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101.
Catalytic C?H borylation has been reported using newly designed iron complexes bearing a 4,5,6,7‐tetrahydroisoindol‐2‐ide‐based PNP pincer ligand. The reaction tolerated various five‐membered heteroarenes, such as pyrrole derivatives, as well as six‐membered aromatic compounds, such as toluene. Successful examples of the iron‐catalyzed sp3 C?H borylation of anisole derivatives were also presented. 相似文献
102.
Guijun Ma Yohichi Suzuki Rupashree Balia Singh Aki Iwanaga Yosuke Moriya Tsutomu Minegishi Jingyuan Liu Takashi Hisatomi Hiroshi Nishiyama Masao Katayama Kazuhiko Seki Akihiro Furube Taro Yamada Kazunari Domen 《Chemical science》2015,6(8):4513-4518
The particulate semiconductor La5Ti2CuS5O7 (LTC) with a band gap energy of 1.9 eV functioned as either a photocathode or a photoanode when embedded onto Au or Ti metal layers, respectively. By applying an LTC/Au photocathode and LTC/Ti photoanode to, respectively, photoelectrochemical (PEC) water reduction and oxidation concurrently, zero-bias overall water splitting was accomplished under visible light irradiation. The band structures of LTC/Au and LTC/Ti calculated using a semiconductor device simulator (AFORS-HET) confirmed the critical role of the solid/solid junction of the metal back contact in the charge separation and PEC properties of LTC photoelectrodes. The prominently long lifetime of photoexcited charge carriers in LTC, confirmed by transient absorption spectroscopy, allowed the utilization of both photoexcited electrons and holes depending on the band structure at the solid/solid junction. 相似文献
103.
Takumi Nakanishi Yuta Hori Shuqi Wu Hiroyasu Sato Atsushi Okazawa Prof. Norimichi Kojima Yusuke Horie Hajime Okajima Prof. Akira Sakamoto Yoshihito Shiota Prof. Kazunari Yoshizawa Prof. Osamu Sato 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(35):14891-14897
A proton–electron coupling system, exhibiting unique bistability or multistability of the protonated state, is an attractive target for developing new switchable materials based on proton dynamics. Herein, we present an iron(II) hydrazone crystalline compound, which displays the stepwise transition and bistability of proton transfer at the crystal level. These phenomena are realized through the coupling with spin transition. Although the multi-step transition with hysteresis has been observed in various systems, the corresponding behavior of proton transfer has not been reported in crystalline systems; thus, the described iron(II) complex is the first example. Furthermore, because proton transfer occurs only in one of the two ligands and π electrons redistribute in it, the dipole moment of the iron(II) complexes changes with the proton transfer, wherein the total dipole moment in the crystal was canceled out owing to the antiferroelectric-like arrangement. 相似文献
104.
Dr. Takayuki Iwata Mizuki Hyodo Takuto Fukami Prof. Dr. Yoshihito Shiota Prof. Dr. Kazunari Yoshizawa Prof. Dr. Mitsuru Shindo 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(39):8506-8510
We report herein an efficient method to synthesize triptycenes by the reaction of benzynes and anthranoxides, which are electron-rich and readily prepared from the corresponding anthrones. Using this method, 1,9-syn-substituted triptycenes were regioselectively obtained employing 3-methoxybenzynes. This method was also applied to synthesize pentiptycenes. A DFT study revealed that the cycloaddition of lithium anthranoxide and benzyne proceeds stepwise. 相似文献
105.
Yasumasa Nishiwaki Kazunari Masutani Yoshiharu Kimura Chan-Woo Lee 《Journal of polymer science. Part A, Polymer chemistry》2020,58(6):860-871
Bis-hydroxyl-terminated poly(1,2-propylene succinate) (PPS-diols) with high molecular weight (10–40 kDa) are prepared by two-step melt polycondensation of succinic acid and 1,2-propanediol with Ti(BuO)4 as the catalyst. By using these PPS-diols as macroinitiators, the ring-opening polymerization of d - and l -lactides is readily conducted to obtain enantiomeric ABA triblock copolymers consisting of poly(l -lactide) and PPS (B) (t-l -PPS) as well as those of poly(d -lactide) and PPS (B) (t-d -PPS) which have higher PPS compositions (20–70 wt%) in addition to high molecular weight (20–80 kD). The Tg, Tm, and ΔHm values of the t-l -PPS copolymers as well as the stereo mixtures of t-l -PPS/t-d -PPS are controlled to linearly decrease with increasing the PPS content. The copolymers also exhibit higher elastomeric properties with increasing the PPS content. The tensile properties of the copolymer films having higher PPS contents (both the single block copolymers and stereo mixtures) are comparable to those of the oil-based thermoplastic elastomers. It is therefore concluded that these block copolymers can afford thermoplastic elastomers or flexible plastic materials having a 100% biobased content. 相似文献
106.
107.
Osamu Iwanaga Mayuko Miyanishi Toshihiro Tachibana Takaaki Miyazaki Yoshihito Shiota Kazunari Yoshizawa Hiroyuki Furuta 《Molecules (Basel, Switzerland)》2022,27(21)
The factors that affect acceleration and high trans/cis selectivity in the catalytic cyclopropanation reaction of styrene with ethyl diazoacetate by cobalt N-confused porphyrin (NCP) complexes were investigated using density functional theory calculations. The reaction rate was primarily related to the energy gap between the cobalt–carbene adduct intermediates, A and B, which was affected by the NCP skeletons and axial pyridine ligands more than the corresponding porphyrin complex. In addition, high trans/cis stereoselectivity was determined at the TS1 and, in part, in the isomerization process at the carbon-centered radical intermediates, Ctrans and Ccis. 相似文献
108.
Prof. Dr. Kazuyuki Takahashi Kiko Kawamukai Mitsunobu Okai Prof. Dr. Tomoyuki Mochida Dr. Takahiro Sakurai Prof. Dr. Hitoshi Ohta Dr. Takashi Yamamoto Prof. Dr. Yasuaki Einaga Prof. Dr. Yoshihito Shiota Prof. Dr. Kazunari Yoshizawa 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(4):1253-1257
Unprecedented anionic FeIII spin crossover (SCO) complexes involving a weak‐field O,N,O‐tridentate ligand were discovered. The SCO transition was evidenced by the temperature variations in magnetic susceptibility, Mössbauer spectrum, and coordination structure. The DFT calculations suggested that larger coefficients on the azo group in the HOMO?1 of a ligand might contribute to the enhancement of a ligand‐field splitting energy. The present anionic SCO complex also exhibited the light‐ induced excited‐spin‐state trapping effect. 相似文献
109.
Yurina Sekine Kimiko Okazaki Tomoko Ikeda-Fukazawa Masatoshi Ichikawa Kenichi Yoshikawa Sada-atsu Mukai Kazunari Akiyoshi 《Colloid and polymer science》2014,292(2):325-331
The viscoelastic behavior of a cholesterol-modified pullulan (CHP) nanogel at various concentrations was measured using passive particle-tracking microrheology. Microrheology measures stress–strain relationships in small volumes of material by monitoring the response of probes embedded in the medium. Although microrheology is a useful way to overcome sample volume limitations, the application of the method to CHP nanogel systems has not been reported. The viscoelastic spectra of the CHP nanogels obtained from the microrheological measurements were in good agreement with the bulk rheological measurements for each sample, demonstrating that microrheological measurement is effective in CHP nanogel systems. The gelation behavior of CHP nanogel dispersions containing pullulans of different molecular weights was also investigated by microrheology. CHP nanogels made from 1.0 or 4.0?×?105 molecular weight pullulans formed a macrogel at around 3.0 wt%, whereas the CHP nanogel consisting of 0.55?×?105 molecular weight pullulan did not form a macrogel. This suggests that the mechanical properties of the system can be controlled by the molecular weight of the pullulan used. These insights into gelation behavior should be useful in predicting the most favorable conditions for developing novel materials. 相似文献
110.
Nanosize hydrogels (nanogels) are polymer nanoparticles with three‐dimensional networks, formed by chemical and/or physical cross‐linking of polymer chains. Recently, various nanogels have been designed, with a particular focus on biomedical applications. In this review, we describe recent progress in the synthesis of nanogels and nanogel‐integrated hydrogels (nanogel cross‐linked gels) for drug‐delivery systems (DDS), regenerative medicine, and bioimaging. We also discuss chaperone‐like functions of physical cross‐linking nanogel (chaperoning engineering) and organic‐inorganic hybrid nanogels. © 2010 The Japan Chemical Journal Forum and Wiley Periodicals, Inc. Published online in Wiley InterScience ( www.interscience.wiley.com ) DOI 10.1002/tcr.201000008 相似文献