Repurposing a Bio-Inspired NiFe Hydrogenase Model for CO2 Reduction with Selective Production of Methane as the Unique C-Based Product - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue ACS Energy Letters Année : 2020

Repurposing a Bio-Inspired NiFe Hydrogenase Model for CO2 Reduction with Selective Production of Methane as the Unique C-Based Product

Résumé

In the current environmental and economic context, there is an urgent need to develop catalytic systems to efficiently activate and transform abundant small molecules while demonstrating selectivity when multielectron processes are involved. This is especially true for catalytic production of CH4 from CO2, as a limited number of active photo- or electro-catalysts have been described to date. Herein, we report the unprecedented reactivity of a molecular electrocatalyst physiadsorbed on a graphite electrode: the bioinspired [(LNiFeCp)-Ni-N2S2-Fe-II-Cp-II(CO)]+ (L-N2S2 = 2,2'-(2,2'-bipryridine-6,6'-diyl)bis- (1,1'-diphenylethanethiolate) complex selectively and catalytically reduces CO2 in acidic aqueous solution to produce a mixture of CH4 and H-2. Under optimized conditions, at pH 4, Faradaic yields of 12% and 66% for CH4 and H-2 production (TOFCH4 = 214 s(-1), TOFH2 approximate to 5.1 x 10(3) s(-1)) are measured, respectively. We demonstrate that this binuclear NiFe catalyst is stable for hours under controlled potential electrolysis conditions.

Domaines

Catalyse
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Dates et versions

hal-03100365 , version 1 (18-10-2022)

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Md Estak Ahmed, Suzanne Adam, Dibyajyoti Saha, Jennifer Fize, Vincent Artero, et al.. Repurposing a Bio-Inspired NiFe Hydrogenase Model for CO2 Reduction with Selective Production of Methane as the Unique C-Based Product. ACS Energy Letters, 2020, 5 (12), pp.3837-3842. ⟨10.1021/acsenergylett.0c02002⟩. ⟨hal-03100365⟩
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