Pyrolysis‐Free Synthesized Catalyst towards Acidic Oxygen Reduction by Deprotonation

• Published in: Angewandte Chemie International Edition 2021-09, Vol.60 (38), p.20865-20871
• Main Authors: Zang, Ying, Mi, Chunxia, Wang, Rui, Chen, Hong, Peng, Peng, Xiang, Zhonghua, Zang, Shuang‐Quan, Mak, Thomas C. W.
• Format: Article
• Language: English
• Subjects: acidic conditions; Catalysts; Chemical reduction; Chemical synthesis; deprotonation; Fuel cells; Fuel technology; Inactivation; Maximum power density; Oxygen; oxygen reduction; Oxygen reduction reactions; Pyrolysis; pyrolysis-free; Renewable energy
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202106661

Acidic oxygen reduction is vital for renewable energy devices such as fuel cells. However, many aspects of the catalytic process are still uncertain—especially the large difference in activity in acidic and alkaline media. Thus, the design and synthesis of model catalysts to determine the active centers and the inactivation mechanism are urgently needed. We report a pyrolysis‐free synthesis route to fabricate a catalyst (CPF‐Fe@NG) for oxygen reduction in acidic conditions. By introducing a deprotonation process, we extended the oxygen reduction reaction (ORR) activity from alkaline to acidic conditions. CPF‐Fe@NG demonstrated outstanding performance with a half‐wave potential of 853 mV (vs. RHE) and good stability after 10000 cycles in 1 M HClO4. The pyrolysis‐free route could also be used to assemble fuel cells, with a maximum power density of 126 mW cm−2. Our findings offer new insights into the ORR process to optimize catalysts for both mechanistic studies and practical applications. A catalyst possessing well‐defined active sites and intrinsic activity for the oxygen reduction reaction was prepared by a pyrolysis‐free route. The performance of the catalyst was explored in acidic media by introducing a deprotonation process.