Reversible transition of an amorphous Cu-Al oxyfluoride into a highly active electrocatalyst for NO3−reduction to NH3

Autor: Guiet, Amandine, Simonin, Alexandre, Bemana, Hossein, Al-Mahayni, Hasan, Li, Junnan, Kuruvinashetti, Kiran, Moury, Romain, Hémon-Ribaud, Annie, Chartrand, Daniel, Maisonneuve, Vincent, Lhoste, Jérôme, Seifitokaldani, Ali, Rochefort, Dominic, Kornienko, Nikolay
Zdroj: Chem Catalysis; May 2023, Vol. 3 Issue: 5
Abstrakt: The electrochemical conversion of NO3−to NH3is an emerging route to an essential chemical feedstock and potential fuel. Underpinning the field’s development is the discovery of efficient electrocatalysts and insights into the reaction mechanism. To this end, a Cu-based oxyfluoride, Cu3Al2OF10, prepared through a facile co-precipitation and annealing of the corresponding hydrated fluoride r-Cu3Al2F12(H2O)12, was found to be exceptionally active, attaining a NH3Faradaic efficiency (FE) of up to 57% for the 8-electron NO3−to NH3pathway (−0.4 VRHE) with a mass activity of up to 1220 A.g−1at −0.6 VRHE. Electroanalytical and operandospectroscopic investigations revealed a reversible transition to a phase entailing Cu nanoparticles embedded within the amorphous oxyfluoride matrix that was predominantly responsible for the catalyst’s activity. Overall, this work stands to open avenues for transition metal fluoride materials within the field of N-based electrocatalysis.
Databáze: Supplemental Index