Electrocatalytic reduction of biomass-derived furfural (FF) represents a sustainable route to produce furfuryl alcohol (FA) and 2-methylfuran (MF) as a value-added chemical and a biofuel, respectively. However, achieving high selectivity for MF as well as tuning the selectivity between FA and MF within one reaction system remain challenging. Herein, we have reported an electrode–electrolyte interface modification strategy, enabling FA and MF selectivity steering under the same reaction conditions. Specifically, by modifying copper (Cu) electrocatalysts with butyl trimethylammonium bromide (BTAB), we achieved a dramatic shift in selectivity from producing FA (selectivity: 83.8%; Faradaic efficiency, FE: 68.9%) to MF (selectivity: 80.1%; FE: 74.8%). We demonstrated that BTAB adsorption over Cu modulates the electrical double layer (EDL) structure, which repels interfacial water and weakens the hydrogen-bond (H-bond) network for proton transfer, thus impeding FF-to-FA conversion by suppression of the hydrogen atom transfer (HAT) process. On the contrary, FF-to-MF conversion was less affected. This work shows the potential of engineering of the electrode–electrolyte interface for selectivity control in electrocatalysis.

中文翻译：

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通过电极-电解质界面改性实现电催化糠醛还原的转向选择性

生物质衍生的糠醛 (FF) 的电催化还原代表了分别生产糠醇 (FA) 和 2-甲基呋喃 (MF) 作为增值化学品和生物燃料的可持续途径。然而，实现 MF 的高选择性以及在一个反应​​系统内调节 FA 和 MF 之间的选择性仍然具有挑战性。在此，我们报道了一种电极-电解质界面修饰策略，可在相同的反应条件下实现 FA 和 MF 选择性转向。具体来说，通过用丁基三甲基溴化铵 (BTAB) 改性铜 (Cu) 电催化剂，我们实现了选择性的显着转变，从生产 FA（选择性：83.8%；法拉第效率，FE：68.9%）到 MF（选择性：80.1%；FE） ：74.8%）。我们证明了 BTAB 在 Cu 上的吸附调节了双电层 (EDL) 结构，从而排斥界面水并削弱了质子转移的氢键 (H-bond) 网络，从而通过抑制氢来阻碍 FF 到 FA 的转化。原子转移（HAT）过程。相反，FF 到 MF 的转换受到的影响较小。这项工作展示了电极-电解质界面工程在电催化选择性控制方面的潜力。