全文获取类型
收费全文 | 15194篇 |
免费 | 2154篇 |
国内免费 | 1757篇 |
专业分类
化学 | 12273篇 |
晶体学 | 512篇 |
力学 | 1355篇 |
综合类 | 48篇 |
数学 | 289篇 |
物理学 | 4628篇 |
出版年
2024年 | 49篇 |
2023年 | 196篇 |
2022年 | 462篇 |
2021年 | 500篇 |
2020年 | 804篇 |
2019年 | 573篇 |
2018年 | 514篇 |
2017年 | 557篇 |
2016年 | 821篇 |
2015年 | 824篇 |
2014年 | 878篇 |
2013年 | 1278篇 |
2012年 | 854篇 |
2011年 | 1029篇 |
2010年 | 875篇 |
2009年 | 901篇 |
2008年 | 970篇 |
2007年 | 998篇 |
2006年 | 880篇 |
2005年 | 734篇 |
2004年 | 699篇 |
2003年 | 696篇 |
2002年 | 465篇 |
2001年 | 399篇 |
2000年 | 338篇 |
1999年 | 256篇 |
1998年 | 236篇 |
1997年 | 192篇 |
1996年 | 152篇 |
1995年 | 108篇 |
1994年 | 117篇 |
1993年 | 77篇 |
1992年 | 72篇 |
1991年 | 55篇 |
1990年 | 57篇 |
1989年 | 48篇 |
1988年 | 34篇 |
1987年 | 54篇 |
1986年 | 61篇 |
1985年 | 75篇 |
1984年 | 41篇 |
1983年 | 42篇 |
1982年 | 50篇 |
1981年 | 36篇 |
1980年 | 20篇 |
1979年 | 12篇 |
1978年 | 4篇 |
1977年 | 2篇 |
1971年 | 6篇 |
1957年 | 1篇 |
排序方式: 共有10000条查询结果,搜索用时 31 毫秒
991.
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
992.
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
993.
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
994.
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
995.
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
996.
In this work, a novel electrochemiluminescent (ECL) pesticide sensor based on zinc oxide nanocrystals decorated nickel foam is proposed for determination of imidacloprid for the first time. The silica film was used as a morphology‐controlling factor for modification of the electrode with zinc oxide nanocrystals. Zinc oxide was selected as luminescent material due to its cheapness, non‐toxicity, high thermal stability and excellent luminescence properties which truly adhered on the surface of nickel foam. The K2S2O8 was used as strong co‐reactant for this purpose. The silica template plays an important role in controlling the size of ZnO nanocrystals. The Physical morphology of the ZnO/Ni‐foam electrode was performed by electrochemical impedance spectroscopy, Brunauer‐Emmett‐Teller (BET), X‐Ray diffraction analysis, field emission scanning electron microscopy, and energy‐dispersive X‐ray analysis. The ultra‐sensitive electrochemiluminescence method was successfully used for ultra‐trace determination of imidacloprid. The linear dynamic range and low detection limit were obtained 3×10?14 ?8×10?8 M and 4.4×10?15 M, respectively. Also, the relative standard deviation for 15 repetitive optical signals was calculated 1.09 %.The present ECL sensor exhibited superior performance toward the accurate determination of imidacloprid with good reproducibility and stability. 相似文献
997.
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
998.
《Journal of Saudi Chemical Society》2020,24(3):289-302
Chemotherapy is the most common treatment for all cancer patients but this treatment poses many side effects due to lack of drug’s selectivity. To overcome this problem, utilizing a better and more effective delivery agent is the solution. Mesoporous silica nanoparticles (MSNs) emerged as a promising platform in development of drug delivery agent. This is due to its desirable properties such as tunable pores, large surface area, good biocompatibility and easy functionalization. Furthermore, these properties can be tuned through the utilization of alternative template such as pyridinium ionic liquid. Besides, by employing surface functionalization, the effectiveness of MSNs as drug delivery agent may also increase. This work reported the usage of 1-hexadecylpyridinium bromide ionic liquid as template for MSNs production and the surface of MSNs was then further functionalized via post – grafting method in order to obtain MSN – NH2, MSN – SH and MSN – COOH as drug carrier, respectively. These functionalized MSNs were then used to study the drug loading and drug release of hydrophilic drug, gemcitabine and hydrophobic drug, quercetin. For quercetin, MSN-NH2 had the highest drug loading percentage (72%) and slowest release (14%) in 48 h while for gemcitabine, it was found that MSN-COOH had the highest drug loading percentage (45%) and slowest release (15%) in 48 h. Based on the results, it is suggested that mesoporous silica nanoparticle with surface functionalization has suitable properties for controlled drug release which gives constant release behavior over a period of time to avoid repeated administration of drug where the drug is administered at a fixed dosage and regular time interval. 相似文献
999.
《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
1000.
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