全文获取类型
收费全文 | 3020篇 |
免费 | 392篇 |
国内免费 | 223篇 |
专业分类
化学 | 2066篇 |
晶体学 | 44篇 |
力学 | 110篇 |
综合类 | 8篇 |
数学 | 434篇 |
物理学 | 973篇 |
出版年
2023年 | 39篇 |
2022年 | 48篇 |
2021年 | 81篇 |
2020年 | 113篇 |
2019年 | 104篇 |
2018年 | 93篇 |
2017年 | 84篇 |
2016年 | 125篇 |
2015年 | 156篇 |
2014年 | 143篇 |
2013年 | 261篇 |
2012年 | 270篇 |
2011年 | 288篇 |
2010年 | 167篇 |
2009年 | 152篇 |
2008年 | 197篇 |
2007年 | 187篇 |
2006年 | 140篇 |
2005年 | 137篇 |
2004年 | 92篇 |
2003年 | 110篇 |
2002年 | 67篇 |
2001年 | 76篇 |
2000年 | 58篇 |
1999年 | 48篇 |
1998年 | 44篇 |
1997年 | 35篇 |
1996年 | 45篇 |
1995年 | 30篇 |
1994年 | 36篇 |
1993年 | 36篇 |
1992年 | 24篇 |
1991年 | 24篇 |
1990年 | 10篇 |
1989年 | 28篇 |
1988年 | 14篇 |
1987年 | 8篇 |
1986年 | 20篇 |
1985年 | 10篇 |
1984年 | 12篇 |
1983年 | 2篇 |
1982年 | 5篇 |
1979年 | 2篇 |
1977年 | 3篇 |
1975年 | 3篇 |
1974年 | 1篇 |
1973年 | 3篇 |
1940年 | 1篇 |
1938年 | 1篇 |
1936年 | 1篇 |
排序方式: 共有3635条查询结果,搜索用时 18 毫秒
31.
M. A. Waghmare Mu. Naushad Z. A. Alothman A. U. Ubale H. M. Pathan 《Journal of Solid State Electrochemistry》2017,21(9):2531-2545
Zirconium oxide (ZrO2) is acquiring considerable attention of most of the research groups and leading to a large number of publications due to its unique properties, especially in the context of emerging trends in the third generation of solar cell research. ZrO2 films offer magnificent aspects related to physicochemical properties, and the properties are found to be dependent on synthesis methods. In the present review, various deposition techniques used to grow zirconium oxide thin films and their application to enhance the quantum efficiency of titanium oxide (TiO2) based dye-sensitized solar cells (DSSCs) are discussed. Also, the modulated performances of DSSCs fabricated by growing the conformal ZrO2 insulating films to retard interfacial recombination dynamics on preformed TiO2 films are discussed. 相似文献
32.
Sijia Peng Ruirui Sun Dr. Wenjuan Wang Dr. Chunlai Chen 《Angewandte Chemie (International ed. in English)》2017,56(24):6882-6885
Single-molecule fluorescence resonance energy transfer (sm-FRET) has become a widely used tool to reveal dynamic processes and molecule mechanisms hidden under ensemble measurements. However, the upper limit of fluorescent species used in sm-FRET is still orders of magnitude lower than the association affinity of many biological processes under physiological conditions. Herein, we introduce single-molecule photoactivation FRET (sm-PAFRET), a general approach to break the concentration barrier by using photoactivatable fluorophores as donors. We demonstrate sm-PAFRET by capturing transient FRET states and revealing new reaction pathways during translation using μm fluorophore labeled species, which is 2–3 orders of magnitude higher than commonly used in sm-FRET measurements. sm-PAFRET serves as an easy-to-implement tool to lift the concentration barrier and discover new molecular dynamic processes and mechanisms under physiological concentrations. 相似文献
33.
Quanwu Mu 《Frontiers of Mathematics in China》2017,12(6):1457-1468
Let d ? 3 be an integer, and set r = 2d?1 + 1 for 3 ? d ? 4, \(\tfrac{{17}}{{32}} \cdot 2^d + 1\) for 5 ? d ? 6, r = d2+d+1 for 7 ? d ? 8, and r = d2+d+2 for d ? 9, respectively. Suppose that Φ i (x, y) ∈ ?[x, y] (1 ? i ? r) are homogeneous and nondegenerate binary forms of degree d. Suppose further that λ1, λ2,..., λ r are nonzero real numbers with λ1/λ2 irrational, and λ1Φ1(x1, y1) + λ2Φ2(x2, y2) + · · · + λ r Φ r (x r , y r ) is indefinite. Then for any given real η and σ with 0 < σ < 22?d, it is proved that the inequality has infinitely many solutions in integers x1, x2,..., x r , y1, y2,..., y r . This result constitutes an improvement upon that of B. Q. Xue.
相似文献
$$\left| {\sum\limits_{i = 1}^r {{\lambda _i}\Phi {}_i\left( {{x_i},{y_i}} \right) + \eta } } \right| < {\left( {\mathop {\max \left\{ {\left| {{x_i}} \right|,\left| {{y_i}} \right|} \right\}}\limits_{1 \leqslant i \leqslant r} } \right)^{ - \sigma }}$$
34.
Zhenjie Mu Yuhao Zhu Yufeng Zhang Anwang Dong Chunyan Xing Ziru Niu Prof. Dr. Bo Wang Prof. Dr. Xiao Feng 《Angewandte Chemie (International ed. in English)》2023,62(17):e202300373
Pore environment and aggregated structure play a vital role in determining the properties of porous materials, especially regarding the mass transfer. Reticular chemistry imparts covalent organic frameworks (COFs) with well-aligned micro/mesopores, yet constructing hierarchical architectures remains a great challenge. Herein, we reported a COF-to-COF transformation methodology to prepare microtubular COFs. In this process, the C3-symmetric guanidine units decomposed into C2-symmetric hydrazine units, leading to the crystal transformation of COFs. Moreover, the aggregated structure and conversion degree varied with the reaction time, where the hollow tubular aggregates composed of mixed COF crystals could be obtained. Such hierarchical architecture leads to enhanced mass transfer properties, as proved by the adsorption measurement and chemical catalytic reactions. This self-template strategy was successfully applied to another four COFs with different building units. 相似文献
35.
Feifan Li Xinyang Mu Xueqing Tang Ge Song Hongzhao Sun Xiuling Zha Peiyan Sun Jianhui Fang Dongmei Hu Shan Cong Zhigang Zhao 《Angewandte Chemie (International ed. in English)》2023,62(12):e202218055
Non-metallic materials have emerged as a new family of active substrates for surface-enhanced Raman scattering (SERS), with unique advantages over their metal counterparts. However, owing to their inefficient interaction with the incident wavelength, the Raman enhancement achieved with non-metallic materials is considerably lower with respect to the metallic ones. Herein, we propose colourful semiconductor-based SERS substrates for the first time by utilizing a Fabry-Pérot cavity, which realize a large freedom in manipulating light. Owing to the delicate adjustment of the absorption in terms of both frequency and intensity, resonant absorption can be achieved with a variety of non-metal SERS substrates, with the sensitivity further enhanced by ≈100 times. As a typical example, by introducing a Fabry-Pérot-type substrate fabricated with SiO2/Si, a rather low detection limit of 10−16 M for the SARS-CoV-2S protein is achieved on SnS2. This study provides a realistic strategy for increasing SERS sensitivity when semiconductors are employed as SERS substrates. 相似文献
36.
Xingju Li Jiaqian Wang Qiao Yuan Xiangen Song Jiali Mu Yao Wei Li Yan Fanfei Sun Siquan Feng Yutong Cai Zheng Jiang Zhongkang Han Yunjie Ding 《Angewandte Chemie (International ed. in English)》2023,62(33):e202307570
Heterogeneous single-metal-site catalysts usually suffer from poor stability, thereby limiting industrial applications. Dual Pd1−Ru1 single-atom-sites supported on porous ionic polymers (Pd1−Ru1/PIPs) were constructed using a wetness impregnation method. The two isolated metal species in the form of a binuclear complex were immobilized on the cationic framework of PIPs through ionic bonds. Compared to the single Pd- or Ru-site catalyst, the dual single-atom system exhibits higher activity with 98 % acetylene conversion and near 100 % selectivity to dialkoxycarbonylation products, as well as better cycling stability for ten cycles without obvious decay. Based on DFT calculations, it was found that the single-Ru site exhibited a strong CO adsorption energy of −1.6 eV, leading to an increase in the local CO concentration of the catalyst. Notably, the Pd1−Ru1/PIPs catalyst had a much lower energy barrier of 2.49 eV compared to 3.87 eV of Pd1/PIPs for the rate-determining step. The synergetic effect between neighboring single sites Pd1 and Ru1 not only enhanced the overall activity, but also stabilized PdII active sites. The discovery of synergetic effects between single sites can deepen our understanding of single-site catalysts at the molecular level. 相似文献
37.
Jiashen Zhou Lin Zhang Yiran Wang Wenyan Song Yuzhou Huang Yajuan Mu Werner Schmitz Shu-Yu Zhang Houwen Lin Hong-Zhuan Chen Fei Ye Liang Zhang 《Angewandte Chemie (International ed. in English)》2023,62(46):e202313109
The short-chain dehydrogenase/reductase (SDR) superfamily members acyl-ACP reductases FabG and FabI are indispensable core enzymatic modules and catalytic orientation controllers in type-II fatty acid biosynthesis. Herein, we report their distinct substrate allosteric recognition and enantioselective reduction mechanisms. FabG achieves allosteric regulation of ACP and NADPH through ACP binding across two adjacent FabG monomers, while FabI follows an irreversible compulsory order of substrate binding in that NADH binding must precede that of ACP on a discrete FabI monomer. Moreover, FabG and FabI utilize a backdoor residue Phe187 or a “rheostat” α8 helix for acyl chain length selection, and their corresponding triad residues Ser142 or Tyr145 recognize the keto- or enoyl-acyl substrates, respectively, facilitating initiation of nucleophilic attack by NAD(P)H. The other two triad residues (Tyr and Lys) mediate subsequent proton transfer and (R)-3-hydroxyacyl- or saturated acyl-ACP production. 相似文献
38.
39.
研究高活性和稳定性的非贵金属基析氢催化剂对解决当前能源危机和环境污染问题具有重要意义.碳化钨具有与贵金属Pt类似的d带电子结构,因而成为一类新兴的非贵金属析氢催化剂,受到广泛关注.磷掺杂是提高催化剂析氢活性的有效方法之一,然而目前最常见的构筑磷掺杂方法是使用多金属氧酸盐(POMs,如H3PW12O40),其固定的W/P原子比导致W2C中的掺杂浓度难以调控,并且磷掺杂主要是进入碳载体而不是碳化物本身,从而导致无法明确杂原子对其电催化析氢活性的贡献.本文采用植酸(PA)为磷源设计合成了可控磷掺杂W2C纳米颗粒,并探讨了催化剂组分、杂原子掺杂位置与析氢性能之间的关系.深入研究了磷掺杂碳化钨(WCP)的化学结构和析氢活性.与原始的W2C催化剂相比,WCP具有更高的本征活性、更快的电子转移速率和更多的活性位数量,并且在酸性和碱性条件下均表现出较好的析氢性能.特别是过电位为-200 mV时,WCP催化剂的本征活性在酸性和碱性条件下分别为0.07和0.56 H2 s-1,高出纯W2C(0.01和0.05 H2 S-1)数倍.同时,在电流密度为-10 mA cm-2时,优化后的WCP催化剂在酸性和碱性条件下的析氢过电位分别降低了96和88 mV.XPS及EDS元素分析结果表明,随磷源添加量增加,磷掺杂从碳化钨表面逐渐向内部扩散,进一步说明磷取代位置与析氢活性之间的构效关系,高浓度的表面磷取代可以加速质子捕获过程,从而显著提高其析氢活性,而过量的内部磷取代会破坏W2C结构,降低电子转移速率,从而导致析氢性能下降.利用密度泛函理论计算深入研究了WCP具有较好析氢性能的原因,与内部磷取代相比,表面磷取代会使碳化钨表现出更合适的氢吸附自由能,并且更加有效地降低了氢释放势垒,从而优化了析氢反应动力学.综上,本文为元素掺杂工艺提供了新的思路,同时研究了表面异质原子对析氢活性的关键作用,为该类催化材料的构效关系研究提供了新思路. 相似文献
40.
Mubashir Hussain Zhen Chen Mu Lv Jingyi Xu Xiaohan Dong Jingzhou Zhao Song Li Yan Deng Nongyue He Zhiyang Li Bin Liu 《中国化学快报》2021,31(12):3163-3167
The rapid identification of pathogens is crucial in controlling the food quality and safety. The proposed system for the rapid and label-free identification of pathogens is based on the principle of laser scattering from the bacterial microbes. The clinical prototype consists of three parts: the laser beam, photodetectors, and the data acquisition system. The bacterial testing sample was mixed with 10 mL distilled water and placed inside the machine chamber. When the bacterial microbes pass by the laser beam, the scattering of light occurs due to variation in size, shape, and morphology. Due to this reason, different types of pathogens show their unique light scattering patterns. The photo-detectors were arranged at the surroundings of the sample at different angles to collect the scattered light. The photodetectors convert the scattered light intensity into a voltage waveform. The waveform features were acquired by using the power spectral characteristics, and the dimensionality of extracted features was reduced by applying minimal-redundancy-maximal-relevance criterion (mRMR). A support vector machine (SVM) classifier was developed by training the selected power spectral features for the classification of three different bacterial microbes. The resulting average identification accuracies of E. faecalis,E. coli and S. aureus were 99%, 87%, and 94%, respectively. The overall experimental results yield a higher accuracy of 93.6%, indicating that the proposed device has the potential for label-free identification of pathogens with simplicity, rapidity, and cost-effectiveness. 相似文献