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排序方式: 共有139条查询结果,搜索用时 15 毫秒
51.
Mark John P. Mandigma Jonas
urauskas Callum I. MacGregor Lee J. Edwards Ahmed Shahin Ludwig d'Heureuse Philip Yip David J. S. Birch Thomas Gruber Jrg Heilmann Matthew P. John Joshua P. Barham 《Chemical science》2022,13(7):1912
We report an organophotocatalytic, N–CH3-selective oxidation of trialkylamines in continuous flow. Based on the 9,10-dicyanoanthracene (DCA) core, a new catalyst (DCAS) was designed with solubilizing groups for flow processing. This allowed O2 to be harnessed as a sustainable oxidant for late-stage photocatalytic N–CH3 oxidations of complex natural products and active pharmaceutical ingredients bearing functional groups not tolerated by previous methods. The organophotocatalytic gas–liquid flow process affords cleaner reactions than in batch mode, in short residence times of 13.5 min and productivities of up to 0.65 g per day. Spectroscopic and computational mechanistic studies showed that catalyst derivatization not only enhanced solubility of the new catalyst compared to poorly-soluble DCA, but profoundly diverted the photocatalytic mechanism from singlet electron transfer (SET) reductive quenching with amines toward energy transfer (EnT) with O2.An N–CH3-selective trialkylamine oxidation to N-formamides is reported in continuous flow using gaseous O2. A novel, enhanced-solubility dicyanoanthracene organophotocatalyst switched the photochemical mechanism from electron to energy transfer. 相似文献
52.
Najeeb Ur Rehman Mohd Nazam Ansari Abdul Samad Wasim Ahmad 《Molecules (Basel, Switzerland)》2022,27(4)
Fenchone is a bicyclic monoterpene found in a variety of aromatic plants, including Foeniculum vulgare and Peumus boldus, and is used in the management of airways disorders. This study aimed to explore the bronchodilator effect of fenchone using guinea pig tracheal muscles as an ex vivo model and in silico studies. A concentration-mediated tracheal relaxant effect of fenchone was evaluated using isolated guinea pig trachea mounted in an organ bath provided with physiological conditions. Sustained contractions were achieved using low K+ (25 mM), high K+ (80 mM), and carbamylcholine (CCh; 1 µM), and fenchone inhibitory concentration–response curves (CRCs) were obtained against these contractions. Fenchone selectively inhibited with higher potency contractions evoked by low K+ compared to high K+ with resultant EC50 values of 0.62 mg/mL (0.58–0.72; n = 5) and 6.44 mg/mL (5.86–7.32; n = 5), respectively. Verapamil (VRP) inhibited both low and high K+ contractions at similar concentrations. Pre-incubation of the tracheal tissues with K+ channel blockers such as glibenclamide (Gb), 4-aminopyridine (4-AP), and tetraethylammonium (TEA) significantly shifted the inhibitory CRCs of fenchone to the right towards higher doses. Fenchone also inhibited CCh-mediated contractions at comparable potency to its effect against high K+ [6.28 mg/mL (5.88–6.42, n = 4); CCh] and [6.44 mg/mL (5.86–7.32; n = 5); high K+]. A similar pattern was obtained with papaverine (PPV), a phosphodiesterase (PDE), and Ca2+ inhibitor which inhibited both CCh and high K+ at similar concentrations [10.46 µM (9.82–11.22, n = 4); CCh] and [10.28 µM (9.18–11.36; n = 5); high K+]. However, verapamil, a standard Ca2+ channel blocker, showed selectively higher potency against high K+ compared to CCh-mediated contractions with respective EC50 values of 0.84 mg/mL (0.82–0.96; n = 5) 14.46 mg/mL (12.24–16.38, n = 4). The PDE-inhibitory action of fenchone was further confirmed when its pre-incubation at 3 and 5 mg/mL potentiated and shifted the isoprenaline inhibitory CRCs towards the left, similar to papaverine, whereas the Ca2+ inhibitory-like action of fenchone pretreated tracheal tissues were authenticated by the rightward shift of Ca2+ CRCs with suppression of maximum response, similar to verapamil, a standard Ca2+ channel blocker. Fenchone showed a spasmolytic effect in isolated trachea mediated predominantly by K+ channel activation followed by dual inhibition of PDE and Ca2+ channels. Further in silico molecular docking studies provided the insight for binding of fenchone with Ca2+ channel (−5.3 kcal/mol) and K+ channel (−5.7), which also endorsed the idea of dual inhibition. 相似文献
53.
M. Wasim A. Rahman J. H. Zaidi S. Waheed S. Ahmad 《Journal of Radioanalytical and Nuclear Chemistry》2002,254(1):219-222
The proposed reference material from the International Atomic Energy Agency, namely IAEA-407 (Fish Homogenate) was analyzed using instrumental neutron activation analysis (INAA). 15 elements, Al, As, Cl, Co, Cr, Fe, Hg, Mg, Mn, K, Na, Sb, Se, V and Zn, were determined using two irradiations (5 minutes and 5 hours) and four countings. IAEA-MA-A-1/TM (Copepoda Homogenate), NIST-SRM-1566 (Oyster Tissue), NIST-SRM-1572 (Citrus Leaves) and NIST-SRM-1577a (Bovine Liver) were utilized as standards in the quantification step. 相似文献
54.
From a combined analysis of the stoichiometric composition and Urbach tail in samples of CuInSe2, CuInTe2, and CuGaTe2 of the I-III-VI2 family of chalcopyrite semiconductors, it is found that the energy hνp involved in the electron/exciton-phonon interaction is a linear function of a parameter Δz which is the sum of the deviations from ideal molecularity Δx and anion to cation ratio Δy. It gives evidence that in the copper ternaries hνp is associated to the structural defects caused by cation-cation, cation-anion, and other intrinsic disorders. The high value of hνp found in the studied samples, higher than the highest optical mode, is shown to come from the contribution of the additional phonon energy due to structural defects. This is in agreement with recently proposed models of the temperature dependence of the Urbach energy. 相似文献
55.
Double Deprotonation of Pyridinols Generates Potent Organic Electron‐Donor Initiators for Haloarene–Arene Coupling 下载免费PDF全文
Joshua P. Barham Dr. Graeme Coulthard Ryan G. Kane Nathan Delgado Dr. Matthew P. John Prof. Dr. John A. Murphy 《Angewandte Chemie (International ed. in English)》2016,55(14):4492-4496
Transition metal‐free couplings of haloarenes with arenes, triggered by the use of alkali metal alkoxides in the presence of an organic additive, are receiving significant attention in the literature. Most of the known organic additives effect coupling of iodoarenes, but not bromoarenes, to arenes. Recently it was reported that 2‐pyridinecarbinol ( 11 ) extends the reaction to aryl bromides. This paper investigates the mechanism, and reports evidence for dianions derived from 11 as electron donors to initiate the reaction. It also proposes routes by which electron‐poor benzoyl derivatives can be transformed into electron donors to initiate these reactions. 相似文献
56.
Yanhui Zhang Hao Teng Ying Gao Muhammad Wasim Afzal Jingye Tian Xi Chen Haoyang Tang Tony D. James Yuan Guo 《中国化学快报》2021,31(11):2917-2920
Triazolopyridines are an important kind of fused-ring compounds. A HOCl-promoted triazolopyridine formation strategy is reported here for the first time in which hypochlorous acid (HOCl) mildly and efficiently promotes the formation of 1,2,4-triazolo[4,3-a]pyridines NT1-NT6 from various 2-pyridylhydrazones N1-N6. N6, a rhodol-pyridylhydrazone hybrid, was developed into a fluorescent probe for the selective detection of HOCl, and successfully applied to probe endogenous HOCl in living cells and zebrafish in situ and in real time. The present intramolecular cyclization reaction is selective and atom-economical, thereby not only providing an important approach for the convenient synthesis of triazolopyridines, but also offering a general strategy for sensitive, selective and biocompatible detection of endogenous HOCl in complex biosystems. 相似文献
57.
M. Wasim W. A. Zafar M. Tufail M. Arif M. Daud A. Ahmad 《Journal of Radioanalytical and Nuclear Chemistry》2011,287(3):821-826
To study the impurity elements, which render color-induced topaz long lived radionuclides, three samples of topaz, from three
different cities of the Northern Pakistan (Baltistan, Gilgit and Mardan) were analyzed using k
0 instrumental neutron activation analysis (k
0-INAA). The samples were irradiated in Pakistan Research Reactor-1 (PARR-1) and PARR-2 at Pakistan Institute of Nuclear Science
& Technology (PINSTECH), Islamabad. The method was validated by analyzing IAEA-S7 reference material. In three samples a total
of 22 trace level impurity elements were quantified. Among impurities, 10 elements including As, Ce, Ga, Ge, La, Na, Sb, Sc,
U and Zn were common in topaz of all the three places. The storage time has been calculated for each sample required to bring
the induced radioactivity down to permissible level given by US National Regulatory Commission. 相似文献
58.
Wasiq Ali Yaan Li Muhammad Asif Zahoor Raja Wasim Ullah Khan Yigang He 《Entropy (Basel, Switzerland)》2021,23(9)
In this study, an application of deep learning-based neural computing is proposed for efficient real-time state estimation of the Markov chain underwater maneuvering object. The designed intelligent strategy is exploiting the strength of nonlinear autoregressive with an exogenous input (NARX) network model, which has the capability for estimating the dynamics of the systems that follow the discrete-time Markov chain. Nonlinear Bayesian filtering techniques are often applied for underwater maneuvering state estimation applications by following state-space methodology. The robustness and precision of NARX neural network are efficiently investigated for accurate state prediction of the passive Markov chain highly maneuvering underwater target. A continuous coordinated turning trajectory of an underwater maneuvering object is modeled for analyzing the performance of the neural computing paradigm. State estimation modeling is developed in the context of bearings only tracking technology in which the efficiency of the NARX neural network is investigated for ideal and complex ocean environments. Real-time position and velocity of maneuvering object are computed for five different cases by varying standard deviations of white Gaussian measured noise. Sufficient Monte Carlo simulation results validate the competence of NARX neural computing over conventional generalized pseudo-Bayesian filtering algorithms like an interacting multiple model extended Kalman filter and an interacting multiple model unscented Kalman filter. 相似文献
59.
Lisa Wirtz Wasim Haider Dr. Volker Huch Dr. Michael Zimmer Dr. André Schäfer 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(28):6176-6184
The Lewis acidities of a series of [n]magnesocenophanes ( 1 a – d ) have been investigated computationally and found to be a function of the tilt of the cyclopentadienyl moieties. Their catalytic abilities in amine borane dehydrogenation/dehydrocoupling reactions have been probed, and C[1]magnesocenophane ( 1 a ) has been shown to effectively catalyze the dehydrogenation/dehydrocoupling of dimethylamine borane ( 2 a ) and diisopropylamine borane ( 2 b ) under ambient conditions. Furthermore, the mechanism of the reaction with 2 a has been investigated experimentally and computationally, and the results imply a ligand-assisted mechanism involving stepwise proton and hydride transfer, with dimethylaminoborane as the key intermediate. 相似文献
60.
Dieter Seebach H. Michael Bürger Hans-Martin Müller Urs D. Lengweiler Albert K. Beck Kathy E. Sykes Phil A. Barker Peter J. Barham 《Helvetica chimica acta》1994,77(4):1099-1123
Repetitive treatment of the biopolymer P(3-HB) (molecular weight > 105 Dalton, storage or s-P(3-HB)), with lithium hexamethyl disilazanid (LHMDS) at ?70° in THF leads to a mixture of oligomers with increasingly sharp distribution around a 15-, 30-, and 45mer. Discrete fragments are also isolated when P(3-HB) is heated under reflux (89°) in neat Et3N. Linear oligo(3-HB) derivatives ( 3-7 ) containing up to 96 3-HB units are synthesized using an exponential segment-coupling strategy. These oligomers are used to calibrate size-exclusion chromatography columns for the analysis of oligo(3-HB) samples from the different sources. The linear oligo-(3-HB) derivatives also served as a model with respect to the physical properties of high molecular weight P(3-HB) and were investigated as such by transmission electron microscopy (TEM) and by small- and wide-angle X-ray scattering (SAXS and WAXS). The thicknesses of the lamellar crystallites (long periods) formed by the 8mer, 16mer, and 32mer, are ca. 26, 52, and 53 Å, respectively, indicating that the 32mer molecules are folded once, very tightly, into a ‘hair-pin’-type conformation. High-molecular-weight P(3-HB), which was crystallized in a similar way, also has a lamellar crystallite thickness of ca. 50–65 Å. Thus, the treatment of P(3-HB) with LHMDS at low temperature causes etching of the amorphous regions, an effect well known in polymer science for studying the regularity of chain folding. The ca. 50-Å packing within the tight folds of P(3-HB) is discussed in view of its possible function in ion transport through cell membranes. 相似文献