Resonance-Promoted Formic Acid Oxidation via Dynamic Electrocatalytic Modulation
Resonance-Promoted Formic Acid Oxidation via Dynamic Electrocatalytic Modulation
复制标题
DOI：
10.1021/acscatal.0c02201
复制
发表时间：
2020-09-04
期刊：
影响因子：
12.9
通讯作者：
Abdelrahman, Omar A.
中科院分区：
文献类型：
--
作者：
Gopeesingh, Joshua;Ardagh, M. Alexander;Abdelrahman, Omar A.
更快的催化剂能够更有效地将分子转化为有用的产品，并提高自然资源的利用率，这是一个公认的真理。然而，由Sabatier原理定义的静态催化剂性能的限制促使了催化剂设计的动态方法，由此催化剂在不同的能量状态之间振荡。本文通过甲酸在铂电极上的电催化氧化实验，验证了动态催化共振的概念。在0和0.8 V NHE之间通过方波以不同频率（10（-3）< f < 103 Hz）振荡电动势使转换频率增加到类似于100 Hz下的20 s（-1），比最佳恒电位条件快一个数量级（20 x）。我们属性的加速动态催化nonfaradaic甲酸脱水到表面结合的一氧化碳在低电位，然后在高电位的表面氧化和解吸到二氧化碳。
It is a truth universally acknowledged that faster catalysts enable more efficient transformation of molecules to useful products and enhance the utilization of natural resources. However, the limit of static catalyst performance defined by the Sabatier principle has motivated a dynamic approach to catalyst design, whereby catalysts oscillate between varying energetic states. In this work, the concept of dynamic catalytic resonance was experimentally demonstrated via the electrocatalytic oxidation of formic acid over Pt. Oscillation of the electrodynamic potential between 0 and 0.8 V NHE via a square waveform at varying frequency (10(-3) < f < 103 Hz) increased the turnover frequency to similar to 20 s(-1) at 100 Hz, over one order of magnitude (20x) faster than optimal potentiostatic conditions. We attribute the accelerated dynamic catalysis to nonfaradaic formic acid dehydration to surface-bound carbon monoxide at low potentials, followed by surface oxidation and desorption to carbon dioxide at high potentials.