Abstract
The reduction of carbon dioxide into valuable chemical products is a promising solution to address carbon balance and energy issues. Herein, amorphous nitrided copper-iron oxides are prepared by gas-phase nitriding of CuFe-layered double hydroxide precursors with urea as a nitrogen source. The obtained materials show high activity for CO2 electroreduction to methane and formic acid, achieving a total Faraday efficiency of 74.7% at −0.7 V vs. RHE and exhibiting continuous 10 h durability in the H-cell. The uniformly distributed Cu+ sites act as active sites by losing electrons to activate CO2. During the CO2 electroreduction, CO2 is converted to *COOH via proton-electron coupling; *COOH combines directly with a proton in solution to produce the HCOOH product; and the other part of *COOH undergoes a protonated dehydration process to form the *CHO intermediate, which dehydrates again to form CH4. This study provides a new approach for designing CO2 electroreduction catalysts.
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