Synthesis and electrochemical study of iron, chromium and tungsten aminocarbenes: Role of ligand structure and central metal nature
Several series of Fischer-type aminocarbene complexes with central Fe, Cr or W atoms and with various carbene substitution were synthesized and electrochemically investigated by dc-polarography and cyclic voltammetry. The shifts and changes of reduction and oxidation potentials were evaluated using...
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| Vydáno v: | Electrochimica acta Ročník 55; číslo 27; s. 8341 - 8351 |
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| Médium: | Journal Article Konferenční příspěvek |
| Jazyk: | angličtina |
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Kidlington
Elsevier Ltd
30.11.2010
Elsevier |
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| ISSN: | 0013-4686, 1873-3859 |
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| Abstract | Several series of Fischer-type aminocarbene complexes with central Fe, Cr or W atoms and with various carbene substitution were synthesized and electrochemically investigated by dc-polarography and cyclic voltammetry. The shifts and changes of reduction and oxidation potentials were evaluated using the linear free energy relationship (LFER) approach with respect to (a) the type of coordination, (b) the substitution on the carbene ligand and (c) the nature of the central metal atom. The analysis of measured data confirms that the reduction center is localized on the carbene moiety and is strongly influenced by both electronic and sterical properties of its substituents. The oxidation proceeds on the metal and depends mainly on its nature and on the π-acidity of the ligands. Electrochemistry thus represents an important experimental approach to the description and understanding of the molecular electronic structure and redox properties. Experimental results are supported by DFT calculation of HOMO and LUMO orbitals shape and composition. |
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| AbstractList | Several series of Fischer-type aminocarbene complexes with central Fe, Cr or W atoms and with various carbene substitution were synthesized and electrochemically investigated by dc-polarography and cyclic voltammetry. The shifts and changes of reduction and oxidation potentials were evaluated using the linear free energy relationship (LFER) approach with respect to (a) the type of coordination, (b) the substitution on the carbene ligand and (c) the nature of the central metal atom. The analysis of measured data confirms that the reduction center is localized on the carbene moiety and is strongly influenced by both electronic and sterical properties of its substituents. The oxidation proceeds on the metal and depends mainly on its nature and on the [pi]-acidity of the ligands. Electrochemistry thus represents an important experimental approach to the description and understanding of the molecular electronic structure and redox properties. Experimental results are supported by DFT calculation of HOMO and LUMO orbitals shape and composition. Several series of Fischer-type aminocarbene complexes with central Fe, Cr or W atoms and with various carbene substitution were synthesized and electrochemically investigated by dc-polarography and cyclic voltammetry. The shifts and changes of reduction and oxidation potentials were evaluated using the linear free energy relationship (LFER) approach with respect to (a) the type of coordination, (b) the substitution on the carbene ligand and (c) the nature of the central metal atom. The analysis of measured data confirms that the reduction center is localized on the carbene moiety and is strongly influenced by both electronic and sterical properties of its substituents. The oxidation proceeds on the metal and depends mainly on its nature and on the π-acidity of the ligands. Electrochemistry thus represents an important experimental approach to the description and understanding of the molecular electronic structure and redox properties. Experimental results are supported by DFT calculation of HOMO and LUMO orbitals shape and composition. |
| Author | Záliš, Stanislav Hoskovcová, Irena Dvořák, Dalimil Zvěřinová, Radka Ludvík, Jiří Tobrman, Tomáš Roháčová, Jana |
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| Cites_doi | 10.1002/cber.19731061213 10.1039/p19950001265 10.1016/S0022-328X(00)93302-3 10.1016/0022-328X(90)80112-D 10.1021/ol0342094 10.1021/ja00233a018 10.1007/BF00533485 10.1021/om00093a021 10.1021/om010533w 10.1016/j.electacta.2004.12.047 10.1063/1.476673 10.1021/om0605837 10.1016/j.jorganchem.2005.07.048 10.1021/jo00820a024 10.1039/dt9800002032 10.1021/om00011a022 10.1063/1.464913 10.1021/om00001a081 10.1103/PhysRevA.38.3098 |
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| Keywords | Voltammetry–polarography Fischer aminocarbene complexes LFER Structurally dependent redox properties HOMO–LUMO displacement Chromium Organic compounds Frontier orbital Chromium Carbonyl Complexes Orbital interaction Organic ligand Theoretical study Voltammetry Transition metal Carbonyl Complexes Tungsten Organic compounds Ylidene complex Iron Organic compounds Iron Carbonyl Complexes Electrochemical properties Polarography Aminocarbene Density functional method Property structure relationship HOMO-LUMO displacement Voltammetry-polarography Chemical synthesis Tungsten Carbonyl Complexes |
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| SubjectTerms | Carbenes Chemistry Chromium Electronics Exact sciences and technology Fischer aminocarbene complexes HOMO–LUMO displacement Iron LFER Ligands Molecular structure Orbitals Organic chemistry Organometalloidal and organometallic compounds Preparations and properties Reduction Structurally dependent redox properties Transition metals derivatives Voltammetry–polarography |
| Title | Synthesis and electrochemical study of iron, chromium and tungsten aminocarbenes: Role of ligand structure and central metal nature |
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