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Abstract Efficient CO 2 electroreduction (CO 2 RR) to ethanol holds promise to generate value‐added chemicals and harness renewable energy simultaneously. Yet, it remains an ongoing challenge due to the competition with thermodynamically more preferred ethylene production. Herein, we presented a CO 2 reduction predilection switch from ethylene to ethanol (ethanol‐to‐ethylene ratio of ~5.4) by inherently implanting Cu sites with perfluorooctane to create interfacial noncovalent interactions. The 1.83 %F‐Cu 2 O organic–inorganic hybrids (OIHs) exhibited an extraordinary ethanol faradaic efficiency (FE ethanol ) of ∼55.2 %, with an impressive ethanol partial current density of 166 mA cm −2 and excellent robustness over 60 hours of continuous operation. This exceptional performance ranks our 1.83 %F‐Cu 2 O OIHs among the best‐performing ethanol‐oriented CO 2 RR electrocatalysts. Our findings identified that C 8 F 18 could strengthen the interfacial hydrogen bonding connectivity, which consequently promotes the generation of active hydrogen species and preferentially favors the hydrogenation of *CHCOH to *CHCHOH, thus switching the reaction from ethylene‐preferred to ethanol‐oriented. The presented investigations highlight opportunities for using noncovalent interactions to tune the selectivity of CO 2 electroreduction to ethanol, bringing it closer to practical implementation requirements.
Zhou et al. (Tue,) studied this question.