As exciting candidates for next-generation energy storage, all-solid-state lithium batteries (ASSLBs) are highly dependent on advanced solid-state electrolytes (SSEs). Here, using cost-effective LaCl3 and CeCl3 lattice (UCl3-type structure) as the host and further combined with a multiple-cation mixed strategy, we report a series of UCl3-type SSEs with high room-temperature ionic conductivities over 10−3 S cm−1 and good compatibility with high-voltage oxide cathodes. The intrinsic large-size hexagonal one-dimensional channels and highly disordered amorphous phase induced by multi-metal cation species are believed to trigger fast multiple ionic conductions of Li+, Na+, K+, Cu+, and Ag+. The UCl3-type SSEs enable a stable prototype ASSLB capable of over 3000 cycles and high reversibility at −30 °C. Further exploration of the brand-new multiple-cation mixed chlorides is likely to lead to the development of advanced halide SSEs suitable for ASSLBs with high energy density. 相似文献
992.
Jiahui Zeng Yu Fu Yue Wu Shanshan Wang Wenxiang Zhang Prof. Heping Ma 《Angewandte Chemie (International ed. in English)》2023,62(42):e202310235
Xe is an ideal anesthetic gas, but it has not been widely used in practice due to its high cost and low output. Closed-circuit Xe recovery and recycling is an economically viable method to ensure adequate supply in medical use. Herein, we design an innovative way to recover Xe by using a stable fluorinated metal-organic framework (MOF) NbOFFIVE-1-Ni to eliminate CO2 from moist exhaled anesthetic gases. Unlike other Xe recovery MOFs with low Xe/CO2 selectivity (less than 10), NbOFFIVE-1-Ni could achieve absolute molecular sieve separation of CO2/Xe with excellent CO2 selectivity (825). Mixed-gas breakthrough experiments assert the potential of NbOFFIVE-1-Ni as a molecular sieve adsorbent for the effective and energy-efficient removal of carbon dioxide with 99.16 % Xe recovery. Absolute CO2/Xe separation in NbOFFIVE-1-Ni makes closed-circuit Xe recovery and recycling can be easily realized, demonstrating the potential of NbOFFIVE-1-Ni for important anesthetic gas regeneration under ambient conditions. 相似文献
993.
Tiantian Wu Hong Wang Run Tian Shuang Guo Yuhui Liao Prof. Jianbing Liu Prof. Baoquan Ding 《Angewandte Chemie (International ed. in English)》2023,62(46):e202311698
Bacteria infection is a significant obstacle in the clinical treatment of exposed wounds facing widespread pathogens. Herein, we report a DNA origami-based bactericide for efficient anti-infection therapy of infected wounds in vivo. In our design, abundant DNAzymes (G4/hemin) can be precisely organized on the DNA origami for controllable generation of reactive oxygen species (ROS) to break bacterial membranes. After the destruction of the membrane, broad-spectrum antibiotic levofloxacin (LEV, loaded in the DNA origami through interaction with DNA duplex) can be easily delivered into the bacteria for successful sterilization. With the incorporation of DNA aptamer targeting bacterial peptidoglycan, the DNA origami-based bactericide can achieve targeted and combined antibacterial therapy for efficiently promoting the healing of infected wounds. This tailored DNA origami-based nanoplatform provides a new strategy for the treatment of infectious diseases in vivo. 相似文献
994.
Zhicheng Bao Meirong Huang Prof. Dr. Yan Xu Prof. Dr. Xinhao Zhang Prof. Dr. Yun-Dong Wu Prof. Dr. Jianbo Wang 《Angewandte Chemie (International ed. in English)》2023,62(9):e202216356
Bisborylalkanes play important roles in organic synthesis as versatile bifunctional reagents. The two boron moieties in these compounds can be selectively converted into other functional groups through cross-coupling, oxidation or radical reactions. Thus, the development of efficient methods for synthesizing bisborylalkanes is highly demanded. Herein we report a new strategy to access bisborylalkanes through the reaction of N-trisylhydrazones with diboronate, in which the bis(boryl) methane is transformed into 1,2-bis(boronates) via formal carbene insertion. Since the N-trisylhydrazones can be readily derived from the corresponding aldehydes, this strategy represents a practical synthesis of 1,2-diboronates with broad substrate scope. Mechanistic studies reveal an unusual neighboring group effect of 1,1-bis(boronates), which accounts for the observed regioselectivity when unsymmetric 1,1-diboronates are applied. 相似文献
995.
Yunchuan Pu Mingang Zhao Xu Liang Shaoyu Wang Dr. Hongjian Wang Ziting Zhu Dr. Yanxiong Ren Zhiming Zhang Prof. Guangwei He Prof. Dan Zhao Prof. Zhongyi Jiang 《Angewandte Chemie (International ed. in English)》2023,62(22):e202302355
We report a covalent organic framework (COF) induced seeding strategy to fabricate metal–organic framework (MOF) membranes. Contrary to graphene oxide nuclei-depositing substrate, COF substrate has uniform pore size, high microporosity and abundant functional groups. We designed a series of charged COF nanosheets to induce the formation of ZIF-8@COF nanosheet seeds with high aspect ratio over 150, which were readily processed into a compact and uniform seed layer. The resulting ZIF-8 membranes with thickness down to 100 nm exhibit an ultrahigh C3H6/C3H8 separation performance and superior long-term stability. Our strategy is also validated by fabricating ultrathin ZIF-67 and UiO-66 membranes. 相似文献
996.
Yao Qian Dr. Xiangyu Guo Prof. Yunfang Wang Prof. Zheng Ouyang Prof. Xiaoxiao Ma 《Angewandte Chemie (International ed. in English)》2023,62(52):e202312275
Spatial lipidomics based on mass spectrometry imaging (MSI) is a powerful tool for fundamental biology studies and biomarker discovery. But the structure-resolving capability of MSI is limited because of the lack of multiplexed tandem mass spectrometry (MS/MS) method, primarily due to the small sample amount available from each pixel and the poor ion usage in MS/MS analysis. Here, we report a mobility-modulated sequential dissociation (MMSD) strategy for multiplex MS/MS imaging of distinct lipids from biological tissues. With ion mobility-enabled data-independent acquisition and automated spectrum deconvolution, MS/MS spectra of a large number of lipid species from each tissue pixel are acquired, at no expense of imaging speed. MMSD imaging is highlighted by MS/MS imaging of 24 structurally distinct lipids in the mouse brain and the revealing of the correlation of a structurally distinct phosphatidylethanolamine isomer (PE 18 : 1_18 : 1) from a human hepatocellular carcinoma (HCC) tissue. Mapping of structurally distinct lipid isomers is now enabled and spatial lipidomics becomes feasible for MSI. 相似文献
997.
Dr. Jiakang Tang Dr. Ji Liu Dr. Qizhen Zheng Rui Yao Prof. Dr. Ming Wang 《Angewandte Chemie (International ed. in English)》2023,62(48):e202312784
Mitochondria-targeted bioorthogonal catalysis holds promise for controlling cell function precisely, yet achieving selective and efficient chemical reactions within organelles is challenging. In this study, we introduce a new strategy using protein-integrated hydrogen-bonded organic frameworks (HOFs) to enable synergistic bioorthogonal chemical catalysis and enzymatic catalysis within mitochondria. Utilizing catalytically active tris(4,4′-dicarboxylicacid-2,2′-bipyridyl) ruthenium(II) to self-assemble with [1,1′-biphenyl]-4,4′-biscarboximidamide, we synthesized nanoscale RuB-HOFs that exhibit high photocatalytic reduction activity. Notably, RuB-HOFs efficiently enter cells and preferentially localize to mitochondria, where they facilitate bioorthogonal photoreduction reactions. Moreover, we show that RuB-HOFs encapsulating catalase can produce hydrogen sulfide (H2S) in mitochondria through photocatalytic reduction of pro-H2S and degrade hydrogen peroxide through enzymatic catalysis simultaneously, offering a significant neuroprotective effect against oxidative stress. Our findings not only introduce a versatile chemical toolset for mitochondria-targeted bioorthogonal catalysis for prodrug activation but also pave the way for potential therapeutic applications in treating diseases related to cellular oxidative stress. 相似文献
998.
Guopeng Du Pingliang Zhu Jing Wang Xinjin Li Dao-Peng Zhang Chuan-Zeng Wang Prof. Dr. Feng-Gang Sun 《European journal of organic chemistry》2023,26(6):e202201382
Herein, we report a palladium/norbornene/copper co-catalyzed single-step approach that merges selective ortho C−H bond esterification with ipso thiolation for construction of synthetically versatile 2-arylthio aryl esters under exceptionally mild conditions. Importantly, this process proceeded in a highly efficient manner, allowing alkoxycarbonyl and thio groups to be installed into one aryl iodides simultaneously by harnessing thiocarbonate as bifunctional reagent. The method has been demonstrated to accommodate good functionalities and features broad substrate scope. 相似文献
999.
Meiyun Su Lina Guo Peiyu Mao Meng Xiao Prof. Dr. Wenjie Liu Prof. Dr. Shaohua Wang 《European journal of organic chemistry》2023,26(29):e202300268
The catalyst-free electrochemical halogenation and trifluoromethylation of 4H-pyrido[1,2-a]pyrimidin-4-ones was realized under external-oxidant-free conditions. This strategy provides an easy and green access to functionalized new 4H-pyrido[1,2-a]pyrimidin-4-one derivatives with broad scope, good functional group tolerance and high regioselectivity. 相似文献
1000.
Jing-Xiang Wang Dr. Avery C. Vilbert Dr. Chang Cui Dr. Evan N. Mirts Lucas H. Williams Wantae Kim Prof. Dr. Y. Jessie Zhang Prof. Dr. Yi Lu 《Angewandte Chemie (International ed. in English)》2023,62(52):e202314019
The key to type 1 copper (T1Cu) function lies in the fine tuning of the CuII/I reduction potential (E°′T1Cu) to match those of its redox partners, enabling efficient electron transfer in a wide range of biological systems. While the secondary coordination sphere (SCS) effects have been used to tune E°′T1Cu in azurin over a wide range, these principles are yet to be generalized to other T1Cu-containing proteins to tune catalytic properties. To this end, we have examined the effects of Y229F, V290N and S292F mutations around the T1Cu of small laccase (SLAC) from Streptomyces coelicolor to match the high E°′T1Cu of fungal laccases. Using ultraviolet-visible absorption and electron paramagnetic resonance spectroscopies, together with X-ray crystallography and redox titrations, we have probed the influence of SCS mutations on the T1Cu and corresponding E°′T1Cu. While minimal and small E°′T1Cu increases are observed in Y229F- and S292F-SLAC, the V290N mutant exhibits a major E°′T1Cu increase. Moreover, the influence of these mutations on E°′T1Cu is additive, culminating in a triple mutant Y229F/V290N/S292F-SLAC with the highest E°′T1Cu of 556 mV vs. SHE reported to date. Further activity assays indicate that all mutants retain oxygen reduction reaction activity, and display improved catalytic efficiencies (kcat/KM) relative to WT-SLAC. 相似文献