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31.
Takayuki Komatsu Kazuya Aida Tuyoshi Honma Yasuhiko Benino Ryuji Sato 《Journal of the American Ceramic Society》2002,85(1):193-199
The structural relaxation kinetics at the glass transition in tellurium oxide (TeO2 )-based glasses has been examined from viscosity and heat-capacity measurements to clarify the features of the structural relaxation in fragile oxide glass-forming liquids. A large decoupling between enthalpy relaxation and viscous flow, i.e., a large discrepancy between the activation energies for the enthalpy relaxation (recovery), Δ H , and viscous flow, E η , has been demonstrated in TeO2 -based glasses. The values in x K2 O· x MgO·(100 − 2 x )TeO2 glasses, for example, are ∼919–1051 kJ/mol for Δ H and ∼ 577–701 kJ/mol for E η , given the ratio of Δ H/E η ≈ 1.44–1.59. Some viscosity and heat-capacity data (all data have been reported previously) obtained from similar experiments in Sb2 O3 –B2 O3 glasses belonging to the category of strong glass-forming liquids have been reanalyzed in this paper for comparison; a strong coupling was found to exist between Δ H and E η , i.e., Δ H/E η ≈ 0.98–1.18. An origin of decoupling between Δ H and E η in fragile glass-forming systems such as TeO2 -based glasses has been discussed by considering the glass structure model for fragile glasses; strongly bonded correlated (highly constrained) regions are surrounded or connected by weakly bonded noncorrelated (unconstrained) parts. 相似文献
32.
Seiji Inaba Yasuhiko Benino Shinji Kohara Hideo Hosono Setsuro Ito 《Journal of the American Ceramic Society》2020,103(6):3631-3641
Orientation anisotropy, which is well known in organic polymers with appropriate network structures, is less common in oxide glasses. We present the intermediate-range order in anisotropic alkali metaphosphate glass which consists of oriented PO4 tetrahedral chains and intervening alkali cations along the elongation direction. The X-ray total structure factor S(Q) indicates that the inter-chain spacing depends on the size of alkali cations and varies from 5.03 to 6.28 Å. The mixed alkali effect is primarily related to an increase of the separation. The total correlation function T(r) provides the first definite evidence that the anisotropic structure is composed of phosphorus-bridging oxygen bonds (P–OB) lying along the elongation direction and phosphorus-non-bridging oxygen bonds (P–OT) oriented perpendicular to the elongation direction. The present result unveils fundamental aspects of the anisotropic structure of an oxide glass and provides essential information for the development of oxide glasses to control structural anisotropy. 相似文献
33.
Hiromasa Yagyu Yoshikazu Hirai Akio Uesugi Yoshihide Makino Koji Sugano Toshiyuki Tsuchiya Osamu Tabata 《Polymer》2012,53(21):4834-4842
The mechanical properties of an epoxy-based chemically amplified resists with various cross-linking ratios were simulated using a newly developed coarse-grained molecular dynamics simulation that employs a bead–spring model. Models with the different cross-linking ratios were created in the molecular dynamics calculation step and uniaxial elongation simulations were performed. The results reveal that the simulated elastic modulus of the resist modeled by the Kremer–Grest model with an extended angle bending potential depends on the cross-linking ratio, its dependency exhibits good agreement with that determined by nanoindentation tests. 相似文献
34.
35.
Liposome‐Based in Vitro Evolution of Aminoacyl‐tRNA Synthetase for Enhanced Pyrrolysine Derivative Incorporation 下载免费PDF全文
Dr. Atsuko Uyeda Dr. Takayoshi Watanabe Dr. Yasuhiko Kato Prof. Hajime Watanabe Prof. Tetsuya Yomo Prof. Takahiro Hohsaka Dr. Tomoaki Matsuura 《Chembiochem : a European journal of chemical biology》2015,16(12):1797-1802
Methanosarcina species pyrrolysyl‐tRNA synthetase (PylRS) attaches Pyl to its cognate amber suppressor tRNA. The introduction of two mutations (Y384F and Y306A) into PylRS was previously shown to generate a mutant, designated LysZ‐RS, that was able to attach N‐benzyloxycarbonyl‐L ‐lysine (LysZ) to its cognate tRNA. Despite the potential of LysZ derivatives, further LysZ‐RS engineering has not been performed; consequently, we aimed to generate LysZ‐RS mutants with improved LysZ incorporation activity through in vitro directed evolution. Using a liposome‐based in vitro compartmentalization (IVC) approach, we screened a randomly mutagenized gene library of LysZ‐RS and obtained a mutant that showed increased LysZ incorporation activity both in vitro and in vivo. The ease and high flexibility of liposome‐based IVC should enable the evolution of not only LysZ‐RS that can attach various LysZ derivatives but also of other enzymes involved in protein translation. 相似文献
36.
Takahiro Ohkubo Eiji Tsuchida Kenzo Deguchi Shinobu Ohki Tadashi Shimizu Toshiya Otomo Yasuhiko Iwadate 《Journal of the American Ceramic Society》2018,101(3):1122-1134
It remains a challenge to establish structural models of multicomponent oxide glass systems. In this study, we have investigated 68.3SiO2–16.1B2O3–4.2Al2O3–11.4Na2O glass and melt structures by ab initio molecular dynamics (AIMD) simulations. The atomic configurations obtained from AIMD simulations were validated against 17O solid‐state NMR spectrum under 24.0 T and neutron diffraction data, and excellent agreement was achieved. The bond lengths, angles, and coordination geometries were statistically analyzed for each atomic species. Here we particularly address the role of minor atomic species such as five‐coordinate Si (SiV) and Al (AlV). The SiV–O bond lengths and O–SiV–O angle distribution in the glass indicated 1.718 Å and three peaks at 90°, 120°, and 175°, which are assigned to a coordination geometry of the trigonal bipyramidal structure. Ring statistic analysis revealed that SiV and AlV were found to preferentially contribute to the formation of small ring sizes. 相似文献
37.
Yasuhiko Otsuki Toshihisa Kajiwara Kazumori Funatsu 《Polymer Engineering and Science》1997,37(7):1171-1181
Numerical viscoelastic simulations were carried out using a K-BKZ type of separable integral constitutive equation. Both reversible and irreversible models were tried for several types of damping functions to calculate the annular extrudate behavior of high-density polyethylene (HDPE). There are two aims in this study; first, to clarify the properties of these dumping functions, and second, to investigate the influence of rheological characteristics on annular extrudate swell. In these numerical simulations, relaxation spectrum and shear viscosity were fixed, and the other characteristics were varied. The reversional response of the damping function mainly has an effect on the magnitude of the area swell even if the die is straight. The irreversible model expresses the experimental results of annular extrudate swell better than the reversible model. The accurate fitting of N1 by the damping model is important for predicting it. The magnitude of N1 predicted from the Wagner exponential model is lower than that of the PSM model, and the area swell shows the same tendency as N1. A modified PSM model that allows the N1 curve to shift can fit the magnitude of area swell. The relationship between the diameter and thickness of the extrudate depends on N2/N1, and it was estimated by simple linear elasticity of solids. The time dependent viscosity varies with the type of damping function, and it influences the time-dependent swell. 相似文献
38.
Kazuya Aida Yasuhiko Benino Vesselin Dimitrov Takayuki Komatsu Ryuji Sato 《Journal of the American Ceramic Society》2000,83(5):1192-1198
The kinetics of enthalpy relaxation (recovery) at the glass transition in x K2 O·(20− x )MgO·80TeO2 glasses has been examined from heat capacity measurements using differential scanning calorimetry to clarify the features of the structural relaxation in ternary TeO2 -based glasses. Ternary glasses such as 10K2 O·10MgO·80TeO2 show high thermal resistance against crystallization compared with binary glasses. The degree of fragility m estimated from the activation energy for viscous flow E η and the glass transition temperature T g is m = 55–62, indicating a fragile character in TeO2 -based glasses. Large heat capacity changes of 43.1–48.2 J·mol−1 ·K−1 are also observed at the glass transition. The activation energy for enthalpy relaxation Δ H is evaluated from the cooling rate dependence of the limiting fictive temperature, and values of Δ H = 897–1268 kJ·mol−1 are obtained. Negative deviation from additivity in Δ H is also observed. Values of the Kovacs–Aklonis–Huchinson–Ramos (KAHR) parameter θ estimated from Δ H and T g are 0.33–0.42 K−1 . It has been proposed that ternary glasses have more homogeneous and constrained glass structure compared with binary glasses. 相似文献
39.
Tomoo Yamamura Tomonori Mori Ki Chul Park Yasuhiko Fujii Hiroshi Tomiyasu 《The Journal of Supercritical Fluids》2009,51(1):43-49
Catalytic reduction gasification in the presence of ruthenium(IV) dioxide (RuO2) in supercritical water was used to decompose intractable biomass. The gasification of model biomass samples (glucose, cellulose, and heterocyclic compounds), and low-purity biomass samples obtained from a paper-recycling facility (paper sludge) and from a sewage treatment plant (sewage sludge) were studied. In clear contrast to another catalysts, the RuO2 catalyst completely gasified cellulose to produce mainly hydrogen, methane, and carbon dioxide under various conditions (e.g., 673 K at 30 MPa and 773 K at 50 MPa). As for heterocyclic compounds, nitrogen compounds did not deactivate the RuO2 catalyst; the gasification of carbazole proceeded completely. Furthermore, paper sludge was almost completely decomposed in supercritical water with RuO2 at 723 K. 相似文献
40.
Makoto Miyazawa Yasuhiko Irie Kazuki Kashimoto Naoko Nishina Mitsuru Kondo Sachiko Yasue Kenji Maeda Fumio Uchida 《Inorganic chemistry communications》2009,12(4):336-339
Three new complexes, [Zn(dbsf)2(dmf)2] · 5.5dmf (dbsf = 4,4′-sulfonyldibenzoate) (1β), [Cu(tdsa)(phen)2] · 1.5EtOH (tdsa = 5,5′-thiodisalicylate, phen = 1,10-phenanthroline) (2), and [Cu(sdp)(phen) · Cu(Hsdp)(phen)(CH3COO)] · 3EtOH (sdp = 4,4′-sulfonyldiphenolate) (3) were prepared and structurally characterized. Complex 1β shows a one-dimensional coordination framework constructed from bridges between Zn(II) centers with two ligands. Complex 2 is a monomeric complex, which assembles by π–π interactions. Complex 3 shows a unique two-dimensional coordination framework that is constructed from two Cu(II) centers, sdp, and Hsdp. The redox properties of these three complexes were characterized by solid-state cyclic voltammetry. Complexes 1β and 3 show irreversible reduction waves because of the reduction of their sulfone sites. Complex 2 shows an irreversible oxidation wave because of oxidation of the sulfide site. 相似文献