High-Entropy Perovskite Oxides as a Family of Electrocatalysts for Efficient and Selective Nitrogen Oxidation
At a Glance
Section titled āAt a Glanceā| Metadata | Details |
|---|---|
| Publication Date | 2024-06-24 |
| Journal | ACS Nano |
| Authors | Hui Zheng, Yunxia Liu, Ziwei Ma, Elke Debroye, Jinyu Ye |
| Institutions | Jiangnan University, Northwestern Polytechnical University |
| Citations | 33 |
Abstract
Section titled āAbstractāElectrocatalytic nitrogen oxidation reaction (NOR) can convert nitrogen (N<sub>2</sub>) into nitrate (NO<sub>3</sub><sup>-</sup>) under ambient conditions, providing an attractive approach for synthesis of NO<sub>3</sub><sup>-</sup>, alternative to the current approach involving the harsh Haber-Bosch and Ostwald oxidation processes that necessitate high temperature, high pressure, and substantial carbon emission. Developing efficient NOR catalysts is a prerequisite, which remains a formidable challenge, owing to the weak activation/dissociation of N<sub>2</sub>. A variety of NOR electrocatalysts have been developed, but their NOR kinetics are still extremely sluggish, resulting in inferior Faradaic Efficiencies. Here, we report a high-entropy Ru-based perovskite oxide (denoted as Ru-HEP) that can function as a high-performance NOR catalyst and exhibit a high NO<sub>3</sub><sup>-</sup> yield rate of 39.0 Ī¼mol mg<sup>-1</sup> h<sup>-1</sup> with a Faradaic Efficiency of 32.8%. Both our experimental results and theoretical calculations suggest that the high-entropy configuration of Ru-HEP perovskite oxide can markedly enhance the oxygen-vacancy concentration, where the Ru sites and their neighboring oxygen vacancies can serve as unsaturated centers and decrease the overall energy barrier for N<sub>2</sub> electrooxidation, thereby leading to promoted NOR kinetics. This work presents an alternative avenue for promoting NOR catalysis on perovskite oxides through the high-entropy engineering strategy.