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Total Synthesis and Structure Elucidation of JBIR‐39: A Linear Hexapeptide Possessing Piperazic Acid and γ‐Hydroxypiperazic Acid Residues 下载免费PDF全文
Dr. Masahito Yoshida Naoki Sekioka Dr. Miho Izumikawa Dr. Ikuko Kozone Dr. Motoki Takagi Dr. Kazuo Shin‐ya Prof. Dr. Takayuki Doi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(7):3031-3041
The total synthesis and stereochemical structural elucidation of JBIR‐39, containing four nonproteinogenic piperazic acid (Piz) residues, is reported. The synthesis includes Sc(OTf)3‐catalyzed acylation of a Piz(γ‐OTBS) derivative with piperazic acid chloride, providing the desired Piz‐Piz(γ‐OTBS) dipeptide in high yield without epimerization. After assembling two additional Piz moieties and (S)‐isoleucic acid at the N‐terminus, amidation with the (R)‐α‐methylserine ester at the C‐terminus, and deprotection afforded the desired (2R,8S)‐hexapeptide, which is the assumed structure of JBIR‐39. Although the spectral data of the (2R,8S)‐hexapeptide was not identical to JBIR‐39, further synthesis of three stereoisomers confirmed the stereochemical structure of JBIR‐39 to be (2S,6S,8S,11R,16S,21R,26S,27S). 相似文献
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Enhancement of Light Absorption Ability of Synthetic Chlorophyll Derivatives by Conjugation with a Difluoroboron Diketonate Group 下载免费PDF全文
Dr. Yusuke Kinoshita Dr. Yuichi Kitagawa Prof. Dr. Hitoshi Tamiaki 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(29):9996-10001
The enhancement of the light absorption ability of synthetic chlorophyll derivatives is demonstrated. Chlorophyll derivatives directly conjugated with a difluoroboron 1,3‐diketonate group at the C3 position were synthesized from methyl pyropheophorbide‐d through Barbier acylmethylation of the C3‐formyl moiety, oxidation of the C3‐carbinol, and difluoroboron complexation of the diketonate. Electronic absorption spectra in a diluted solution showed that the synthetic conjugates gave an absorption band at λ=400–500 nm, with a Qy band shifted to a longer wavelength of λ≈700 nm. DFT calculations demonstrated that the absorption bands and redshifts were ascribable to the coupling of the LUMO of chlorin with that of the difluoroboron diketonate moiety. The introduction of a pyrenyl group at the C33‐position of the conjugate afforded an additional charge‐transfer band over λ=500 nm, producing a pigment that bridged the green gap in standard chlorophylls. 相似文献
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Inside Cover: Enhancement of Light Absorption Ability of Synthetic Chlorophyll Derivatives by Conjugation with a Difluoroboron Diketonate Group (Chem. Eur. J. 29/2016) 下载免费PDF全文
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Yuanlin Li Tianfang Zheng Yanxiang Liu Prof. Georgiy G. Levchenko Prof. Wei Han Prof. Aleksey V. Pashchenko Prof. Shin-ichi Sasaki Prof. Hitoshi Tamiaki Prof. Xiao-Feng Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(56):e202201855
Hydrogen energy is an abundant, clean, sustainable and environmentally friendly renewable energy source. Therefore, the production of hydrogen by photocatalytically splitting water on semiconductors has been considered in recent years as a promising and sustainable strategy for converting solar energy into chemical energy to replace conventional energy sources and to solve the growing problem of environmental pollution and the global energy crisis. However, highly efficient solar-driven photocatalytic hydrogen production remains a huge challenge due to the poor visible light response of available photocatalytic materials and the low efficiency of separation and transfer of photogenerated electron-hole pairs. In the present work, organic heterojunction structures based on bacteriochlorophyll (BChl) and chlorophyll (Chl) molecules were introduced and used for solar-driven photocatalytic hydrogen production from water under visible light. Also, noble metal-free photocatalyst was successfully constructed on Ti3C2Tx nanosheets by simple successive deposition of Chl and BChl, which was used for the photocatalytic splitting water to hydrogen evolution reaction (HER). The results show that the optimal BChl@Chl@Ti3C2Tx composite has a high HER performance with 114 μmol/h/gcat, which is much higher than the BChl@Ti3C2Tx and Chl@Ti3C2Tx composites. 相似文献
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Takashi Yoshimoto Prof. Dr. Hisako Hashimoto Dr. Nozomi Takagi Prof. Dr. Shigeyoshi Sakaki Naoki Hayakawa Dr. Tsukasa Matsuo Prof. Dr. Hiromi Tobita 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(15):3795-3798
A tungsten silylyne complex having a W≡Si triple bond reacted with two molecules of aldehydes at room temperature to give W−Si−O−C four-membered metallacycles by [2+2] cycloaddition and subsequent formyl hydrogen transfer from one aldehyde molecule to another. Upon heating to 70 °C, the four-membered metallacycles underwent metathesis-like fragmentation cleanly to afford carbyne complexes and “silanoic esters,” in a manner similar to that of metallacyclobutadiene, an intermediate of alkyne metathesis reactions, and dimerization of the latter products gave 1,3-cyclodisiloxanes. The “silanoic ester” was also trapped by pivalaldehyde to give a [2+2] cycloaddition product in high yield. 相似文献
7.
Siti Masturah binti Fakhruddin Kosuke Ino Kumi Y. Inoue Yuji Nashimoto Hitoshi Shiku 《Electroanalysis》2022,34(2):212-226
Bipolar electrode-based (BPE-based) electrochromic devices have garnered increasing attention in the past decade. These BPE-based electrochromic devices have been used for analytical health monitoring, point-of-care (POC) diagnostics, and chemical sensing. In this review, we highlight recent progress made regarding BPE-based electrochromic devices constructed for these analytical applications. Various, available electrochromic materials are summarized in the first section, after which the different device types (e. g., paper-based and self-powered) are discussed. Biological- and chemical-based analytical demonstrations of these devices are then reviewed. Finally, we conclude this review with a perspective on the future developments of BPE-based electrochromic devices in analytical applications. 相似文献
8.
Noriki Kutsumura Kota Shibuya Hitoshi Yamaguchi Takao Saito 《Tetrahedron letters》2017,58(43):4099-4102
Regioselective elimination of a vicinal bis-triflate having an adjacent ether oxygen functional group has been developed. Considered in the context of our studies of the regioselective elimination of vicinal dibromide, the key to the mechanism involves the electron-withdrawing inductive effect of the neighboring oxygen functional group. Aliphatic vinyl triflate was shown to be effective in Suzuki–Miyaura cross coupling compared with corresponding aliphatic vinyl bromide. 相似文献
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