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101.
Correlating EPR and X-ray structural analysis of arsenite-inhibited forms of aldehyde oxidoreductase
Anders Thapper D. R. Boer Carlos D. Brondino José J. G. Moura Maria J. Romão 《Journal of biological inorganic chemistry》2007,12(3):353-366
Two arsenite-inhibited forms of each of the aldehyde oxidoreductases from Desulfovibrio gigas and Desulfovibrio desulfuricans have been studied by X-ray crystallography and electron paramagnetic resonance (EPR) spectroscopy. The molybdenum site of
these enzymes shows a distorted square-pyramidal geometry in which two ligands, a hydroxyl/water molecule (the catalytic labile
site) and a sulfido ligand, have been shown to be essential for catalysis. Arsenite addition to active as-prepared enzyme
or to a reduced desulfo form yields two different species called A and B, respectively, which show different Mo(V) EPR signals.
Both EPR signals show strong hyperfine and quadrupolar couplings with an arsenic nucleus, which suggests that arsenic interacts
with molybdenum through an equatorial ligand. X-ray data of single crystals prepared from EPR-active samples show in both
inhibited forms that the arsenic atom interacts with the molybdenum ion through an oxygen atom at the catalytic labile site
and that the sulfido ligand is no longer present. EPR and X-ray data indicate that the main difference between both species
is an equatorial ligand to molybdenum which was determined to be an oxo ligand in species A and a hydroxyl/water ligand in
species B. The conclusion that the sulfido ligand is not essential to determine the EPR properties in both Mo–As complexes
is achieved through EPR measurements on a substantial number of randomly oriented chemically reduced crystals immediately
followed by X-ray studies on one of those crystals. EPR saturation studies show that the electron transfer pathway, which
is essential for catalysis, is not modified upon inhibition.
Electronic supplementary material Supplementary material is available in the online version of this article at and is accessible for authorized users. 相似文献
102.
Biomass and population structure of Constrictotermes cyphergaster (Silvestri) were studied in an area of dry forest of caatinga in the State of Paraiba, northeastern Brazil. Twelve nests of different sizes were randomly collected, being six during the dry season (November 2004 and 2005) and six during the wet season (March 2004). Soldier and worker populations varied between 4880 and 118800 individuals per nest. The ratio between soldiers and workers did not significantly vary between seasons. Biomass (measured as fresh weight) of individuals varied between 13.9 and 408.8 g per nest, and soldiers and workers had significantly greater biomass during the wet season. The estimated density of nests of C. cyphergaster was 59.0 +/- 22.53 active nests/ha. Quantitative data of the study colonies and data on the nest abundance showed that C. cyphergaster encompassed some 278.2 individuals/m(2), with approximately 0.9 g (fresh weight)/m(2). These data suggest that C. cyphergaster is an important consumer of vegetal matter and, therefore, an important species affecting the nutrient cycling and energy flow in the caatinga vegetation. 相似文献
103.
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105.
Sinara Santos Jardim André Passaglia Schuch Camila Moura Pereira Elgion Lucio Silva Loreto 《Cell stress & chaperones》2015,20(5):843-851
There are many complex interactions between transposable elements (TEs) and host genomes. Environmental changes that induce stressful conditions help to contribute for increasing complexity of these interactions. The transposon mariner-Mos1 increases its mobilization under mild heat stress. It has putative heat shock elements (HSEs), which are probably activated by heat shock factors (HSFs). Ultraviolet radiation (UVC) is a stressor that has been suggested as able to activate heat shock protein genes (Hsp). In this study, we test the hypothesis that if UVC induces Hsp expression, as heat does, it could also promote mariner-Mos1 transposition and mobilization. The Drosophila simulans white-peach is a mutant lineage that indicates the mariner-Mos1 transposition phenotypically through the formation of mosaic eyes. This lineage was exposed to UVC or mild heat stress (28 °C) in order to evaluate the induction of mariner-Mos1 expression by RT-qPCR, as well as the mariner-Mos1 mobilization activity based on the count number of red spots in the eyes. The effects of both treatments on the developmental time of flies and cell cycle progression were also investigated. Both the analysis of eyes and mariner-Mos1 gene expression indicate that UVC radiation has no effect in mariner-Mos1 transposition, although heat increases the expression and mobilization of this TE soon after the treatment. However, the expression of Hsp70 gene increased after 24 h of UVC exposure, suggesting different pathway of activation. These results showed that heat promotes mariner-Mos1 mobilization, although UVC does not induce the expression or mobilization of this TE.
Electronic supplementary material
The online version of this article (doi:10.1007/s12192-015-0611-2) contains supplementary material, which is available to authorized users. 相似文献106.
107.
Cristiano S. Moura Michal Abrahamowicz Marie-Eve Beauchamp Diane Lacaille Yishu Wang Gilles Boire Paul R. Fortin Louis Bessette Claire Bombardier Jessica Widdifield John G. Hanly Debbie Feldman Walter Maksymowych Christine Peschken Cheryl Barnabe Steve Edworthy Sasha Bernatsky CAN-AIM 《Arthritis research & therapy》2015,17(1)
IntroductionUse of disease-modifying anti-rheumatic drugs (DMARDs) in rheumatoid arthritis (RA) may prevent joint damage and potentially reduce joint replacement surgeries. We assessed the association between RA drug use and joint replacement in Quebec, Canada.MethodsA cohort of new-onset RA patients was identified from Quebec’s physician billing and hospitalization databases from 2002–2011. The outcome was defined using procedure codes submitted by orthopedic surgeons. Medication use was obtained from pharmacy databases. We used alternative Cox regression models with time-dependent variables measuring the cumulative effects of past use during different time windows (one model focussing on the first year after cohort entry) for methotrexate (MTX), and other DMARDs. Models were adjusted for baseline sociodemographics, co-morbidity and prior health service use, time-dependent cumulative use of other drugs (anti-tumor necrosis factor [anti-TNF] agents, other biologics, cyclooxygenase-2 inhibitors [COXIBs], nonselective nonsteroidal antiinflammatory drugs [NSAIDs], and systemic steroids), and markers of disease severity.ResultsDuring follow-up, 608 joint replacements occurred among 11,333 patients (median follow-up: 4.6 years). The best-fitting model relied on the cumulative early use (within the first year after cohort entry) of MTX and of other DMARDs, with an interaction between MTX and other DMARDs. In this model, greater exposure within the first year, to either MTX (adjusted hazard ratio, HR = 0.95 per 1 month, 95 % confidence interval, 95 % CI 0.93-0.97) or other DMARDs (HR = 0.97, 95 % CI 0.95-0.99) was associated with longer time to joint replacement.ConclusionsOur results suggest that longer exposure to either methotrexate (MTX) or other DMARDs within the first year after RA diagnosis is associated with longer time to joint replacement surgery.
Electronic supplementary material
The online version of this article (doi:10.1186/s13075-015-0713-3) contains supplementary material, which is available to authorized users. 相似文献108.
Simone Dell’Acqua Sofia R. Pauleta Isabel Moura José J. G. Moura 《Journal of biological inorganic chemistry》2011,16(2):183-194
This review focuses on the novel CuZ center of nitrous oxide reductase, an important enzyme owing to the environmental significance
of the reaction it catalyzes, reduction of nitrous oxide, and the unusual nature of its catalytic center, named CuZ. The structure
of the CuZ center, the unique tetranuclear copper center found in this enzyme, opened a novel area of research in metallobiochemistry.
In the last decade, there has been progress in defining the structure of the CuZ center, characterizing the mechanism of nitrous
oxide reduction, and identifying intermediates of this reaction. In addition, the determination of the structure of the CuZ
center allowed a structural interpretation of the spectroscopic data, which was supported by theoretical calculations. The
current knowledge of the structure, function, and spectroscopic characterization of the CuZ center is described here. We would
like to stress that although many questions have been answered, the CuZ center remains a scientific challenge, with many hypotheses
still being formed. 相似文献
109.
Patrícia M. Paes de Sousa Sofia R. Pauleta M. Lurdes Simões Gonçalves Graham W. Pettigrew Isabel Moura José J. G. Moura Margarida M. Correia dos Santos 《Journal of biological inorganic chemistry》2011,16(2):209-215
In this work it is demonstrated that the characterization of c-type haem containing proteins by electrochemical techniques needs to be cautiously performed when using pyrolytic graphite
electrodes. An altered form of the cytochromes, which has a redox potential 300 mV lower than that of the native state and
displays peroxidatic activity, can be induced by interaction with the pyrolytic graphite electrode. Proper control experiments
need to be performed, as altered conformations of the enzymes containing c-type haems can show activity towards the enzyme substrate. The work was focused on the study of the activation mechanism
and catalytic activity of cytochrome c peroxidase from Paracoccus
pantotrophus. The results could only be interpreted with the assignment of the observed non-turnover and catalytic signals to a non-native
conformation state of the electron-transferring haem. The same phenomenon was detected for Met–His monohaem cytochromes (mitochondrial
cytochrome c and Desulfovibrio
vulgaris cytochrome c-553), as well as for the bis-His multihaem cytochrome c
3 from Desulfovibrio
gigas, showing that this effect is independent of the axial coordination of the c-type haem protein. Thus, the interpretation of electrochemical signals of c-type (multi)haem proteins at pyrolytic graphite electrodes must be carefully performed, to avoid misassignment of the signals
and incorrect interpretation of catalytic intermediates. 相似文献
110.
Cristiano S. Mota Maria G. Rivas Carlos D. Brondino Isabel Moura José J. G. Moura Pablo J. González Nuno M. F. S. A. Cerqueira 《Journal of biological inorganic chemistry》2011,16(8):1255-1268
Metal-dependent formate dehydrogenases (Fdh) from prokaryotic organisms are members of the dimethyl sulfoxide reductase family
of mononuclear molybdenum-containing and tungsten-containing enzymes. Fdhs catalyze the oxidation of the formate anion to
carbon dioxide in a redox reaction that involves the transfer of two electrons from the substrate to the active site. The
active site in the oxidized state comprises a hexacoordinated molybdenum or tungsten ion in a distorted trigonal prismatic
geometry. Using this structural model, we calculated the catalytic mechanism of Fdh through density functional theory tools.
The simulated mechanism was correlated with the experimental kinetic properties of three different Fdhs isolated from three
different Desulfovibrio species. Our studies indicate that the C–H bond break is an event involved in the rate-limiting step of the catalytic cycle.
The role in catalysis of conserved amino acid residues involved in metal coordination and near the metal active site is discussed
on the basis of experimental and theoretical results. 相似文献