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51.
Paneque M Poveda ML Carmona E Salazar V 《Dalton transactions (Cambridge, England : 2003)》2005,(8):1422-1427
The bulky 2,5-dimethylthiophene (2,5-Me2T) reacts at 60 degrees C with TpMe2Ir(C2H4)2 to give a mixture of two TpMe2Ir(III) hydride products, 3 and 4, that contain in addition a thienyl (3) or a thienyl-derived ligand (4). For the generation of 3 only sp2 C-H activation is needed, but the formation of 4 requires also the activation of an sp3 C-H bond and the formation of a new C-C bond (between vinyl and thienyl fragments). In the presence of 2,5-Me2T, compound 4 reacts further to produce a complex thiophenic structure (5, characterized by X-ray methods) that derives formally from two molecules of 2,5-Me2T and a vinyl fragment. Compounds 3-5 can be readily protonated by [H(OEt2)2][BAr'4](Ar'= 3,5-C6H3(CF3)2), with initial generation of carbene ligands (in the case of 3 and 5) as a consequence of H+ attack at the beta-carbon of the Ir-thienyl unit. Free, substituted thiophenes, derived from the original 2,5-Me2T, may be isolated in this way. 相似文献
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Dr. Salvador Conejero Dr. Joaquín López‐Serrano Prof. Dr. Margarita Paneque Dr. Ana Petronilho Prof. Dr. Manuel L. Poveda Florencia Vattier Dr. Eleuterio Álvarez Prof. Dr. Ernesto Carmona 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(15):4644-4664
The complex [TpMe2Ir(C6H5)2(N2)] reacts with several 2‐substituted pyridines to generate N‐heterocyclic carbenes resulting from a formal 1,2‐hydrogen shift from C6 to N. In this paper we provide a detailed report of the scope and the mechanistic aspects (both experimental and theoretical) of the tautomerisation of 2‐substituted pyridines. 相似文献
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Alvarez E Conejero S Paneque M Petronilho A Poveda ML Serrano O Carmona E 《Journal of the American Chemical Society》2006,128(40):13060-13061
Steric strains (F-strain or front-strain) in the acid-base interaction between the Lewis acid [TpMe2Ir(C6H5)2] and 2-substituted pyridines Lewis bases, are responsible for the stabilization of the C-adducts (2) of the respective pyridine carbene tautomers over the expected N-adducts. 相似文献
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Dr. Sha Zhu Dr. Yerri Jagadeesh Dr. Anh Tuan Tran Dr. Shuki Imaeda Dr. Alisdair Boraston Dr. Dominic S. Alonzi Dr. Ana Poveda Dr. Yongmin Zhang Dr. Jérôme Désiré Dr. Julie Charollais-Thoenig Dr. Stéphane Demotz Prof. Atsushi Kato Dr. Terry D. Butters Prof. Jesús Jiménez-Barbero Prof. Matthieu Sollogoub Prof. Yves Blériot 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(44):11291-11297
Mucopolysaccharidosis type IIIB is a devastating neurological disease caused by a lack of the lysosomal enzyme, α-N-acetylglucosaminidase (NAGLU), leading to a toxic accumulation of heparan sulfate. Herein we explored a pharmacological chaperone approach to enhance the residual activity of NAGLU in patient fibroblasts. Capitalizing on the three-dimensional structures of two modest homoiminosugar-based NAGLU inhibitors in complex with bacterial homolog of NAGLU, CpGH89, we have synthesized a library of 17 iminosugar C-glycosides mimicking N-acetyl-D-glucosamine and bearing various pseudo-anomeric substituents of both α- and β-configuration. Elaboration of the aglycon moiety results in low micromolar selective inhibitors of human recombinant NAGLU, but surprisingly it is the non-functionalized and wrongly configured β-homoiminosugar that was proved to act as the most promising pharmacological chaperone, promoting a 2.4 fold activity enhancement of mutant NAGLU at its optimal concentration. 相似文献