Article: Carbon neutral electrochemical conversion of carbon dioxide mediated by [Mn+(cyclam)Cln] (M = Ni2+ and Co3+) on mercury free electrodes and ionic liquids as reaction media
Green chemistry. 2017 Feb. 21, v. 19, no. 4
2017
Abstract: In this work, the electrochemical reduction of carbon dioxide using [Mn+(cyclam)Cln] (M = Ni2+ and ... parameters, such as a heterogeneous electron transfer rate was calculated. Results indicate a faster M(ii)/M ...
Abstract | In this work, the electrochemical reduction of carbon dioxide using [Mn+(cyclam)Cln] (M = Ni2+ and Co3+) as electrocatalysts has been studied in 1-butyl-3-methylimidazolium tetrafluoroborate and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (BMImBF4 and BMImNTf2 respectively) ionic liquids as reaction media. Complexes were characterized electrochemically in these salts and relevant parameters, such as a heterogeneous electron transfer rate was calculated. Results indicate a faster M(ii)/M(i) redox process in BMImBF4 despite its higher viscosity compared to BMImNTF2. Cyclic voltammetry experiments demonstrated that [Ni(cyclam)Cl2] is the most active macrocycle, towards the reaction under survey. For this compound, potential controlled electrolysis was carried out at−1.4 V vs. Ag/AgCl in BMImBF4 as a solvent, yielding only CO as a reaction product, with a turnover frequency (TOF) of 0.73 h−1. NMR spectra for the ionic liquids, after electrolysis, show that the applied potential does not affect the chemical structure of the salts. FT-IR thin layer spectroelectrochemical experiments in CO2 saturated solution in BMImBF4 at −1.4 V vs. Ag/AgCl show the formation of [Ni(cyclam)CO]+ as precursor species, and also the most stable [Ni(CO)4]. |
---|---|
Keywords | Fourier transform infrared spectroscopy ; carbon ; carbon dioxide ; carbon monoxide ; catalysts ; chemical structure ; cobalt ; electrochemistry ; electrodes ; electrolysis ; electron transfer ; green chemistry ; ionic liquids ; mercury ; nickel ; nuclear magnetic resonance spectroscopy ; silver ; silver chloride ; surveys ; viscosity |
Language | English |
Dates of publication | 2017-0221 |
Size | p. 1155-1162. |
Publishing place | The Royal Society of Chemistry |
Document type | Article |
ZDB-ID | 2006274-6 |
ISSN | 1463-9270 ; 1463-9262 |
ISSN (online) | 1463-9270 |
ISSN | 1463-9262 |
DOI | 10.1039/c6gc02599d |
Database | NAL-Catalogue (AGRICOLA) |
More links
Kategorien
Order via subito
This service is chargeable due to the Delivery terms set by subito. Orders including an article and supplementary material will be classified as separate orders. In these cases, fees will be demanded for each order.