The electrochemical reduction of carbon dioxide (CO2RR) is a viable route for the transformation of intermittent renewable energy into high energy density chemical vectors (e.g. CO) or into fuels. Differently from metal nanoparticle electrocatalysts, the use of organometallic molecular complexes affords more efficient metal utilization, limits poisoning phenomena and allows the tuning of selectivity by varying the electronic and coordination properties of the metal center. Herein the organometallic complex (fac-Mn(apbpy)(CO)3Br) (apbpy = 4-(4-aminophenyl)-2,2'-bipyridine) was covalently anchored on a gas diffusion layer which was further employed as cathode in an aqueous gas-liquid interface complete electrolysis flow cell microreactor. The decorated gas diffusion layer electrode was able to convert CO2 into CO and HCOOH with faradaic efficiencies (FE) of 76% and 10% with a CO-productivity close to 70 Nl min-1 gMn-1 reaching CO2RR turnover numbers up to 1.6·105.This result largely outperforms a state-of-the-art gold nanoparticle electrocatalyst (Au/C 10 wt%) operating in the same cell conditions
Turning Manganese into Gold: efficient electrochemical CO2 reduction by a fac-Mn(apbpy)(CO)3Br complex in a gas-liquid interface flow cell
Jonathan Filippi;Hamish A. Miller;Alessandro Lavacchi;Francesco Vizza
2021
Abstract
The electrochemical reduction of carbon dioxide (CO2RR) is a viable route for the transformation of intermittent renewable energy into high energy density chemical vectors (e.g. CO) or into fuels. Differently from metal nanoparticle electrocatalysts, the use of organometallic molecular complexes affords more efficient metal utilization, limits poisoning phenomena and allows the tuning of selectivity by varying the electronic and coordination properties of the metal center. Herein the organometallic complex (fac-Mn(apbpy)(CO)3Br) (apbpy = 4-(4-aminophenyl)-2,2'-bipyridine) was covalently anchored on a gas diffusion layer which was further employed as cathode in an aqueous gas-liquid interface complete electrolysis flow cell microreactor. The decorated gas diffusion layer electrode was able to convert CO2 into CO and HCOOH with faradaic efficiencies (FE) of 76% and 10% with a CO-productivity close to 70 Nl min-1 gMn-1 reaching CO2RR turnover numbers up to 1.6·105.This result largely outperforms a state-of-the-art gold nanoparticle electrocatalyst (Au/C 10 wt%) operating in the same cell conditionsFile | Dimensione | Formato | |
---|---|---|---|
prod_446307-doc_160419.pdf
Open Access dal 21/02/2023
Descrizione: “This document is the Accepted Manuscript version of a Published Work that appeared in final form in https://doi.org/10.1016/j.cej.2021.129050.”
Tipologia:
Documento in Post-print
Licenza:
Creative commons
Dimensione
4.95 MB
Formato
Adobe PDF
|
4.95 MB | Adobe PDF | Visualizza/Apri |
Chemical Engineering Journal 416 (2021) 129050.pdf
solo utenti autorizzati
Tipologia:
Versione Editoriale (PDF)
Licenza:
NON PUBBLICO - Accesso privato/ristretto
Dimensione
3.41 MB
Formato
Adobe PDF
|
3.41 MB | Adobe PDF | Visualizza/Apri Richiedi una copia |
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.