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Abstract
Copper-based materials can reliably convert carbon dioxide into multi-carbon products but they suffer from poor activity and product selectivity. The atomic structure-activity relationship of electrocatalysts for the selectivity is controversial due to the lacking of systemic multiple dimensions for operando condition study. Herein, we synthesized high-performance CO2RR catalyst comprising of CuO clusters supported on N-doped carbon nanosheets, which exhibited high C2+ products Faradaic efficiency of 73% including decent ethanol selectivity of 51% with a partial current density of 14.4 mA/cm−2 at −1.1 V vs. RHE. We evidenced catalyst restructuring and tracked the variation of the active states under reaction conditions, presenting the atomic structure-activity relationship of this catalyst. Operando XAS, XANES simulations and Quasi-in-situ XPS analyses identified a reversible potential-dependent transformation from dispersed CuO clusters to Cu2-CuN3 clusters which are the optimal sites. This cluster can’t exist without the applied potential. The N-doping dispersed the reduced Cun clusters uniformly and maintained excellent stability and high activity with adjusting the charge distribution between the Cu atoms and N-doped carbon interface. By combining Operando FTIR and DFT calculations, it was recognized that the Cu2-CuN3 clusters displayed charge-asymmetric sites which were intensified by CH3* adsorbing, beneficial to the formation of the high-efficiency asymmetric ethanol.
Highlights
Copper-based materials can reliably convert carbon dioxide into multi-carbon products but they suffer from poor activity and product selectivity
The linear sweep voltammetry (LSV) curves demonstrated that the activity of Cu/ N0.14C was better than other contrast samples with maximum current density
The nanosheet structure was further confirmed by atomic force microscopy (AFM), and the corresponding height profiles of the scans showed a thickness of about 0.6 nm (Supplementary Fig. 2)
Summary
Copper-based materials can reliably convert carbon dioxide into multi-carbon products but they suffer from poor activity and product selectivity. The prepared Cu/N0.14C catalyst with appropriate nitrogen content displayed high C2+ products Faradaic efficiency of 73% which includes ethanol FE of 51% at the potential of −1.1 V vs RHE with a current density of −14.4 mA/cm−2 in 0.1 M KHCO3 electrolyte It exhibited superb longterm CO2 electroreduction durability over 10 h. The well-defined self-reconstruction for the active sites of Cu/N0.14C facilitate the in-depth mechanistic understandings from complementary Operando Spectroscopy (XAS, XPS and FTIR), XANES simulations and theoretical calculations to present the atomic structureactivity relationship between the ethanol selectivity and in situ dynamic structure (local structure, electronic structure and the adsorbed intermediates), that would benefit the recognition for the CO2RR process
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