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排序方式: 共有204条查询结果,搜索用时 15 毫秒
1.
Zhitao Cui Wei Du Chengwei Xiao Qiaohong Li Rongjian Sa Chenghua Sun Zuju Ma 《Frontiers of Physics》2020,15(6):63502
MoS2 is a promising candidate for hydrogen evolution reaction (HER), while its active sites are mainly distributed on the edge sites rather than the basal plane sites. Herein, a strategy to overcome the inertness of the MoS2 basal surface and achieve high HER activity by combining single-boron catalyst and compressive strain was reported through density functional theory (DFT) computations. The ab initio molecular dynamics (AIMD) simulation on B@MoS2 suggests high thermodynamic and kinetic stability. We found that the rather strong adsorption of hydrogen by B@MoS2 can be alleviated by stress engineering. The optimal stress of −7% can achieve a nearly zero value of ΔGH (~ −0.084 eV), which is close to that of the ideal Pt–SACs for HER. The novel HER activity is attributed to (i) the B– doping brings the active site to the basal plane of MoS2 and reduces the band-gap, thereby increasing the conductivity; (ii) the compressive stress regulates the number of charge transfer between (H)–(B)–(MoS2), weakening the adsorption energy of hydrogen on B@MoS2. Moreover, we constructed a SiN/B@MoS2 heterojunction, which introduces an 8.6% compressive stress for B@MoS2 and yields an ideal ΔGH. This work provides an effective means to achieve high intrinsic HER activity for MoS2. 相似文献
2.
Yulu Jiang Dr. Taro Ozaki Mei Harada Tadachika Miyasaka Dr. Hajime Sato Dr. Kazunori Miyamoto Dr. Junichiro Kanazawa Dr. Chengwei Liu Prof. Dr. Jun-ichi Maruyama Dr. Masaatsu Adachi Dr. Atsuo Nakazaki Prof. Dr. Toshio Nishikawa Prof. Dr. Masanobu Uchiyama Dr. Atsushi Minami Prof. Dr. Hideaki Oikawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(41):18152-18158
Lolitrems are tremorgenic indole diterpenes that exhibit a unique 5/6 bicyclic system of the indole moiety. Although genetic analysis has indicated that the prenyltransferase LtmE and the cytochrome P450 LtmJ are involved in the construction of this unique structure, the detailed mechanism remains to be elucidated. Herein, we report the reconstitution of the biosynthetic pathway for lolitrems employing a recently established genome-editing technique for the expression host Aspergillus oryzae. Heterologous expression and bioconversion of the various intermediates revealed that LtmJ catalyzes multistep oxidation to furnish the lolitrem core. We also isolated the key reaction intermediate with an epoxyalcohol moiety. This observation allowed us to establish the mechanism of radical-induced cyclization, which was firmly supported by density functional theory calculations and a model experiment with a synthetic analogue. 相似文献
3.
Reconstitution of Biosynthetic Machinery for the Synthesis of the Highly Elaborated Indole Diterpene Penitrem 下载免费PDF全文
Dr. Chengwei Liu Koichi Tagami Dr. Atsushi Minami Tomoyuki Matsumoto Jens Christian Frisvad Hideyuki Suzuki Jun Ishikawa Katsuya Gomi Prof. Dr. Hideaki Oikawa 《Angewandte Chemie (International ed. in English)》2015,54(19):5748-5752
Penitrem A is one of the most elaborated members of the fungal indole diterpenes. Two separate penitrem gene clusters were identified using genomic and RNA sequencing data, and 13 out of 17 transformations in the penitrem biosynthesis were elucidated by heterologous reconstitution of the relevant genes. These reactions involve 1) a prenylation‐initiated cationic cyclization to install the bicyclo[3.2.0]heptane skeleton (PtmE), 2) a two‐step P450‐catalyzed oxidative processes forming the unique tricyclic penitrem skeleton (PtmK and PtmU), and 3) five sequential oxidative transformations (PtmKULNJ). Importantly, without conventional gene disruption, reconstitution of the biosynthetic machinery provided sufficient data to determine the pathway. It was thus demonstrated that the Aspergillus oryzae reconstitution system is a powerful method for studying the biosynthesis of complex natural products. 相似文献
4.
Cover Picture: Reconstitution of Biosynthetic Machinery for the Synthesis of the Highly Elaborated Indole Diterpene Penitrem (Angew. Chem. Int. Ed. 19/2015) 下载免费PDF全文
5.
本文建立了粗糙表面部分流体挤压膜的物理力学模型,分析了当粗糙表面间存在流体膜时的挤压特性.对于一维挤压膜问题,当表面粗糙度纹向参数γ≤1时,粗糙度使流体阻尼增大,使平均流体膜的保持性提高;当γ>1时,粗糙度使流体阻尼减小,使平均流体膜的保持性下降.当γ保持不变时,粗糙度增大加快了固体接触的发生,并使固体接触刚度增大. 相似文献
6.
相关分析与谱分析在表面形貌研究中的应用 总被引:2,自引:0,他引:2
本文通过对表面形貌进行相关分析与谱分析,提出了相对波度和有效波度、相对波长和有效波长的概念,并且指出相关分析与谱分析是研究表面形貌润滑效应的有力工具。作者认为,当相对波度为有效波度时,应当同时考虑波长和幅值的摩擦学效应;当相对波度为高频的粗糙度时,只需考虑表面形貌的幅值效应。 相似文献
7.
电流变智能轴承挤压性能分析 总被引:1,自引:0,他引:1
电流变流体的流变性质可以通过调节外加电场(或电压)来控制,且响应时间极短,为此可用来制成电流变智能轴承。这种轴承的优点是可由计算机来监控轴承的工作状态,并根据其工作条件的变化来控制电压高低,从而改变轴承的性能,以适应外界环境。本文采用作者提出的以二次规划法为基础的双线性流变有限元法分析了电流变智能轴承的恒载径向挤压特性,给出了在不同外界电压下的轴承油膜沉降速度和时间曲线,通过数值讨论,证明电流变轴承具有很强的油膜保持能力的优点。 相似文献
8.
Wu Chengwei 《Acta Mechanica Sinica》1993,9(2):124-130
Bilinear rheological lubrication mechanics provides an important basis for the designs of recently developed electrorheological
(ER) “smart”journal bearings and those lubricated by mixed fluid-solid lubricants. But there is not yet a reliable and efficient
numerical method for such a problem of non-Newtonian fluid mechanics. In the present paper, a finite element method (FEM)
together with mat hematical programming solution is successfully used to solve such a problem. A reliable and generalized
numerical method for the designs of electrorheological “smart” journal bearings and the bearings lubricated by mixed fluid-solid
lubricant is presented. 相似文献
9.
Optical Review - In this paper, a novel phase demodulation method for multiple self-mixing interferometry (MSMI) is proposed, which can improve the resolution and accuracy of vibration measurement... 相似文献
10.
Yulu Jiang Taro Ozaki Mei Harada Tadachika Miyasaka Hajime Sato Kazunori Miyamoto Junichiro Kanazawa Chengwei Liu Jun‐ichi Maruyama Masaatsu Adachi Atsuo Nakazaki Toshio Nishikawa Masanobu Uchiyama Atsushi Minami Hideaki Oikawa 《Angewandte Chemie (International ed. in English)》2020,59(41):17996-18002
Lolitrems are tremorgenic indole diterpenes that exhibit a unique 5/6 bicyclic system of the indole moiety. Although genetic analysis has indicated that the prenyltransferase LtmE and the cytochrome P450 LtmJ are involved in the construction of this unique structure, the detailed mechanism remains to be elucidated. Herein, we report the reconstitution of the biosynthetic pathway for lolitrems employing a recently established genome‐editing technique for the expression host Aspergillus oryzae. Heterologous expression and bioconversion of the various intermediates revealed that LtmJ catalyzes multistep oxidation to furnish the lolitrem core. We also isolated the key reaction intermediate with an epoxyalcohol moiety. This observation allowed us to establish the mechanism of radical‐induced cyclization, which was firmly supported by density functional theory calculations and a model experiment with a synthetic analogue. 相似文献