Tuning Electrocatalytic Oxygen Reduction Reaction with Dynamic Control of Electrochemical Interfaces
Tuning Electrocatalytic Oxygen Reduction Reaction with Dynamic Control of Electrochemical Interfaces
复制标题
通过电化学界面的动态控制来调节电催化氧还原反应
DOI：
10.1021/jacs.3c13694
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发表时间：
2024
影响因子：
15
通讯作者：
Ren, Hang
中科院分区：
文献类型：
--
作者：
Lee, Hyein;Ren, Hang
在这里，我们报告的氧还原反应（ORR）的活性和选择性的调谐通过电化学界面的动态调节，以超过传统的电催化的性能。这是通过在金电极上施加ORR工作电位和阴离子吸附电位之间的振荡电位来实现的。振荡电位提高了H2O2的选择性高达1.35倍相比，静态电位，证实了旋转环盘电极和荧光分析测量。我们发现，增强的选择性取决于动态吸附和解吸的阴离子，和增强发生在毫秒或更短的时间尺度。在电位切换后的前5ms内，对H2O2的选择性可达97%左右。我们的研究结果表明，动态界面可以创建一个短暂的，但独特的微环境，新的反应，不能在静态条件下，这提供了一个新的维度控制电催化。
Herein, we report the tuning of the activity and selectivity of the oxygen reduction reaction (ORR) through the dynamic regulation of the electrochemical interfaces to surpass the performance of conventional electrocatalysis. This is achieved by applying an oscillating potential between the ORR operating potential and anion adsorbing potential on a gold electrode. Oscillating potential enhances the selectivity for H2O2by up to 1.35 times compared to the static potential, as confirmed by rotating ring-disk electrode and fluorescence assay measurements. We showed that the enhanced selectivity depends on dynamic adsorption and desorption of anions, and the enhancement occurs in the millisecond time scale or shorter. The transient selectivity to H2O2can reach ∼97% within the first 5 ms after potential switching. Our results suggest that the dynamic interface can create a transient but unique microenvironment for new reactivity that cannot be reproduced under static conditions, which offers a new dimension in controlling electrocatalysis.