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101.
Christopher J. Royer Paul D. Cook 《Protein science : a publication of the Protein Society》2019,28(6):1083-1094
Bacillithiol is a glucosamine‐derived antioxidant found in several pathogenic Gram‐positive bacteria. The compound is involved in maintaining the appropriate redox state within the cell as well as detoxifying foreign agents like the antibiotic fosfomycin. Bacillithiol is produced via the action of three enzymes, including BshA, a retaining GT‐B glycosyltransferase that utilizes UDP‐N‐acetylglucosamine and l ‐malate to produce N‐acetylglucosaminyl‐malate. Recent studies suggest that retaining GT‐B glycosyltransferases like BshA utilize a substrate‐assisted mechanism that goes through an SNi‐like transition state. In a previous study, we relied on X‐ray crystallography as well as computational simulations to hypothesize the manner in which substrates would bind the enzyme, but several questions about substrate binding and the role of one of the amino acid residues persisted. Another study demonstrated that BshA might be subject to feedback inhibition by bacillithiol, but this phenomenon was not analyzed further to determine the exact mechanism of inhibition. Here we present X‐ray crystallographic structures and steady‐state kinetics results that help elucidate both of these issues. Our ligand‐bound crystal structures demonstrate that the active site provides an appropriate steric and geometric arrangement of ligands to facilitate the substrate‐assisted mechanism. Finally, we show that bacillithiol is competitive for UDP‐N‐acetylglucosamine with a Ki value near 120–130 μM and likely binds within the BshA active site, suggesting that bacillithiol modulates BshA activity via feedback inhibition. The work presented here furthers our understanding of bacillithiol metabolism and can aid in the development of inhibitors to counteract resistance to antibiotics such as fosfomycin. 相似文献
102.
103.
Susan C. Fitzer Rona A. R. McGill Sergio Torres Gabarda Brian Hughes Michael Dove Wayne O'Connor Maria Byrne 《Global Change Biology》2019,25(12):4105-4115
Commercial shellfish aquaculture is vulnerable to the impacts of ocean acidification driven by increasing carbon dioxide (CO2) absorption by the ocean as well as to coastal acidification driven by land run off and rising sea level. These drivers of environmental acidification have deleterious effects on biomineralization. We investigated shell biomineralization of selectively bred and wild‐type families of the Sydney rock oyster Saccostrea glomerata in a study of oysters being farmed in estuaries at aquaculture leases differing in environmental acidification. The contrasting estuarine pH regimes enabled us to determine the mechanisms of shell growth and the vulnerability of this species to contemporary environmental acidification. Determination of the source of carbon, the mechanism of carbon uptake and use of carbon in biomineral formation are key to understanding the vulnerability of shellfish aquaculture to contemporary and future environmental acidification. We, therefore, characterized the crystallography and carbon uptake in the shells of S. glomerata, resident in habitats subjected to coastal acidification, using high‐resolution electron backscatter diffraction and carbon isotope analyses (as δ13C). We show that oyster families selectively bred for fast growth and families selected for disease resistance can alter their mechanisms of calcite crystal biomineralization, promoting resilience to acidification. The responses of S. glomerata to acidification in their estuarine habitat provide key insights into mechanisms of mollusc shell growth under future climate change conditions. Importantly, we show that selective breeding in oysters is likely to be an important global mitigation strategy for sustainable shellfish aquaculture to withstand future climate‐driven change to habitat acidification. 相似文献
104.
Xiaoxue Lv Tianyu Lei Bojun Wang Wei Chen Yu Jiao Yin Hu Yichao Yan Jianwen Huang Junwei Chu Chaoyi Yan Chunyang Wu Jianwei Wang Xiaobin Niu Jie Xiong 《Liver Transplantation》2019,9(40)
Due to unprecedented features including high‐energy density, low cost, and light weight, lithium–sulfur batteries have been proposed as a promising successor of lithium‐ion batteries. However, unresolved detrimental low Li‐ion transport rates in traditional carbon materials lead to large energy barrier in high sulfur loading batteries, which prevents the lithium–sulfur batteries from commercialization. In this report, to overcome the challenge of increasing both the cycling stability and areal capacity, a metallic oxide composite (NiCo2O4@rGO) is designed to enable a robust separator with low energy barrier for Li‐ion diffusion and simultaneously provide abundant active sites for the catalytic conversion of the polar polysulfides. With a high sulfur‐loading of 6 mg cm?2 and low sulfur/electrolyte ratio of 10, the assembled batteries deliver an initial capacity of 5.04 mAh cm?2 as well as capacity retention of 92% after 400 cycles. The metallic oxide composite NiCo2O4@rGO/PP separator with low Li‐ion diffusion energy barrier opens up the opportunity for lithium–sulfur batteries to achieve long‐cycle, cost‐effective operation toward wide applications in electric vehicles and electronic devices. 相似文献
105.
Quan Liu Johann Toudert Tengfei Li Mariia Kramarenko Guillermo Martínez‐Denegri Laura Ciammaruchi Xiaowei Zhan Jordi Martorell 《Liver Transplantation》2019,9(20)
In the subwavelength regime, several nanophotonic configurations have been proposed to overcome the conventional light trapping or light absorption enhancement limit in solar cells also known as the Yablonovitch limit. It has been recently suggested that establishing such limit should rely on computational inverse electromagnetic design instead of the traditional approach combining intuition and a priori known physical effect. In the present work, by applying an inverse full wave vector electromagnetic computational approach, a 1D nanostructured optical cavity with a new resonance configuration is designed that provides an ultrabroadband (≈450 nm) light absorption enhancement when applied to a 107 nm thick active layer organic solar cell based on a low‐bandgap (1.32 eV) nonfullerene acceptor. It is demonstrated computationally and experimentally that the absorption enhancement provided by such a cavity surpasses the conventional limit resulting from an ergodic optical geometry by a 7% average over a 450 nm band and by more than 20% in the NIR. In such a cavity configuration the solar cells exhibit a maximum power conversion efficiency above 14%, corresponding to the highest ever measured for devices based on the specific nonfullerene acceptor used. 相似文献
106.
Joel Sanchez Thomas R. Hellstern Laurie A. King Thomas F. Jaramillo 《Liver Transplantation》2019,9(40)
In this work, a methodology is demonstrated to engineer gas diffusion electrodes for nonprecious metal catalysts. Highly active transition metal phosphides are prepared on carbon‐based gas diffusion electrodes with low catalyst loadings by modifying the O/C ratio at the surface of the electrode. These nonprecious metal catalysts yield extraordinary performance as measured by low overpotentials (51 mV at ?10 mA cm?2), unprecedented mass activities (>800 A g?1 at 100 mV overpotential), high turnover frequencies (6.96 H2 s?1 at 100 mV overpotential), and high durability for a precious metal‐free catalyst in acidic media. It is found that a high O/C ratio induces a more hydrophilic surface directly impacting the morphology of the CoP catalyst. The improved hydrophilicity, stemming from introduced oxyl groups on the carbon electrode, creates an electrode surface that yields a well‐distributed growth of cobalt electrodeposits and thus a well‐dispersed catalyst layer with high surface area upon phosphidation. This report demonstrates the high‐performance achievable by CoP at low loadings which facilitates further cost reduction, an important part of enabling the large‐scale commercialization of non‐platinum group metal catalysts. The fabrication strategies described herein offer a pathway to lower catalyst loading while achieving high efficiency and promising stability on a 3D electrode. 相似文献
107.
Ziran Zhao Feidan Gu Haixia Rao Senyun Ye Zhiwei Liu Zuqiang Bian Chunhui Huang 《Liver Transplantation》2019,9(3)
Metal halide perovskite solar cells (PSCs) have emerged as promising candidates for photovoltaic technology with their power conversion efficiencies over 23%. For prototypical organic–inorganic metal halide perovskites, their intrinsic instability poses significant challenges to the commercialization of PSCs. Recently, the scientific community has done tremendous work in composition engineering to develop more robust light‐absorbing layers, including mixed‐ion hybrid perovskites, low‐dimensional hybrid perovskites, and all‐inorganic perovskites. This review provides an overview of the impact of these perovskites on the efficiency and long‐term stability of PSCs. 相似文献
108.
Weijun Ke Lingling Mao Constantinos C. Stoumpos Justin Hoffman Ioannis Spanopoulos Aditya D. Mohite Mercouri G. Kanatzidis 《Liver Transplantation》2019,9(10)
Hybrid halide 2D perovskites deserve special attention because they exhibit superior environmental stability compared with their 3D analogs. The closer interlayer distance discovered in 2D Dion–Jacobson (DJ) type of halide perovskites relative to 2D Ruddlesden–Popper (RP) perovskites implies better carrier charge transport and superior performance in solar cells. Here, the structure and properties of 2D DJ perovskites employing 3‐(aminomethyl)piperidinium (3AMP2+) as the spacing cation and a mixture of methylammonium (MA+) and formamidinium (FA+) cations in the perovskite cages are presented. Using single‐crystal X‐ray crystallography, it is found that the mixed‐cation (3AMP)(MA0.75FA0.25)3Pb4I13 perovskite has a narrower bandgap, less distorted inorganic framework, and larger Pb? I? Pb angles than the single‐cation (3AMP)(MA)3Pb4I13. Furthermore, the (3AMP)(MA0.75FA0.25)3Pb4I13 films made by a solvent‐engineering method with a small amount of hydriodic acid have a much better film morphology and crystalline quality and more preferred perpendicular orientation. As a result, the (3AMP)(MA0.75FA0.25)3Pb4I13‐based solar cells exhibit a champion power conversion efficiency of 12.04% with a high fill factor of 81.04% and a 50% average efficiency improvement compared to the pristine (3AMP)(MA)3Pb4I13 cells. Most importantly, the 2D DJ 3AMP‐based perovskite films and devices show better air and light stability than the 2D RP butylammonium‐based perovskites and their 3D analogs. 相似文献
109.
Practical application of hard carbon materials in sodium‐ion batteries (SIBs) is largely limited by their low initial coulombic efficiency (ICE), which may be improved by increasing the graphitization degree. However, biomass‐derived hard carbon is usually nongraphitizable and extremely difficult to graphitize by direct heating even at 3000 °C. Herein, a general strategy is reported for fabricating hard carbon materials with graphite crystals at 1300 °C promoted by external graphite that serves as a crystal template for the growth of graphite crystals. The graphite crystals enable the contacted pseudographitic domains with a high‐level ordered structure, large domain size, and low defects, leading to an enhanced ICE. The obtained hard carbon materials with graphite crystals, using the carbonized eggshell membranes, and sucrose‐derived microsphere as precursors, achieve very high ICE of 89% and 91% with reversible capacity of 310 and 301 mA h g?1, respectively. Therefore, using external graphite to promote high‐level ordering pseudographitic domains at low temperature is quite useful to improve ICE for SIB applications. 相似文献
110.
Parkinson's disease (PD) is a neurodegenerative disorder involving progressive deterioration of dopaminergic neurons. Although few genetic markers for familial PD are known, the etiology of sporadic PD remains poorly understood. Microarray data was analysed for induced pluripotent stem cells (iPSCs) derived from PD patients and mature neuronal cells (mDA) differentiated from these iPSCs. Combining expression and semantic similarity, a highly-correlated PD interactome was constructed that included interactions of established Parkinson's disease marker genes. A novel three-way comparative approach was employed, delineating topologically and functionally important genes. These genes showed involvement in pathways like Parkin-ubiquitin proteosomal system (UPS), immune associated biological processes and apoptosis. Of interest are three genes, eEF1A1, CASK, and PSMD6 that are linked to PARK2 activity in the cell and thereby form attractive candidate genes for understanding PD. Network biology approach delineated in this study can be applied to other neurodegenerative disorders for identification of important genetic regulators. 相似文献