Modulating the Cu₂O Photoelectrode/Electrolyte Interface with Bilayer Surfactant Simulating Cell Membranes for...

The low solubility of CO₂ molecules and the competition of the hydrogen evolution reaction (HER) in aqueous electrolytes pose significant challenges to the current photoelectrochemical (PEC) CO₂ reduction reaction. In this study, inspired by the bilayer phospholipid molecular structure of cell membranes, we developed a Cu₂O/Sn photocathode that was modified with the bilayer surfactant DHAB for achieving high CO₂ permeability and suppressed HER. The Cu₂O/Sn/DHAB photocathode stabilizes the *OCHO intermediate and facilitates the production of HCOOH. Our findings show that the Faradaic efficiency (FE) of HCOOH by the Cu₂O/Sn/DHAB photoelectrode is 83.3%, significantly higher than that achieved with the Cu₂O photoelectrode (FE_HCOOH = 30.1%). Furthermore, the FE_H2 produced by the Cu₂O/Sn/DHAB photoelectrode is only 2.95% at -0.6 V vs RHE. The generation rate of HCOOH by the Cu₂O/Sn/DHAB photoelectrode reaches 1.52 mmol·cm^-2·h^-1·L^-1 at -0.7 V vs RHE. Our study provides a novel approach for the design of efficient photocathodes for CO₂ reduction.