3 years ago

Stabilizing Double Perovskite for Effective Bifunctional Oxygen Electrocatalysis in Alkaline Conditions

Stabilizing Double Perovskite for Effective Bifunctional Oxygen Electrocatalysis in Alkaline Conditions
Meng Li, Babak Shalchi Amirkhiz, Jian Chen, Yi-Fei Sun, Jing-Li Luo, Yimin Zeng, Ya-Qian Zhang, Bin Hua, Ning Yan
Oxygen electrocatalysis is at the heart of the emerging energy conversion and storage devices including reversible fuel cells and metal-air batteries. However, replacing the noble-metal-based oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts with affordable and robust alternatives remains challenging to date. Herein, we report a cation-ordered double perovskite oxide, i.e., PrBa0.85Ca0.15MnFeO5+δ, with excellent stability and activity in both OER and ORR. The layered crystal structure provides ordered oxygen vacancy channels and a vast amount of surface oxygen defects, while the moderate amount of iron dopant keeps the B-site cations at high oxidation state with optimal eg fillings. Importantly, the DFT calculations along with the advanced TEM analysis verify that the incorporation of Ca at the A-site stabilizes the perovskite structure under potential bias. Such a bifunctional catalyst shows comparable, if not better, activity relative to the state-of-the-art perovskite oxides (e.g., Ba0.5Sr0.5Co0.8Fe0.2O3−δ) while demonstrating remarkably enhanced robustness. This work presents a rational approach of designing efficient, robust, and cost-effective perovskite oxide for oxygen electrocatalysis and sheds light on the influences of the crystallographic structure on the catalytic property.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b01114

DOI: 10.1021/acs.chemmater.7b01114

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