全文获取类型
收费全文 | 385篇 |
免费 | 4篇 |
国内免费 | 14篇 |
专业分类
化学 | 293篇 |
晶体学 | 10篇 |
力学 | 2篇 |
综合类 | 1篇 |
物理学 | 97篇 |
出版年
2023年 | 53篇 |
2022年 | 9篇 |
2021年 | 6篇 |
2020年 | 6篇 |
2019年 | 4篇 |
2018年 | 2篇 |
2017年 | 2篇 |
2016年 | 11篇 |
2015年 | 5篇 |
2014年 | 8篇 |
2013年 | 11篇 |
2012年 | 26篇 |
2011年 | 18篇 |
2010年 | 10篇 |
2009年 | 4篇 |
2008年 | 16篇 |
2007年 | 14篇 |
2006年 | 11篇 |
2005年 | 8篇 |
2004年 | 8篇 |
2003年 | 18篇 |
2002年 | 19篇 |
2001年 | 15篇 |
2000年 | 9篇 |
1999年 | 4篇 |
1998年 | 2篇 |
1997年 | 10篇 |
1996年 | 12篇 |
1995年 | 13篇 |
1994年 | 10篇 |
1993年 | 15篇 |
1992年 | 7篇 |
1991年 | 10篇 |
1990年 | 8篇 |
1989年 | 4篇 |
1988年 | 2篇 |
1987年 | 2篇 |
1986年 | 2篇 |
1985年 | 3篇 |
1984年 | 1篇 |
1981年 | 3篇 |
1980年 | 2篇 |
排序方式: 共有403条查询结果,搜索用时 46 毫秒
1.
O. Guselnikova J.P. Fraser N. Soldatova E. Sviridova A. Ivanov R. Rodriguez A.Y. Ganin P. Postnikov 《Materials Today Chemistry》2022
Covalent functionalization of 2D materials provides a tailored approach towards tuning of their chemical, optical, and electronic properties making the search for new ways to graft small molecules important. Herein, the reaction with (3,5-bis(trifluoromethyl)phenyl)iodonium salt is revealed as an effective strategy for functionalization of MoTe2 thin films. Upon decomposition of the salt, the generated radicals graft covalently as aryl-(CF3)2 groups at the surface of both metallic (1T’) and semiconducting (2H) polymorphs of MoTe2. Remarkably, the reactivity of the salt is governed by the electronic structure of the given polymorph. While the functionalization of the metallic MoTe2 occurs spontaneously, the semiconducting MoTe2 requires activation by light. The reaction proceeds with the elimination of oxide from the original films yielding the functionalized products that remain protected in ambient conditions, presenting a viable solution to the ageing of MoTe2 in air. 相似文献
2.
Prof. Qinghao Li Qi Liang Dr. Hui Zhang Sichen Jiao Dr. Zengqing Zhuo Dr. Junyang Wang Prof. Qiang Li Prof. Jie-Nan Zhang Prof. Xiqian Yu 《Angewandte Chemie (International ed. in English)》2023,62(5):e202215131
Charge compensation on anionic redox reaction (ARR) has been promising to realize extra capacity beyond transition metal redox in battery cathodes. The practical development of ARR capacity has been hindered by high-valence oxygen instability, particularly at cathode surfaces. However, the direct probe of surface oxygen behavior has been challenging. Here, the electronic states of surface oxygen are investigated by combining mapping of resonant Auger electronic spectroscopy (mRAS) and ambient pressure X-ray photoelectron spectroscopy (APXPS) on a model LiCoO2 cathode. The mRAS verified that no high-valence oxygen can sustain at cathode surfaces, while APXPS proves that cathode electrolyte interphase (CEI) layer evolves and oxidizes upon oxygen gas contact. This work provides valuable insights into the high-valence oxygen degradation mode across the interface. Oxygen stabilization from surface architecture is proven a prerequisite to the practical development of ARR active cathodes. 相似文献
3.
Dr. Keke Guo Weijun Li Yuhong He Xiaopeng Feng Jinmei Song Wanting Pan Wei Qu Prof. Bai Yang Prof. Haotong Wei 《Angewandte Chemie (International ed. in English)》2023,62(23):e202303445
The low-dimensional halide perovskites have attracted increasing attention due to their improved moisture stability, reduced defects, and suppressed ions migration in many optoelectronic devices such as solar cells, light-emitting diodes, X-ray detectors, and so on. However, they are still limited by their large band gap and short charge carriers’ diffusion length. Here, we demonstrate that the introduction of metal ions into organic interlayers of two-dimensional (2D) perovskite by cross-linking the copper paddle-wheel cluster-based lead bromide ([Cu(O2C−(CH2)3−NH3)2]PbBr4) perovskite single crystals with coordination bonds can not only significantly reduce the perovskite band gap to 0.96 eV to boost the X-ray induced charge carriers, but can also selectively improve the charge carriers’ transport along the out-of-plane direction and blocking the ions motion paths. The [Cu(O2C−(CH2)3−NH3)2]PbBr4 single-crystal device can reach a record charges/ions collection ratio of 1.69×1018±4.7 % μGyair−1 s, and exhibit a large sensitivity of 1.14×105±7% μC Gyair−1 cm−2 with the lowest detectable dose rate of 56 nGyair s−1 under 120 keV X-rays irradiation. In addition, [Cu(O2C−(CH2)3−NH3)2]PbBr4 single-crystal detector exposed to the air without any encapsulation shows excellent X-ray imaging capability with long-term operational stability without any attenuation of 120 days. 相似文献
4.
Zhiguo Sun Huijuan Zhang Linlin Cao Xiaokang Liu Dan Wu Xinyi Shen Xue Zhang Zihang Chen Sen Ru Xiangyu Zhu Zhiyuan Xia Qiquan Luo Faqiang Xu Prof. Tao Yao 《Angewandte Chemie (International ed. in English)》2023,62(13):e202217719
The construction and understanding of synergy in well-defined dual-atom active sites is an available avenue to promote multistep tandem catalytic reactions. Herein, we construct a dual-hetero-atom catalyst that comprises adjacent Cu-N4 and Se-C3 active sites for efficient oxygen reduction reaction (ORR) activity. Operando X-ray absorption spectroscopy coupled with theoretical calculations provide in-depth insights into this dual-atom synergy mechanism for ORR under realistic device operation conditions. The heteroatom Se modulator can efficiently polarize the charge distribution around symmetrical Cu-N4 moieties, and serve as synergistic site to facilitate the second oxygen reduction step simultaneously, in which the key OOH*-(Cu1-N4) transforms to O*-(Se1-C2) intermediate on the dual-atom sites. Therefore, this designed catalyst achieves satisfied alkaline ORR activity with a half-wave potential of 0.905 V vs. RHE and a maximum power density of 206.5 mW cm−2 in Zn-air battery. 相似文献
5.
Prof. Yoann Olivier Prof. Juan-Carlos Sancho-García 《Angewandte Chemie (International ed. in English)》2023,62(38):e202305501
New heterocyclic diradicaloids based on boron and nitrogen-doped polycyclic systems with open-shell ground-states are obtained via concomitant structural and quinoidal extensions, thus allowing to merge the best of both design strategies. A combination of experimental characterization and theoretical calculations have helped disclose their electronic structure, as well as rationalize their associated magnetic and photophysical properties, spanning the chemical space of available molecular templates for cutting-edge applications in organic electronics and spintronics. 相似文献
6.
Qiu-Chen Peng Dr. Yu-Bing Si Jia-Wang Yuan Qi Yang Zi-Ying Gao Dr. Yuan-Yuan Liu Dr. Zhao-Yang Wang Dr. Kai Li Prof. Shuang-Quan Zang Prof. Ben Zhong Tang 《Angewandte Chemie (International ed. in English)》2023,62(40):e202308194
X-ray imaging technology has achieved important applications in many fields and has attracted extensive attentions. Dynamic X-ray flexible imaging for the real-time observation of the internal structure of complex materials is the most challenging type of X-ray imaging technology, which requires high-performance X-ray scintillators with high X-ray excited luminescence (XEL) efficiency as well as excellent processibility and stability. Here, a macrocyclic bridging ligand with aggregation-induced emission (AIE) feature was introduced for constructing a copper iodide cluster-based metal–organic framework (MOF) scintillator. This strategy endows the scintillator with high XEL efficiency and excellent chemical stability. Moreover, a regular rod-like microcrystal was prepared through the addition of polyvinyl pyrrolidone during the in situ synthesis process, which further enhanced the XEL and processibility of the scintillator. The microcrystal was used for the preparation of a scintillator screen with excellent flexibility and stability, which can be used for high-performance X-ray imaging in extremely humid environments. Furthermore, dynamic X-ray flexible imaging was realized for the first time. The internal structure of flexible objects was observed in real time with an ultrahigh resolution of 20 LP mm−1. 相似文献
7.
Wei Zhang Ping Sui Prof. Wei Zheng Prof. Lingyun Li Prof. Shuaihua Wang Prof. Ping Huang Wen Zhang Qi Zhang Prof. Yan Yu Prof. Xueyuan Chen 《Angewandte Chemie (International ed. in English)》2023,62(45):e202309230
Eco-friendly lead-free organic–inorganic manganese halides (OIMHs) have attracted considerable attention in various optoelectronic applications because of their superior optical properties and flexible solution processibility. Herein, we report a novel pseudo-2D layered OIMH (MTP)2MnBr4 (MTP: methyltriphenylphosphonium), which exhibits intense green emission under UV/blue or X-ray excitation, with a near-unity photoluminescence quantum yield, high resistance to thermal quenching (I150 °C=84.1 %) and good photochemical stability. These features enable (MTP)2MnBr4 as an efficient green phosphor for blue-converted white light-emitting diodes, demonstrating a commercial-level luminous efficiency of 101 lm W−1 and a wide color gamut of 116 % NTSC. Moreover, these (MTP)2MnBr4 crystals showcase outstanding X-ray scintillation properties, delivering a light yield of 67000 photon MeV−1, a detection limit of 82.4 nGy s−1, and a competitive spatial resolution of 6.2 lp mm−1 for X-ray imaging. This work presents a new avenue for the exploration of eco-friendly luminescent OIMHs towards multifunctional light-emitting applications. 相似文献
8.
Dr. Jifu Duan Dr. Anja Hemschemeier David J. Burr Dr. Sven T. Stripp Prof. Eckhard Hofmann Prof. Thomas Happe 《Angewandte Chemie (International ed. in English)》2023,62(7):e202216903
Hydrogenases are H2 converting enzymes that harbor catalytic cofactors in which iron (Fe) ions are coordinated by biologically unusual carbon monoxide (CO) and cyanide (CN−) ligands. Extrinsic CO and CN−, however, inhibit hydrogenases. The mechanism by which CN− binds to [FeFe]-hydrogenases is not known. Here, we obtained crystal structures of the CN−-treated [FeFe]-hydrogenase CpI from Clostridium pasteurianum. The high resolution of 1.39 Å allowed us to distinguish intrinsic CN− and CO ligands and to show that extrinsic CN− binds to the open coordination site of the cofactor where CO is known to bind. In contrast to other inhibitors, CN− treated crystals show conformational changes of conserved residues within the proton transfer pathway which could allow a direct proton transfer between E279 and S319. This configuration has been proposed to be vital for efficient proton transfer, but has never been observed structurally. 相似文献
9.
Xiang Li Guodong Zhang Yunqiu Hua Fucai Cui Xue Sun Jiaxin Liu Hongjie Liu Yanxiao Bi Zhongjie Yue Zhongjun Zhai Haibing Xia Xutang Tao 《Angewandte Chemie (International ed. in English)》2023,62(50):e202315817
Inorganic Bi-based perovskites have shown great potential in X-ray detection for their large absorption to X-rays, diverse low-dimensional structures, and eco-friendliness without toxic metals. However, they suffer from poor carrier transport properties compared to Pb-based perovskites. Here, we propose a mixed-halogen strategy to tune the structural dimensions and optoelectronic properties of Cs3Bi2I9−nBrn (0≤n≤9). Ten centimeter-sized single crystals are successfully grown by the Bridgman technique. Upon doping bromine to zero-dimensional Cs3Bi2I9, the crystal transforms into a two-dimensional structure as the bromine content reaches Cs3Bi2I8Br. Correspondingly, the optoelectronic properties are adjusted. Among these crystals, Cs3Bi2I8Br exhibits negligible ion migration, moderate resistivity, and the best carrier transport capability. The sensitivities in 100 keV hard X-ray detection are 1.33×104 and 1.74×104 μC Gyair−1 cm−2 at room temperature and 75 °C, respectively, which are the highest among all reported bismuth perovskites. Moreover, the lowest detection limit of 28.6 nGyair s−1 and ultralow dark current drift of 9.12×10−9 nA cm−1 s−1 V−1 are obtained owing to the high ionic activation energy. Our work demonstrates that Br incorporation is an effective strategy to enhance the X-ray detection performance by tuning the dimensional and optoelectronic properties. 相似文献
10.
脑疾病的诊疗、 探索高级脑功能机制和理解意识本源对脑科学研究具有重要意义. 成像技术在阐明脑科学神经系统结构和功能中发挥了重要作用. 迄今, 核磁共振成像、 光学成像和电子显微镜成像技术已为脑科学研究提供了强有力的手段, 取得了突出的进展. 同步辐射X射线显微成像技术具有高分辨率、 快成像速度和高穿透深度等优点, 是一类与已有技术互补的新型脑成像技术. 本文介绍了核磁共振波谱、 光学显微镜和电子显微镜等成像方法在脑成像领域中的应用, 重点阐述了同步辐射X射线成像的优势以及在脑结构成像和功能成像中的应用. 在此基础上, 展望了同步辐射X射线成像应用于脑科学研究的未来发展方向, 讨论了该技术在绘制人脑联接图谱中的优势及可行性. 相似文献