Graceful choreography for CO ₂ and H ₂ O: One challenge for efficient electrochemical reduction of carbon dioxide (CO ₂ ) is that the gas is hydrophobic, but many of its desirable reactions require water (H ₂ O). García de Arquer et al. addressed this problem by combining a copper electrocatalyst with an ionomer assembly that intersperses sulfonate-lined paths for the H ₂ O with fluorocarbon channels for the CO ₂ . The electrode architecture enables production of two-carbon products such as ethylene and ethanol at current densities just over an ampere per square centimeter. Science , this issue p. 661

Producing liquid fuels such as ethanol from CO₂, H₂O, and renewable electricity offers a route to store sustainable energy. The search for efficient electrocatalysts for the CO₂ reduction reaction relies on tuning the adsorption strength of carbonaceous intermediates. Here, we report a complementary approach in which we utilize hydroxide and oxide doping of a catalyst surface to tune the adsorbed hydrogen on Cu. Density functional theory studies indicate that this doping accelerates water dissociation and changes the hydrogen adsorption energy on Cu. We synthesize and investigate a suite of metal-hydroxide-interface-doped-Cu catalysts, and find that the most efficient, Ce(OH)_x-doped-Cu, exhibits an ethanol Faradaic efficiency of 43% and a partial current density of 128 mA cm⁻². Mechanistic studies, wherein we combine investigation of hydrogen evolution performance with the results of operando Raman spectroscopy, show that adsorbed hydrogen hydrogenates surface *HCCOH, a key intermediate whose fate determines branching to ethanol versus ethylene.