Electrocatalytic semi-hydrogenation of alkynols holds tremendous advantages over conventional thermocatalysis process. However, the selectivity-activity seesaw effect is a principal obstacle to its further development. Inspired by interfacial self-assembled monolayers, alkanethiols with different alkyl chain lengths are employed to modify the Cu surface for controllably modulating the activity and selectivity in the semi-hydrogenation of alkynols. 1-dodecanethiol-modified Cu nanowires (Cu NWs) exhibit the optimal electrosynthesis of 2-methyl-3-buten-2-ol with excellent specific selectivity (above 93%) in the semi-hydrogenation of 2-methyl-3-butyn-2-ol. Mechanistic studies reveal that the proportion of liquid-like water increases while the proportion of isolated water reduces at the hydrophobic interface. Moreover, we assemble a larger 3 × 100 cm² electrolyzer stack, which can deliver a single-pass alkynol conversion rate of 95% and an excellent alkenol selectivity of 94% at a 15 A stack current. Eventually, the Cu NWs catalyst with thiol treatment is also applicable to the semi-hydrogenation of various unsaturated alkynols.

中文翻译：

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硫醇处理调节电化学炔醇半氢化的界面润湿性


与传统的热催化工艺相比，炔醇的电催化半氢化具有巨大的优势。然而，选择性-活性跷跷板效应是其进一步发展的主要障碍。受界面自组装单层的启发，具有不同烷基链长度的烷硫醇被用来修饰Cu表面，以可控地调节炔醇半氢化的活性和选择性。 1-十二烷硫醇修饰的铜纳米线（Cu NWs）在2-甲基-3-丁烯-2-醇的半氢化反应中表现出最佳的2-甲基-3-丁烯-2-醇电合成效果，具有优异的选择性（高于93%） 2-ol。机理研究表明，在疏水界面处，液态水的比例增加，而孤立水的比例减少。此外，我们组装了一个更大的3 × 100 cm ²电解槽堆，在15 A堆电流下可以提供95%的单程炔醇转化率和94%的优异的烯醇选择性。最终，经过硫醇处理的Cu NWs催化剂也适用于各种不饱和炔醇的半加氢。