Re(I) NHC Complexes for Electrocatalytic Conversion of CO2
| Autor: | George Majetich, Charles J. Stanton, Henry F. Schaefer, Tong Jin, Jonathon E. Vandezande, Jay Agarwal, Clifford P. Kubiak, Charles W. Machan, Gonghu Li |
|---|---|
| Rok vydání: | 2016 |
| Předmět: |
010405 organic chemistry
Infrared 010402 general chemistry 01 natural sciences 0104 chemical sciences Inorganic Chemistry Metal chemistry.chemical_compound chemistry Yield (chemistry) visual_art visual_art.visual_art_medium Physical chemistry Density functional theory Chelation Physical and Theoretical Chemistry Cyclic voltammetry Carbene Faraday efficiency |
| Zdroj: | Inorganic chemistry. 55(6) |
| ISSN: | 1520-510X |
| Popis: | The modular construction of ligands around an N-heterocyclic carbene building block represents a flexible synthetic strategy for tuning the electronic properties of metal complexes. Herein, methylbenzimidazolium-pyridine and methylbenzimidazolium-pyrimidine proligands are constructed in high yield using recently established transition-metal-free techniques. Subsequent chelation to ReCl(CO)5 furnishes ReCl(N-methyl-N′-2-pyridylbenzimidazol-2-ylidine)(CO)3 and ReCl(N-methyl-N′-2-pyrimidylbenzimidazol-2-ylidine)(CO)3. These Re(I) NHC complexes are shown to be capable of mediating the two-electron conversion of CO2 following one-electron reduction; the Faradaic efficiency for CO formation is observed to be >60% with minor H2 and HCO2H production. Data from cyclic voltammetry is presented and compared to well-studied ReCl(2,2′-bipyridine)(CO)3 and MnBr(2,2′-bipyridine)(CO)3 systems. Results from density functional theory computations, infrared spectroelectrochemistry, and chemical reductions are also discussed. |
| Databáze: | OpenAIRE |
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