Selective and Stable CO2 Electroreduction to CH4 via Electronic Metal –Support Interaction upon Decomposition/Redeposition of MOF

A copper-based metal-organic framework is synthesized via a solvent-free method. Upon CO2 electroreduction, it undergoes in situ decomposition/redeposition to form abundant interfacial sites between copper nanoparticles and amorphous carbon supports, which stabilize the key intermediates for CH4 formation. Stable production of CH4 with Faradaic efficiency of ≈55% is achieved for 12.5 h. AbstractThe CO2 electroreduction to fuels is a feasible approach to provide renewable energy sources. Therefore, it is necessary to conduct experimental and theoretical investigations on various catalyst design strategies, such as electronic metal –support interaction, to improve the catalytic selectivity. Here a solvent-free synthesis method is reported to prepare a copper (Cu)-based metal–organic framework (MOF) as the precursor. Upon electrochemical CO2 reduction in aqueous electrolyte, it undergoes in situ decomposition/redeposition processes to form abundant interfaces between Cu nanoparticles and amorphous carbon supports. This Cu/C catalyst favors the selective and stable production of CH4 with a Faradaic efficiency of ≈55% at −1.4 V versus reversible hydrogen electrode (RHE) for 12.5 h. The density functional theory calculation reveals the crucial role of interfacial sites between Cu and amorphous carbon support in stabilizing the key intermediates for CO2 reduction to CH4. The adsorption of COOH* and CHO* at the Cu/C interface is up to 0.86  eV stronger than that on Cu(11...
Source: Small - Category: Nanotechnology Authors: Tags: Research Article Source Type: research