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采用密度泛函理论计算研究了在铈表面掺杂的过渡金属(TM)离子对表面晶格氧原子活化的影响.为此,测定了经TM离子修饰的CeO2最稳定(111)表面终端的结构和稳定性.除了保持八面体氧配位的锆和铂掺杂剂外, TM掺杂剂在取代表面Ce离子时更倾向于正方形平面配位.除了Pt(1.14 eV)和Zr(正方形平面配位不稳定)外,所有TM掺杂剂的表面结构从八面体到正方形平面都很容易.通常,四价TM阳离子的离子半径比Ce^4+的小得多,从而导致了显著的拉伸应变晶格,并解释了氧空位形成能量的降低.除Zr外,当产生一个氧空位时,优先形成正方形平面结构.热力学分析表明, TM掺杂CeO2表面在典型环境催化条件下存在氧缺陷.一个具有实际意义的例子是锆掺杂CeO2(111)中的晶格氧容易活化,从而有利于CO氧化.研究结果强调了晶格氧活化的本质和TM掺杂剂在TM-铈固溶催化剂中的优选位置. 相似文献
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A high performance liquid chromatographic method with fluorimetric detection for the determination of aflatoxin M1 (AFM1) in milk has been optimized and validated according to Commission Decision 2002/657/EC by using the conventional validation approach. The procedure for determining selectivity, recovery, precision, decision limit (CCα), detection capability (CCβ) and ruggedness of the method has been reported. The results of the validation process demonstrate the agreement of the method with the provisions of Commission Regulation 401/2006/EC. The mean recovery calculated at three levels of fortification (0.5, 1.0, and 1.5-fold the MRL) was 91% and the maximum relative standard deviation value for the within-laboratory reproducibility was 15%. Limit of detection (LOD) and limit of quantitation (LOQ) values were 0.006 μg kg−1 and 0.015 μg kg−1 while the CCα and CCβ values were 0.058 μg kg−1 and 0.065 μg kg−1, respectively. The relative expanded measurement uncertainty of the method was 7%. The method was not affected by slight variations of some critical factors (ruggedness minor changes) as pre-treatment and clean-up of milk samples, thermal treatment and different storage conditions, as well as by major changes valued in terms of milk produced by different species (buffalo, goat and sheep). The method allowed accurate confirmation analyses of milk samples, resulted positive by the screening method. In fact, the Z-score values attained in a proficiency test round were well below the reference value of 1, proving the excellent laboratory performances. 相似文献
35.
Abe K Hayato Y Iida T Ikeda M Iyogi K Kameda J Koshio Y Kozuma Y Miura M Moriyama S Nakahata M Nakayama S Obayashi Y Sekiya H Shiozawa M Suzuki Y Takeda A Takenaga Y Takeuchi Y Ueno K Ueshima K Watanabe H Yamada S Yokozawa T Ishihara C Kaji H Lee KP Kajita T Kaneyuki K McLachlan T Okumura K Shimizu Y Tanimoto N Martens K Vagins MR Labarga L Magro LM Dufour F Kearns E Litos M Raaf JL Stone JL Sulak LR Goldhaber M Bays K Kropp WR Mine S Regis C Smy MB Sobel HW Ganezer KS Hill J Keig WE Jang JS 《Physical review letters》2011,107(24):241801
We present a search for differences in the oscillations of antineutrinos and neutrinos in the Super-Kamiokande-I, -II, and -III atmospheric neutrino sample. Under a two-flavor disappearance model with separate mixing parameters between neutrinos and antineutrinos, we find no evidence for a difference in oscillation parameters. Best-fit antineutrino mixing is found to be at (Δm2,sin2 2θ)=(2.0×10(-3) eV2, 1.0) and is consistent with the overall Super-K measurement. 相似文献
36.
薄壁杆系结构的梁元分析模型 总被引:1,自引:0,他引:1
本文导出了用于薄壁杆系结构弹性分析的薄壁梁元分析模型,在空间梁元分析模型^[3]的基础上,采用了一种改进的位移模式,考察了薄壁杆件可能发生的拉压,剪切,弯曲,扭转和翘曲等各变形形式以及它们的耦合效应,得出了相应的单元形函数,同时从工程应变的定义出发,采用Taylor级数展开的方法,建立了单元的五阶近似正交变表达式,并建立了相应的薄壁单元刚度方程,从而得出了局部坐标系下单元刚度矩阵的显式,根据本文所导出的薄壁梁元分析模型,编制了相应的结构计算程序,通过算例验证了本文所推导的单元刚度矩阵,同时通过与传统空间梁元计算模型计算结果的比较,阐述了截面翘曲对薄壁杆系结构的影响。 相似文献
37.
Magro G Donnadieu B Caminade AM Majoral JP 《Chemistry (Weinheim an der Bergstrasse, Germany)》2003,9(10):2151-2159
The step-by-step synthesis of the first oligophosphazenes having more than two types of side functions is described. These multifunctionalized oligophosphazenes possess up to four phosphazene linkages and up to four types of functional side groups. These compounds may serve as models for a better understanding of electronic delocalization phenomena in linear inorganic chains, and constitute novel cores for the synthesis of new dendrimeric species possessing several types of functions as end groups, at the level of the core, and within the branches. 相似文献
38.
Bhattarai KM del Amo V Magro G Sisson AL Joos JB Charmant JP Kantacha A Davis AP 《Chemical communications (Cambridge, England)》2006,(22):2335-2337
Cholic acid has been converted into triamine with the all-trans polycyclic allocholanoyl skeleton and co-directed, axial amino groups; the potential of this system as a scaffold is illustrated by conversion to a preorganised anion receptor. 相似文献
39.
A Magnetically Drivable Nanovehicle for Curcumin with Antioxidant Capacity and MRI Relaxation Properties 下载免费PDF全文
Massimiliano Magro René Campos Davide Baratella Giuseppina Lima Katerina Holà Clemens Divoky Rudolf Stollberger Ondrej Malina Claudia Aparicio Giorgio Zoppellaro Prof. Radek Zbořil Prof. Fabio Vianello 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(37):11913-11920
Curcumin possesses wide‐ranging anti‐inflammatory and anti‐cancer properties and its biological activity can be linked to its potent antioxidant capacity. Superparamagnetic maghemite (γ‐Fe2O3), called surface‐active maghemite nanoparticles (SAMNs) were surface‐modified with curcumin molecules, due to the presence of under‐coordinated FeIII atoms on the nanoparticle surface. The so‐obtained curcumin‐modified SAMNs (SAMN@curcumin) had a mean size of 13±4 nm. SAMN@curcumin was characterized by transmission and scanning electron microscopy, UV/Vis, FTIR, and Mössbauer spectroscopy, X‐ray powder diffraction, bulk susceptibility (SQUID), and relaxometry measurements (MRI imaging). The high negative contrast proclivity of SAMN@curcumin to act as potential contrast agent in MRI screenings was also tested. Moreover, the redox properties of bound curcumin were probed by electrochemistry. SAMN@curcumin was studied in the presence of different electroactive molecules, namely hydroquinone, NADH and ferrocyanide, to assess its redox behavior. Finally, SAMN@curcumin was electrochemically probed in the presence of hydrogen peroxide, demonstrating the stability and reactivity of bound curcumin. 相似文献
40.
A Vastly Increased Chemical Variety of RNA Modifications Containing a Thioacetal Structure 下载免费PDF全文
Christina Dal Magro Patrick Keller Dr. Annika Kotter Stephan Werner Dr. Victor Duarte Dr. Virginie Marchand Dr. Michael Ignarski Anja Freiwald Dr. Roman‐Ulrich Müller Prof. Dr. Christoph Dieterich Prof. Dr. Yuri Motorin Dr. Falk Butter Dr. Mohamed Atta Prof. Dr. Mark Helm 《Angewandte Chemie (International ed. in English)》2018,57(26):7893-7897
Recently discovered new chemical entities in RNA modifications have involved surprising functional groups that enlarge the chemical space of RNA. Using LC‐MS, we found over 100 signals of RNA constituents that contained a ribose moiety in tRNAs from E. coli. Feeding experiments with variegated stable isotope labeled compounds identified 37 compounds that are new structures of RNA modifications. One structure was elucidated by deuterium exchange and high‐resolution mass spectrometry. The structure of msms2i6A (2‐methylthiomethylenethio‐N6‐isopentenyl‐adenosine) was confirmed by methione‐D3 feeding experiments and by synthesis of the nucleobase. The msms2i6A contains a thioacetal, shown in vitro to be biosynthetically derived from ms2i6A by the radical‐SAM enzyme MiaB. This enzyme performs thiomethylation, forming ms2i6A from i6A in a first turnover. The new thioacetal is formed by a second turnover. Along with the pool of 36 new modifications, this work describes a new layer of RNA modification chemistry. 相似文献