Presently, realizing high ethanol selectivity in CO₂ electroreduction remains challenging due to difficult C–C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts in ethanol generation from electrocatalytic CO₂ reduction using a crystal plane modification strategy. These novel Cu-based electrocatalysts were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown in situ on copper foils and modifying with surfactants. It was demonstrated that the fabricated Cu-based electrocatalyst featured a predominantly exposed Cu(100) surface loaded with high-density Cu nanoparticles (NPs). The optimal Cu-based electrocatalyst displayed considerably improved CO₂ electroreduction performance, with a Faraday efficiency of 37.9% for ethanol and a maximum Faraday efficiency of 68.0% for C₂₊ products at −1.4 V vs RHE in an H-cell, accompanied by a high current density of 69.9 mA·cm^–2, much better than the particulate Cu-based electrocatalyst. It was unveiled that the Cu(100)-rich surface of nanoscale petals with abundant under-coordinated copper atoms from CuNPs was conducive to the formation and stabilization of key *CH₃CHO and *OC₂H₅ intermediates, thereby promoting ethanol generation. This study highlighted the critical role of CuNP-loaded Cu(100) surface structures on structured Cu-based electrocatalysts in enhancing ethanol production for the CO₂ electroreduction process.

中文翻译：

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结构化铜基催化剂上负载 Cu 纳米颗粒的 Cu(100) 表面结构在促进 CO2 电还原中乙醇生成中的关键作用


目前，由于C-C耦合困难和产品竞争激烈，在CO ₂ 电还原中实现高乙醇选择性仍然具有挑战性。在这项工作中，我们报告了一种创新方法，使用晶面修饰策略提高电催化 CO ₂ 还原生产乙醇中铜基电催化剂的效率。这些新型铜基电催化剂是通过电化学激活在铜箔上原位生长的三维（3D）花状 CuO 微/纳米结构并用表面活性剂进行改性而制成的。结果表明，所制造的铜基电催化剂具有主要暴露的 Cu(100) 表面，负载有高密度铜纳米颗粒 (NP)。最佳的铜基电催化剂表现出显着改善的 CO ₂ 电还原性能，在 -1.4 时乙醇的法拉第效率为 37.9%，C ₂₊ 产物的最大法拉第效率为 68.0% H 电池中的 V vs RHE，伴随着 69.9 mA·cm ^–2 的高电流密度，比颗粒状铜基电催化剂好得多。结果表明，纳米花瓣表面富含 Cu(100)，且具有丰富的 CuNPs 欠配位铜原子，有利于关键 *CH ₃ CHO 和 *OC ₂ 中间体，从而促进乙醇生成。这项研究强调了结构化铜基电催化剂上负载 CuNP 的 Cu(100) 表面结构在提高 CO ₂ 电还原过程中乙醇产量方面的关键作用。