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Oxygen evolution reaction dynamics monitored by an individual nanosheet-based electronic circuit

机译:通过单个基于纳米片的电子电路监测氧释放反应动力学

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摘要

The oxygen evolution reaction involves complex interplay among electrolyte, solid catalyst, and gas-phase and liquid-phase reactants and products. Monitoring catalysis interfaces between catalyst and electrolyte can provide valuable insights into catalytic ability. But it is a challenging task due to the additive solid supports in traditional measurement. Here we design a nanodevice platform and combine on-chip electrochemical impedance spectroscopy measurement, temporary I-V measurement of an individual nanosheet, and molecular dynamic calculations to provide a direct way for nanoscale catalytic diagnosis. By removing O2 in electrolyte, a dramatic decrease in Tafel slope of over 20% and early onset potential of 1.344 V vs. reversible hydrogen electrode are achieved. Our studies reveal that O2 reduces hydroxyl ion density at catalyst interface, resulting in poor kinetics and negative catalytic performance. The obtained in-depth understanding could provide valuable clues for catalysis system design. Our method could also be useful to analyze other catalytic processes.
机译:析氧反应涉及电解质,固体催化剂以及气相和液相反应物及产物之间的复杂相互作用。监测催化剂和电解质之间的催化界面可以提供有关催化能力的宝贵见解。但这是一项具有挑战性的任务,因为传统测量中添加了固体支持物。在这里,我们设计了一个纳米设备平台,并结合了片上电化学阻抗谱测量,单个纳米片的临时I-V测量以及分子动力学计算,为纳米级催化诊断提供了直接途径。通过去除电解液中的O2,与可逆氢电极相比,Tafel斜率显着降低了20%以上,早期启动电位为1.344V。我们的研究表明,O2会降低催化剂界面处的氢氧根离子密度,从而导致不良的动力学性能和负面的催化性能。所获得的深入理解可以为催化系统设计提供有价值的线索。我们的方法对分析其他催化过程也可能有用。

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