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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(28):8323-8327
This study deals with the unprecedented reactivity of dinuclear non‐heme MnII–thiolate complexes with O2, which dependent on the protonation state of the initial MnII dimer selectively generates either a di‐μ‐oxo or μ‐oxo‐μ‐hydroxo MnIV complex. Both dimers have been characterized by different techniques including single‐crystal X‐ray diffraction and mass spectrometry. Oxygenation reactions carried out with labeled 18O2 unambiguously show that the oxygen atoms present in the MnIV dimers originate from O2. Based on experimental observations and DFT calculations, evidence is provided that these MnIV species comproportionate with a MnII precursor to yield μ‐oxo and/or μ‐hydroxo MnIII dimers. Our work highlights the delicate balance of reaction conditions to control the synthesis of non‐heme high‐valent μ‐oxo and μ‐hydroxo Mn species from MnII precursors and O2. 相似文献
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Katalytische Epoxidierung und 1,2‐Dihydroxylierung von Olefinen mit Bispidin‐Eisen(II)/H2O2‐Systemen
Michael R. Bukowski Peter Comba Achim Lienke Christian Limberg Carlos Lopez de Laorden Rubn Mas‐Ballest Michael Merz Lawrence Que 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2006,118(21):3524-3528
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(17):4923-4926
The first transition metal catalyzed hydrophosphination of isocyanates is presented. The use of low‐coordinate iron(II) precatalysts leads to an unprecedented catalytic double insertion of isocyanates into the P−H bond of diphenylphosphine to yield phosphinodicarboxamides [Ph2PC(=O)N(R)C(=O)N(H)R], a new family of derivatized organophosphorus compounds. This remarkable result can be attributed to the low‐coordinate nature of the iron(II) centers whose inherent electron deficiency enables a Lewis‐acid mechanism in which a combination of the steric pocket of the metal center and substrate size determines the reaction products and regioselectivity. 相似文献
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