全文获取类型
收费全文 | 15670篇 |
免费 | 3147篇 |
国内免费 | 1770篇 |
专业分类
化学 | 11483篇 |
晶体学 | 578篇 |
力学 | 1338篇 |
综合类 | 73篇 |
数学 | 345篇 |
物理学 | 6770篇 |
出版年
2024年 | 64篇 |
2023年 | 206篇 |
2022年 | 496篇 |
2021年 | 546篇 |
2020年 | 904篇 |
2019年 | 645篇 |
2018年 | 551篇 |
2017年 | 605篇 |
2016年 | 929篇 |
2015年 | 888篇 |
2014年 | 939篇 |
2013年 | 1480篇 |
2012年 | 952篇 |
2011年 | 1103篇 |
2010年 | 915篇 |
2009年 | 1001篇 |
2008年 | 1060篇 |
2007年 | 1057篇 |
2006年 | 957篇 |
2005年 | 761篇 |
2004年 | 756篇 |
2003年 | 721篇 |
2002年 | 508篇 |
2001年 | 458篇 |
2000年 | 379篇 |
1999年 | 294篇 |
1998年 | 258篇 |
1997年 | 186篇 |
1996年 | 169篇 |
1995年 | 110篇 |
1994年 | 119篇 |
1993年 | 84篇 |
1992年 | 80篇 |
1991年 | 65篇 |
1990年 | 58篇 |
1989年 | 46篇 |
1988年 | 25篇 |
1987年 | 36篇 |
1986年 | 31篇 |
1985年 | 24篇 |
1984年 | 31篇 |
1983年 | 20篇 |
1982年 | 18篇 |
1981年 | 9篇 |
1980年 | 4篇 |
1979年 | 10篇 |
1978年 | 4篇 |
1977年 | 8篇 |
1973年 | 4篇 |
1971年 | 6篇 |
排序方式: 共有10000条查询结果,搜索用时 187 毫秒
931.
David A. Burns Eric M. Press M. A. Siegler Rebekka S. Klausen V. Sara Thoi 《Angewandte Chemie (International ed. in English)》2020,59(2):763-768
We report the synthesis of a set of 2D metal–organic frameworks (MOFs) constructed with organosilicon‐based linkers. These oligosilyl MOFs feature linear SinMe2n(C6H4CO2H)2 ligands (lin‐Sin, n=2, 4) connected by Cu paddlewheels. The stacking arrangement of the 2D sheets is dictated by van der Waals interactions and is tunable by solvent exchange, leading to reversible structural transformations between many crystalline and amorphous phases. 相似文献
932.
Yannan Zhou Qun Xu Tianpei Ge Xiaoli Zheng Li Zhang Pengfei Yan 《Angewandte Chemie (International ed. in English)》2020,59(8):3322-3328
In two‐dimensional (2D) amorphous nanosheets, the electron–phonon coupling triggered by localization of the electronic state as well as multiple‐scattering feature make it exhibit excellent performance in optical science. VS2 nanosheets, especially single‐layer nanosheets with controllable electronic structure and intrinsic optical properties, have rarely been reported owing to the limited preparation methods. Now, a controllable and feasible switching method is used to fabricate 2D amorphous VS2 and partial crystallized 2D VO2(D) nanosheets by altering the pressure and temperature of supercritical CO2 precisely. Thanks to the strong carrier localization and the quantum confinement, the unique 2D amorphous structures exhibit full band absorption, strong photoluminescence, and outstanding photothermal conversion efficiency. 相似文献
933.
Jin Su Takashi Hisatomi Tsutomu Minegishi Kazunari Domen 《Angewandte Chemie (International ed. in English)》2020,59(33):13800-13806
Most CdTe photoanodes and photocathodes show positive and negative photocurrent onset potentials for water oxidation and reduction, respectively, and are thus unable to drive photoelectrochemical (PEC) water splitting without external applied biases. Herein, the activity of a CdTe photoanode having an internal p‐n junction during PEC water oxidation was enhanced by applying a CdCl2 annealing treatment together with surface modifications. The resulting CdTe photoanode generated photocurrents of 1.8 and 5.4 mA cm?2 at 0.6 and 1.2 VRHE, respectively, with a photoanodic current onset potential of 0.22 VRHE under simulated sunlight (AM 1.5G). The CdCl2 annealing increased the grain sizes and lowered the density of grain boundaries, allowing more efficient charge separation. Consequently, a two‐electrode tandem PEC cell comprising a CdTe‐based photoanode and photocathode split water without any external bias at a solar‐to‐hydrogen conversion efficiency of 0.51 % at the beginning of the reaction. 相似文献
934.
Amit Kumar Nitee Kumari Sateesh Dubbu Sumit Kumar Taewan Kwon Jung Hun Koo Jongwon Lim Inki Kim Yoon‐Kyoung Cho Junsuk Rho In Su Lee 《Angewandte Chemie (International ed. in English)》2020,59(24):9460-9469
Interest and challenges remain in designing and synthesizing catalysts with nature‐like complexity at few‐nm scale to harness unprecedented functionalities by using sustainable solar light. We introduce “nanocatalosomes”—a bio‐inspired bilayer‐vesicular design of nanoreactor with metallic bilayer shell‐in‐shell structure, having numerous controllable confined cavities within few‐nm interlayer space, customizable with different noble metals. The intershell‐confined plasmonically coupled hot‐nanospaces within the few‐nm cavities play a pivotal role in harnessing catalytic effects for various organic transformations, as demonstrated by “acceptorless dehydrogenation”, “Suzuki–Miyaura cross‐coupling” and “alkynyl annulation” affording clean conversions and turnover frequencies (TOFs) at least one order of magnitude higher than state‐of‐the‐art Au‐nanorod‐based plasmonic catalysts. This work paves the way towards next‐generation nanoreactors for chemical transformations with solar energy. 相似文献
935.
Qingju Wang Tian Ke Lifeng Yang Zhaoqiang Zhang Xili Cui Zongbi Bao Qilong Ren Qiwei Yang Huabin Xing 《Angewandte Chemie (International ed. in English)》2020,59(9):3423-3428
The separation of xenon/krypton (Xe/Kr) mixture is of great importance to industry, but the available porous materials allow the adsorption of both, Xe and Kr only with limited selectivity. Herein we report an anion‐pillared ultramicroporous material NbOFFIVE‐2‐Cu‐i (ZU‐62) with finely tuned pore aperture size and structure flexibility, which for the first time enables an inverse size‐sieving effect in separation along with record Xe/Kr selectivity and ultrahigh Xe capacity. Evidenced by single‐crystal X‐ray diffraction, the rotation of anions and pyridine rings upon contact of larger‐size Xe atoms adapts cavities to the shape/size of Xe and allows strong host‐Xe interaction, while the smaller‐size Kr is excluded. Breakthrough experiments confirmed that ZU‐62 has a real practical potential for producing high‐purity Kr and Xe from air‐separation byproducts, showing record Kr productivity (206 mL g?1) and Xe productivity (42 mL g?1, in desorption) as well as good recyclability. 相似文献
936.
Aura Valinien Povilas Virbickas Giedr Medvikyt Arnas Ramanavi
ius 《Electroanalysis》2020,32(3):503-509
Prussian blue (PB) is an electrochromic material, which can be used as a signal transducer in the formation of optical urea biosensors. The previous researches in electrochromic properties of PB demonstrated the optical PB response to ammonium ions, which occurs when ammonium ions are interacting with PB layer at a constant 0.2 V vs Ag|AgCl|KClsat potential. In this work PB optical dependence on ammonium ions concentration was applied in the formation of electrochromic urea biosensor. Biosensor was formed by modifying the optically transparent indium tin oxide (ITO) coated glass electrode (glass/ITO) with Prussian blue layer and immobilizing urease (glass/ITO/PB‐urease). Calibration curve showed the linear dependency (R2=0.995) between the change of maximal absorbance (ΔA) and urea concentration in concentration range varying from 3 mM to 30 mM. The highest sensitivity (4 ΔA M?1) of glass/ITO/PB‐urease biosensor is in the concentration range from 7 mM to 30 mM. It was determined that working principle of the glass/ITO/PB‐urease biosensor is not related to pH changes occurring during enzymatic hydrolysis of urea. 相似文献
937.
《Journal of Saudi Chemical Society》2020,24(2):282-287
By using urea linked porous organic polymers as template, a new nano palladium catalyst with low Pd loading can be easily prepared (1.0 wt% Pd only). Although such less amount of Pd was contained in this new catalyst, it is still an effective catalyst for the Suzuki-Miyaura coupling of aryl iodines and aryl boric acids, affording biphenyl products in excellent yields with outstandingly enhanced turnover numbers (up to 10,536) under green solvent (water). 相似文献
938.
Chaohai Wang Jeonghun Kim Jing Tang Jongbeom Na Yong‐Mook Kang Minjun Kim Hyunsoo Lim Yoshio Bando Jiansheng Li Yusuke Yamauchi 《Angewandte Chemie (International ed. in English)》2020,59(5):2066-2070
Carbon aerogels (CAs) with 3D interconnected networks hold promise for application in areas such as pollutant treatment, energy storage, and electrocatalysis. In spite of this, it remains challenging to synthesize high‐performance CAs on a large scale in a simple and sustainable manner. We report an eco‐friendly method for the scalable synthesis of ultralight and superporous CAs by using cheap and widely available agarose (AG) biomass as the carbon precursor. Zeolitic imidazolate framework‐8 (ZIF‐8) with high porosity is introduced into the AG aerogels to increase the specific surface area and enable heteroatom doping. After pyrolysis under inert atmosphere, the ZIF‐8/AG‐derived nitrogen‐doped CAs show a highly interconnected porous mazelike structure with a low density of 24 mg cm?3, a high specific surface area of 516 m2 g?1, and a large pore volume of 0.58 cm?3 g?1. The resulting CAs exhibit significant potential for application in the adsorption of organic pollutants. 相似文献
939.
Zhong Wei Jiang Yang Chun Zou Ting Ting Zhao Shu Jun Zhen Yuan Fang Li Cheng Zhi Huang 《Angewandte Chemie (International ed. in English)》2020,59(8):3300-3306
Synthesizing 2D metal–organic frameworks (2D MOFs) in high yields and rational tailoring of the properties in a predictable manner for specific applications is extremely challenging. Now, a series of porphyrin‐based 2D lanthanide MOFs (Ln‐TCPP, Ln=Ce, Sm, Eu, Tb, Yb, TCPP=tetrakis(4‐carboxyphenyl) porphyrin) with different thickness were successfully prepared in a household microwave oven. The as‐prepared 2D Ln‐TCPP nanosheets showed thickness‐dependent photocatalytic performances towards photooxidation of 1,5‐dihydroxynaphthalene (1,5‐DHN) to synthesize juglone. Particularly, the Yb‐TCPP displayed outstanding photodynamic activity to generate O2? and 1O2. This work not only provides fundamental insights into structure designing and property tailoring of 2D MOFs nanosheets, but also pave a new way to improve the photocatalytic performance. 相似文献
940.
Christoph Gbel Christian Hils Markus Drechsler Dirk Baabe Andreas Greiner Holger Schmalz Birgit Weber 《Angewandte Chemie (International ed. in English)》2020,59(14):5765-5770
Nanoparticles of the spin‐crossover coordination polymer [FeL(bipy)]n were synthesized by confined crystallization within the core of polystyrene‐block‐poly(4‐vinylpyridine) (PS‐b‐P4VP) diblock copolymer micelles. The 4VP units in the micellar core act as coordination sites for the Fe complex. In the bulk material, the spin‐crossover nanoparticles in the core are well isolated from each other allowing thermal treatment without disintegration of their structure. During annealing above the glass transition temperature of the PS block, the transition temperature is shifted gradually to higher temperatures from the as‐synthesized product (T1/2↓=163 K and T1/2↑=170 K) to the annealed product (T1/2↓=203 K and T1/2↑=217 K) along with an increase in hysteresis width from 6 K to 14 K. Thus, the spin‐crossover properties can be shifted towards the properties of the related bulk material. The stability of the nanocomposite allows further processing, such as electrospinning from solution. 相似文献