Highly‐Exposed Single‐Interlayered Cu Edges Enable High‐Rate CO2‐to‐CH4 Electrosynthesis

Abstract The electrochemical CO 2 reduction to CH 4 is a promising approach for producing highly specific combustion fuel but has relatively poor selectivity and activity at high‐current‐density electrolysis. In this work, ultrathin CuGaO 2 nanosheets with highly exposed single‐interlayered Cu edges are synthesized via an induced anisotropic growth strategy. Density functional theory calculations indicate that the exposed single‐interlayered Cu(I) edges on the (001) surface of CuGaO 2 present a high‐density of single‐atomic Cu sites, which feature excellent CO 2 electroreduction catalytic activity toward CH 4 . The CuGaO 2 nanosheet catalysts exhibit efficient and stable CO 2 ‐to‐CH 4 electroreduction with Faradaic efficiency (FE CH4 ) of 71.7% at a high current density of –1 A cm −2 , corresponding to a superior CH 4 partial current density of 717 ± 33 mA cm −2 . This work suggests an attractive design strategy for tuning both the crystal facets and Cu–Cu distance to promote the CH 4 electrosynthesis at high‐current‐density CO 2 reduction.