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1.
《中国化学快报》2020,31(7):1782-1786
Anodic electrocatalyst plays the core role in direct alcohol fuel cells (DAFCs), while traditional Pt-catalysts suffer from limited catalytic activity, high over potential and severe CO poisoning. Herein, by selectively depositing Rh atoms on the defective-sites of Pt nanowires (NWs), we developed a new Pt@Rh NW electrocatalyst that exhibited enhanced electrocatalytic performance for both methanol oxidation (MOR) and ethanol oxidation (EOR). Both cyclic voltammetry (CV) and in-situ infrared spectroscopy revealed that the presence of Rh atoms suppressed the generation of poisonous intermediates and completely oxidized alcohols molecule into CO2. Atomic resolusion spherical aberration corrected high-angle annular dark field scanning transmission electron microscopy (CS-HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDS) mapping analysis revealed that Rh atoms were primarily deposited on the defective sites of Pt NWs. Meanwhile, the presence of Rh atoms also modified the electronic state of Pt atoms and therefore lowered the onset potential for alcohols oxidation potential. This work gives the first clear clue on the role of the defective sites of Pt nanocatalyst poisoning, and propose that selectively blocking these sites with trace amount of Rh is an effective strategy in designing advantageous electrocatalysts. 相似文献
2.
采用超声水浸聚焦斜入射方式进行小棒材表面、近表缺陷检测时,声波在水/棒和棒/缺陷界面会发生反射、折射、散射、衍射及波形转换等一系列物理变换。此时缺陷可检性对声波入射条件十分敏感,常出现由于检测条件设置不当而导致缺陷漏检、误检的情况。为解决这一问题,本文针对小棒材超声斜入射检测中的主要参数——入射角和水距,开展声场及缺陷声响应仿真,研究检测参数对不同部位缺陷检测能力的影响,并对仿真结果进行试验验证。通过研究得到了检测水距、入射角度对缺陷检测能力的影响,并得到最优检测条件。试验验证结果表明研究制定的检测方案可有效检测出表面、近表面裂纹缺陷。 相似文献
3.
《Current Applied Physics》2020,20(11):1237-1243
CIGS solar cells with power conversion efficiency (PCE) in the range of 1.82%–12.30% were obtained by using two-step process, and were further analyzed through various measurement techniques. Material parameters showed diverse values and some trends depending on the device performance. The lower performance device showed small integrated PL intensity, short minority life time, larger defect density and lower activation energy, whereas the higher performance device showed opposite values. We investigated relationship between material parameters and PCE of solar cells, and found that some physical parameters such as integrated PL intensity, minority life time, defect density, and difference between band gap and activation energy (Eg-Ea), which all reflect defect states in bulk and at pn interface, are strongly related with PCE and would be used as a good indicator to evaluate device performance quickly. 相似文献
4.
本文结合可见-近红外-中红外瞬态吸收光谱技术对离子交换法制备的少层MoS2中缺陷介导的载流子动力学进行了详细的解析. 在近红外瞬态吸收光谱中观察到的宽带漂白信号表明少层MoS2纳米片带隙中分布着大量的缺陷态. 实验结果明确揭示了载流子被缺陷态的快速捕获以及进一步的复合过程,证明带隙中的缺陷态对MoS2光生载流子动力学过程起着至关重要的作用. 在中红外瞬态吸收光谱中观察到的正信号到负信号的转变进一步证实了在导带下小于0.24 eV处存在被载流子占据的缺陷态. 这些在少层MoS2纳米片中存在的缺陷态可以作为有效的载流子捕获中心来辅助光生载流子在皮秒时间尺度内完成非辐射复合过程. 相似文献
5.
We studied the oxidation resistance of graphene-coated Cu surface and its layer dependence by directly growing monolayer graphene with different multilayer structures coexisted, di-minishing the influence induced by residue and transfer technology. It is found that the Cu surface coated with the monolayer graphene demonstrate tremendous difference in oxidation pattern and oxidation rate, compared to that coated with the bilayer graphene, which is considered to be originated from the strain-induced linear oxidation channel in monolayer graphene and the intersection of easily-oxidized directions in each layer of bilayer graphene, respectively. We reveal that the defects on the graphene basal plane but not the boundaries are the main oxidation channel for Cu surface under graphene protection. Our finding indi-cates that compared to putting forth efforts to improve the quality of monolayer graphene by reducing defects, depositing multilayer graphene directly on metal is a simple and effective way to enhance the oxidation resistance of graphene-coated metals. 相似文献
6.
层状富锂材料具有超过250 mAh∙g−1的高可逆比容量,被认为是下一代高比能锂离子电池最具商业化前景的正极材料之一。然而,层状富锂材料在实际应用之前仍需解决诸多挑战,如高电压氧释放、层状到岩盐相的结构变化、过渡金属离子迁移等结构劣化,并由此带来了较低的初始库伦效率、电压/容量的衰减以及循环寿命的不足。针对以上问题,进行层状富锂材料改性无疑是一种行之有效的方法。本综述全面介绍了层状富锂材料的结构、组分以及电化学性能,在此基础上对材料改性策略进行了系统阐述,详细介绍了体相掺杂、表面包覆、缺陷设计、离子交换和微结构调控等一系列改性策略的现状以及发展趋势,最终提出了高容量和长循环层状富锂材料和高比能锂离子电池的设计思路。 相似文献
7.
Guanying Ye Prof. Suqin Liu Kuangmin Zhao Prof. Zhen He 《Angewandte Chemie (International ed. in English)》2023,62(21):e202303409
Targeted construction of carbon defects near the N dopants is an intriguing but challenging way to boost the electrocatalytic activity of N-doped carbon toward oxygen reduction reaction (ORR). Here, we report a novel site-specific etching strategy that features targeted anchoring of singlet oxygen (1O2) on the N-adjacent atoms to directionally construct topological carbon defects neighboring the N dopants in N-doped carbon (1O2−N/C). This 1O2−N/C exhibits the highest ORR half-wave potential of 0.915 VRHE among all the reported metal-free carbon catalysts. Pyridinic-N bonded with a carbon pentagon of the neighboring topological carbon defects is identified as the primary active configuration, rendering enhanced adsorption of O2, optimized adsorption energy of the ORR intermediates, and a significantly decreased total energy barrier for ORR. This 1O2-induced site-specific etching strategy is also applicable to different precursors, showing a tremendous potential for targeted construction of high-efficiency active sites in carbon-based materials. 相似文献
8.
Qing Yao Hui Li Dr. Jiawei Xue Dr. Shenlong Jiang Prof. Qun Zhang Prof. Jun Bao 《Angewandte Chemie (International ed. in English)》2023,62(34):e202308140
Inspired by its great success in the photovoltaic field, methylammonium lead iodide perovskite (MAPbI3) has recently been actively explored as photocatalysts in H2 evolution reactions. However, the practical application of MAPbI3 photocatalysts remains hampered by the intrinsically fast trapping and recombination of photogenerated charges. Herein, we propose a novel strategy of regulating the distribution of defective areas to promote charge-transfer dynamics of MAPbI3 photocatalysts. By deliberately designing and synthesizing the MAPbI3 photocatalysts featuring a unique continuation of defective areas, we demonstrate that such a feature enables retardation of charge trapping and recombination via lengthening the charge-transfer distance. As an outcome, such MAPbI3 photocatalysts turn out to achieve an impressive photocatalytic H2 evolution rate as high as 0.64 mmol ⋅ g−1 ⋅ h−1, one order of magnitude higher than that of the conventional MAPbI3 photocatalysts. This work establishes a new paradigm for controlling charge-transfer dynamics in photocatalysis. 相似文献
9.
Dr. Yang Wei Dr. Yue Pan Dr. Enlong Zhou Dr. Ze Yuan Dr. Hao Song Dr. Yilin Wang Dr. Jie Zhou Jiahui Rui Mengjiao Xu Prof. Lixin Ning Dr. Zhanning Liu Dr. Hongyu Wang Prof. Xiaoji Xie Prof. Xiaobin Tang Prof. Haiquan Su Xianran Xing Prof. Ling Huang 《Angewandte Chemie (International ed. in English)》2023,62(27):e202303482
Although large amount of effort has been invested in combating thermal quenching that severely degrades the performance of luminescent materials particularly at high temperatures, not much affirmative progress has been realized. Herein, we demonstrate that the Frenkel defect formed via controlled annealing of Sc2(WO4)3:Ln (Ln=Yb, Er, Eu, Tb, Sm), can work as energy reservoir and back-transfer the stored excitation energy to Ln3+ upon heating. Therefore, except routine anti-thermal quenching, thermally enhanced 415-fold downshifting and 405-fold upconversion luminescence are even obtained in Sc2(WO4)3:Yb/Er, which has set a record of both the Yb3+-Er3+ energy transfer efficiency (>85 %) and the working temperature at 500 and 1073 K, respectively. Moreover, this design strategy is extendable to other hosts possessing Frenkel defect, and modulation of which directly determines whether enhanced or decreased luminescence can be obtained. This discovery has paved new avenues to reliable generation of high-temperature luminescence. 相似文献
10.
Prof. Dr. Dengrong Sun Lok Wing Wong Hok Yin Wong Ka Hei Lai Dr. Lin Ye Xinyao Xv Prof. Dr. Thuc Hue Ly Prof. Dr. Qingming Deng Prof. Dr. Jiong Zhao 《Angewandte Chemie (International ed. in English)》2023,62(4):e202216008
The direct utilization of metal–organic frameworks (MOFs) for electrocatalytic oxygen evolution reaction (OER) has attracted increasing interests. Herein, we employ the low-dose integrated differential phase contrast-scanning transmission electron microscopy (iDPC-STEM) technique to visualize the atomic structure of multivariate MOFs (MTV-MOFs) for guiding the structural design of bulk MOFs for efficient OER. The iDPC-STEM images revealed that incorporating Fe3+ or 2-aminoterephthalate (ATA) into Ni-BDC (BDC: benzenedicarboxylate) can introduce inhomogeneous lattice strain that weaken the coordination bonds, which can be selectively cleaved via a mild heat treatment to simultaneously generate coordinatively unsaturated metal sites, conductive Ni@C and hierarchical porous structure. Thus, excellent OER activity with current densities of 10 and 100 mA cm−2 are achieved over the defective MOFs at small overpotentials of 286 mV and 365 mV, respectively, which is superior to the commercial RuO2 catalyst and most of the bulk MOFs. 相似文献