Efficient CO2 electroreduction (CO2RR) 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 CO2 reduction predilection switch from ethylene to ethanol (ethanol-to-ethylene ratio of ~5.4) by inherently implanting Cu sites with perfluorooctane to create interfacial non-covalent interactions. The 1.83%F-Cu2O organic-inorganic hybrids (OIHs) exhibited an extraordinary ethanol faradaic efficiency (FEethanol) 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-Cu2O OIHs among the best-performing ethanol-oriented CO2RR electrocatalysts. Our findings identified that C8F18 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 CO2 electroreduction to ethanol, bringing it closer to practical implementation requirements.

中文翻译：

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通过用全氟辛烷植入 Cu 位点来调节界面氢键网络，以加速 CO2 电还原为乙醇


高效的 CO2 电还原 （CO2RR） 制乙醇有望同时产生增值化学品并利用可再生能源。然而，由于与热力学上更优选的乙烯生产的竞争，这仍然是一个持续的挑战。在此，我们提出了一种从乙烯到乙醇的 CO2 还原偏好转换（乙醇与乙烯的比率为 ~5.4），方法是在铜位点上植入全氟辛烷以产生界面非共价相互作用。1.83%F-Cu2O 有机-无机杂化物 （OIH） 表现出 ∼55.2% 的非凡乙醇法拉第效率 （FEethanol），具有令人印象深刻的 166 mA cm-2 乙醇部分电流密度，并且在连续运行 60 小时内具有出色的稳健性。这种卓越的性能使我们的 1.83%F-Cu2O OIH 成为性能最佳的乙醇导向型 CO2RR 电催化剂之一。我们的研究发现，C8F18 可以加强界面氢键连接，从而促进活性氢种类的产生，并优先有利于 *CHCOH 氢化为 *CHCHOH，从而将反应从乙烯优选反应转变为乙醇导向反应。所提出的研究强调了使用非共价相互作用来调节 CO2 电还原为乙醇的选择性的机会，使其更接近实际实施要求。