Preferentially Stabilizing the Watershed Intermediates by Adsorbate‐adsorbate Interaction to Accelerate CO2 Electroreduction to Ethanol

Abstract

Returning CO2 to liquid ethanol powered by clean energy offers considerable economic benefits and contributes to reaching the goal of carbon neutrality, but it remains a formidable challenge to achieve high ethanol selectivity due to the inevitable strong competition among various pathways. Herein, an investigation is presented to accelerate CO2 electroreduction to ethanol via preferentially stabilizing the precarious watershed intermediates (*CHCOH) by creating strong adsorbate‐adsorbate interaction. The highly ordered CuOx nanoplates (HO‐CuOx NPLs) featuring abundant amorphous‐crystalline interface exhibit an exceptional ethanol Faradaic efficiency (FEEtOH) of 63.8% and an ethanol‐to‐ethylene ratio of 6.1 at a large ethanol partial current density (jethanol) of 232.8 mA cm−2. The findings decipher that abundant in‐between nanogaps in the amorphous‐crystalline interface enhance the adsorption of *OH, which can preferentially strengthen C─O bonds while weakening the Cu─C interaction of *CHCOH through adsorbate‐adsorbate interaction, thereby enabling a predilection for CO2 to ethanol conversion. Beyond an efficient ethanol‐oriented CO2RR electrocatalyst, the investigations provide an in‐depth understanding of adsorbate‐adsorbate interaction on key CO2RR steps and precise intermediates regulation, which can be extended to a range of energy conversion technologies.