Differentiating Oxygen Exchange Reaction Mechanisms across Phase Boundaries,Journal of the American Chemical Society

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Differentiating Oxygen Exchange Reaction Mechanisms across Phase Boundaries
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-11-16 , DOI: 10.1021/jacs.3c09693
Kaichuang Yang _{1,

2} , Ying Lu ₂ , Yang Hu ₂ , Zihan Xu ₂ , Jieping Zheng ₂ , Haowen Chen ₂ , Jingle Wang ₂ , Yi Yu ₃ , Hui Zhang _{4,

5} , Zhi Liu ₃ , Qiyang Lu _{2,

6}

Affiliation

Triggering phase transitions by controlling the anion stoichiometry is an effective method of tuning the electrocatalytic activity of the functional oxides. However, understanding the potential differences in the reaction mechanism(s) of different phases requires the accurate mapping of phase boundaries during the electrochemical reactions, which can be quite challenging. In this work, we have established a feasible electrochemical method based on the measurement of chemical capacitance to resolve the critical stoichiometry at phase boundaries under operando conditions. We select a simple binary oxide PrO_x as a proof-of-principle model system, which shows excellent activity for high-temperature oxygen incorporation and evolution reactions (OIR/OER). We show that the phase transition can be sensitively probed by quantifying the chemical capacitance, which can be further used for differentiating the OIR/OER mechanisms across the phase boundary of PrO_x. Therefore, our findings provide a new framework for exploring phase engineering as a tool for the design of electrocatalysts.

中文翻译：

区分跨相界的氧交换反应机制

通过控制阴离子化学计量触发相变是调节功能氧化物电催化活性的有效方法。然而，了解不同相反应机制的电位差需要准确绘制电化学反应过程中的相边界，这可能非常具有挑战性。在这项工作中，我们建立了一种基于化学电容测量的可行电化学方法，以解决操作条件下相边界的临界化学计量。我们选择一种简单的二元氧化物 PrO _x作为原理验证模型系统，该系统在高温氧结合和析出反应（OIR/OER）方面表现出优异的活性。我们表明，可以通过量化化学电容来灵敏地探测相变，这可以进一步用于区分 PrO _x相界上的 OIR/OER 机制。因此，我们的研究结果为探索相工程作为电催化剂设计工具提供了一个新的框架。

更新日期：2023-11-16

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