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981.
Praseetha E. Kesavan Vijayalakshmi Pandey Masatoshi Ishida Hiroyuki Furuta Shigeki Mori Iti Gupta 《化学:亚洲杂志》2020,15(13):2015-2028
Beta‐pyrrole‐substituted porphyrin dyads connected by ethynyl linkage to N‐butylcarbazole or triphenylamine donors are reported. Donor‐π‐acceptor type beta‐substituted porphyrin dyads and their Zn(II) and Pd(II) complexes were characterized by MALDI‐MS, NMR, UV‐vis absorption, fluorescence and cyclic voltammetry techniques. The S1 emission dynamics were analyzed by time‐resolved spectroscopy (TCSPC); dyads exhibited efficient energy transfer up to 93% from beta‐donors (N‐butylcarbazole or triphenylamine group) to the porphyrin core. The efficiency of energy transfer for the beta‐substituted porphyrin dyads were much higher than those of the corresponding meso‐substituted porphyrin dyads, reflecting enhanced communications between the beta‐donors and the porphyrin core. The Pd(II) dyads, showed characteristic phosphorescence in the near IR region and very efficient singlet oxygen quantum yields (53–60%); these dyads are promising candidates for photocatalytic oxidations of organic compounds. The donor‐acceptor interaction between the porphyrin core and the beta‐donors was supported by the DFT studies in the porphyrin dyads. 相似文献
982.
Shokichi Tsukamoto Masahiro Takeuchi Takeharu Kawaguchi Emi Togasaki Atsuko Yamazaki Yasumasa Sugita Tomoya Muto Shio Sakai Yusuke Takeda Chikako Ohwada Emiko Sakaida Naomi Shimizu Keigo Nishii Meizi Jiang Koutaro Yokote Hideaki Bujo Chiaki Nakaseko 《Experimental & molecular medicine》2014,46(4):e89
LR11, also known as SorLA or SORL1, is a type-I membrane protein from which a large extracellular part, soluble LR11 (sLR11), is released by proteolytic shedding on cleavage with a disintegrin and metalloproteinase 17 (ADAM17). A shedding mechanism is presumed to have a key role in the functions of LR11, but the evidence for this has not yet been demonstrated. Tetraspanin CD9 has been recently shown to regulate the ADAM17-mediated shedding of tumor necrosis factor-α and intercellular adhesion molecule-1 on the cell surface. Here, we investigated the role of CD9 on the shedding of LR11 in leukocytes. LR11 was not expressed in THP-1 monocytes, but it was expressed and released in phorbol 12-myristate 13-acetate (PMA)-induced THP-1 macrophages (PMA/THP-1). Confocal microscopy showed colocalization of LR11 and CD9 proteins on the cell surface of PMA/THP-1. Ectopic neo-expression of CD9 in CCRF-SB cells, which are LR11-positive and CD9-negative, reduced the amount of sLR11 released from the cells. In contrast, incubation of LR11-transfected THP-1 cells with neutralizing anti-CD9 monoclonal antibodies increased the amount of sLR11 released from the cells. Likewise, the PMA-stimulated release of sLR11 increased in THP-1 cells transfected with CD9-targeted shRNAs, which was negated by treatment with the metalloproteinase inhibitor GM6001. These results suggest that the tetraspanin CD9 modulates the ADAM17-mediated shedding of LR11 in various leukemia cell lines and that the association between LR11 and CD9 on the cell surface has an important role in the ADAM17-mediated shedding mechanism. 相似文献
983.
Dr. Akitaka Ito Akihiro Shimizu Noriaki Kishida Yusuke Kawanaka Dr. Daisuke Kosumi Prof. Dr. Hideki Hashimoto Prof. Dr. Yoshio Teki 《Angewandte Chemie (International ed. in English)》2014,53(26):6715-6719
The excited‐state dynamics of pentacene derivatives with stable radical substituents were evaluated in detail through transient absorption measurements. The derivatives showed ultrafast formation of triplet excited state(s) in the pentacene moiety from a photoexcited singlet state through the contributions of enhanced intersystem crossing and singlet fission. Detailed kinetic analyses for the transient absorption data were conducted to quantify the excited‐state characteristics of the derivatives. 相似文献
984.
Shin‐ichiro Ishida Tomohiro Higashino Dr. Shigeki Mori Hirotaka Mori Dr. Naoki Aratani Dr. Takayuki Tanaka Dr. Jong Min Lim Prof. Dr. Dongho Kim Prof. Dr. Atsuhiro Osuka 《Angewandte Chemie (International ed. in English)》2014,53(13):3427-3431
Protonation of meso‐aryl [28]hexaphyrins(1.1.1.1.1.1) triggered conformational changes. Whereas protonation with trifluoroacetic acid led to the formation of monoprotonated Möbius aromatic species, protonation with methanesulfonic acid led to the formation of diprotonated triangular antiaromatic species. A peripherally hexaphenylated [28]hexaphyrin was rationally designed and prepared to undergo diprotonation to favorably afford a triangular‐shaped antiaromatic species. 相似文献
985.
Discovery of Clostrubin,an Exceptional Polyphenolic Polyketide Antibiotic from a Strictly Anaerobic Bacterium
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Dr. Sacha Pidot Dr. Keishi Ishida Michael Cyrulies Prof. Dr. Christian Hertweck 《Angewandte Chemie (International ed. in English)》2014,53(30):7856-7859
Genome mining of the strictly anaerobic bacterium Clostridium beijerinckii, an industrial producer of solvents, revealed the presence of several cryptic gene clusters for secondary metabolite biosynthesis. To unearth its metabolic potential, a C. beijerinckii strain was cultured under various conditions, which led to the discovery of a deep purple pigment. This novel metabolite, named clostrubin ( 1 ), was isolated and its structure was fully elucidated. The pentacyclic polyphenol features a benzo[a]tetraphene ring topology that is unprecedented for natural products. Stable‐isotope labeling experiments showed that 1 is an aromatic polyketide that folds in a noncanonical manner to form the unusual perifused ring system. In addition to being the first reported polyketide from an anaerobic bacterium, 1 is a potent antibiotic with pronounced activity against various pathogenic bacteria, such as MRSA, VRE, and mycobacteria, with minimum inhibitory concentrations (MIC) of 0.12–0.97 μM . 相似文献
986.
Dr. Shintaro Ishida Fumiya Hirakawa Prof. Dr. Ko Furukawa Dr. Kenji Yoza Prof. Dr. Takeaki Iwamoto 《Angewandte Chemie (International ed. in English)》2014,53(42):11172-11176
Stibinyl and bismuthinyl radicals are recognized as representative intermediates of antimony and bismuth compounds, but still elusive in the condensed phase. We successfully synthesized persistent stibinyl and bismuthinyl radicals in solution by facile dissociation of the corresponding dimers with bulky substituents. We characterized the radicals by NMR and UV/Vis spectroscopy and estimated the thermodynamic parameters for the dissociation equilibria. The radicals show n→p (HOMO→SOMO) transition bands at 497 nm (stibinyl) and 543 nm (bismuthinyl) in 3‐methylpentane and react with a stable nitroxyl radical to give the cross‐radical coupling products in good yields. 相似文献
987.
SiIV Incorporation into a [28]Hexaphyrin That Triggered Formation of Möbius Aromatic Molecules
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Shin‐ichiro Ishida Dr. Takayuki Tanaka Dr. Jong Min Lim Prof. Dr. Dongho Kim Prof. Dr. Atsuhiro Osuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(27):8274-8278
Incorporation of SiIV into an expanded porphyrin has been achieved for the first time. Treatment of [28]hexaphyrin 1 with CH3SiCl3 and N,N‐diisopropylethylamine gave SiIV complex 2 and its N‐fused product 4 that both have Möbius aromatic nature. In both complexes, the coordinated Si atom is satisfied in a typical trigonal bipyramidal coordination. SiIV incorporation induces conformational rigidification and redshifted absorption profiles due to σ–π conjugation between the Si atom and hexaphyrin macrocycle. Tamao–Fleming oxidation of 2 with H2O2 gave β‐hydroxy [28]hexaphyrin 5 , which exists as a ruffled rectangular shape in the solid state, yet it has been revealed to exist predominantly as a twisted Möbius aromatic conformer in CH2Cl2. 相似文献
988.
Silylation Improves the Photodynamic Activity of Tetraphenylporphyrin Derivatives In Vitro and In Vivo
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Prof. Hiroaki Horiuchi Prof. Masahiro Hosaka Hiroyuki Mashio Motoki Terata Prof. Shintaro Ishida Prof. Soichiro Kyushin Prof. Tetsuo Okutsu Prof. Toshiyuki Takeuchi Prof. Hiroshi Hiratsuka 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(20):6054-6060
The effects of silyl and hydrophilic groups on the photodynamic properties of tetraphenylporphyrin (TPP) derivatives have been studied in vitro and in vivo. Silylation led to an improvement in the quantum yield of singlet oxygen sensitization for both sulfo and carboxy derivatives, although the silylation did not affect other photophysical properties. Silylation also improved the cellular uptake efficiency for both sulfo and carboxy derivatives, enhancing the in vitro photodynamic activity of the photosensitizer in U251 human glioma cells. The carboxy derivative (SiTPPC4) was found to show higher cellular uptake efficiency and in vitro photodynamic activity than the corresponding sulfo derivative (SiTPPS4), which indicates that the carboxy group is a more promising hydrophilic group than the sulfo group in the silylated porphyrin. SiTPPC4 was found to show high selective accumulation efficiency in tumors, although almost no tumor selectivity was observed for the nonsilylated porphyrin. The concentration of SiTPPC4 in tumors was 13 times higher than that in muscle 12 h after drug administration. We also studied tumor response after treatment and found that silylation enhanced in vivo photodynamic activity significantly. SiTPPC4 shows higher photodynamic activity than NPe6 with white light irradiation. 相似文献
989.
Topotactic Conversion of β‐Helix‐Layered Silicate into AST‐Type Zeolite through Successive Interlayer Modifications
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Yusuke Asakura Ryosuke Takayama Dr. Toshimichi Shibue Prof. Dr. Kazuyuki Kuroda 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(7):1893-1900
AST‐type zeolite with a plate morphology can be synthesized by topotactic conversion of a layered silicate (β‐helix‐layered silicate; HLS) by using N,N‐dimethylpropionamide (DPA) to control the layer stacking of silicate layers and the subsequent interlayer condensation. Treatment of HLS twice with 1) hydrochloric acid/ethanol and 2) dimethylsulfoxide (DMSO) are needed to remove interlayer hydrated Na ions and tetramethylammonium (TMA) ions in intralayer cup‐like cavities (intracavity TMA ions), both of which are introduced during the preparation of HLS. The utilization of an amide molecule is effective for the control of the stacking sequence of silicate layers. This method could be applicable to various layered silicates that cannot be topotactically converted into three‐dimensional networks by simple interlayer condensation by judicious choice of amide molecules. 相似文献
990.
Sequence‐Specific DNA Recognition by Cyclic Pyrrole–Imidazole Cysteine‐Derived Polyamide Dimers
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Makoto Yamamoto Dr. Toshikazu Bando Hironobu Morinaga Yusuke Kawamoto Kaori Hashiya Prof. Dr. Hiroshi Sugiyama 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(3):752-759
Pyrrole–imidazole (PI) polyamides bind to the minor groove of the DNA duplex in a sequence‐specific manner and thus have the potential to regulate gene expression. To date, various types of PI polyamides have been designed as sequence‐specific DNA binding ligands. One of these, cysteine cyclic PI polyamides containing two β‐alanine molecules, were designed to recognize a 7 bp DNA sequence with high binding affinity. In this study, an efficient cyclization reaction between a cysteine and a chloroacetyl residue was used for dimerization in the synthesis of a unit that recognizes symmetrical DNA sequences. To evaluate specific DNA binding properties, dimeric PI polyamide binding was measured by using a surface plasmon resonance (SPR) method. Extending this molecular design, we synthesized a large dimeric PI polyamide that can recognize a 14 bp region in duplex DNA. 相似文献