Publication date: 10th April 2024
When Max Born looked back to his life's work, he concluded: "I have restricted my work to ideal crystals though I am aware that the theory of the defects in real crystals is practically far more important. This I have left to a younger generation." Indeed, ionic point defects play an important role in determining the phase, structure, properties and functionality of oxide ceramics and thin films. In this talk, I am going to show the methodology and case studies towards a better understanding of the role of ionic point defects (e.g., oxygen vacancies and protons) in determining the activity of oxide electrocatalysts. I will start with our recent work on well-controlled model thin film electrocatalysts for the high-temperature oxygen incorporation reaction (OIR). Combining operando X-ray photoemission spectroscopy and electrochemical measurements, we reveal the change of reaction mechanisms across the phase boundaries triggered by the change of oxygen vacancy concentration. Then I am going to show the encountered complexity when we switch from well-controlled high-temperature solid/gas interfaces to room-temperature solid/liquid interfaces. I will show our recent effort of understanding the room-temperature defect chemistry in model electrocatalysts for the oxygen evolution reaction (OER). Lastly, I will compare the two cases, i.e., high-temperature solid/gas interfaces and room-temperature solid/liquid interfaces, and discuss the similarities and differences towards a better mechanistic understanding of OIR/OER reactions.
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