Wang, Tianlei; (2024) Palladium-based electrocatalysts for oxygen reduction and ethanol oxidation. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

The oxygen reduction reaction (ORR) at the cathode is often the key part in energy conversion devices, such as fuel cells and metal-air batteries. While platinum (Pt) is the commercially available catalyst, palladium (Pd)-based materials are emerging as a compelling alternative for ORR due to their relative abundance, superior methanol tolerance, and better ORR performance in alkaline conditions. Despite these advantages, the real-world application of many high-activity ORR catalysts is hampered by durability concerns. Hence, ensuring the long-term stability of ORR catalysts is a primary concern in this aera. Ethanol oxidation reaction (EOR) holds critical importance in energy conversion and storage, particularly in advancing direct ethanol fuel cells (DEFCs). EOR is of interest due to ethanol as a renewable biofuel with high energy density and lower toxicity compared to methanol. Pt and Pt-based alloys are widely used as catalysts for EOR. However, ongoing research seeks more cost-effective and durable alternatives, including Pd-based catalysts and other transition metals materials. Palladium-based materials, as alternatives to platinum-based materials, exhibit high catalytic activity in both the ORR and the EOR, especially in alkaline solutions, offering promising applications in the energy conversion field. Therefore, this thesis has developed strategies for obtaining robust Pd-based catalysts with enhanced activity for ORR and EOR. Using dealloying methods, strain engineering, and defect engineering strategies, various Pd-based catalysts have been prepared, and in-depth studies have been conducted on their structural changes before and after reactions. Detailed physiochemical and electrochemical characterizations have been performed to reveal the mechanism of structural activation and the relationship between structure and performance.

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