Site-specific synergy by heteronuclear microenvironment atomic editing for oxygen reduction reaction
Siqi Ji, Yuhao Wang, Hongxue Liu, Xue Lü, Yu Wang, Xinlong Tian, Yasong Zhao, J. Hugh Horton, Zhijun Li
Abstract
Although iron-nitrogen-carbon catalysts are appealing for use in the oxygen reduction reaction, achieving high activity and a long lifetime remains a persistent challenge. This necessitates the precise modulation of the active sites’ microenvironment. Herein, we present a microenvironment atomic editing strategy for accessing heteronuclear triatomic Fe and Co sites of Fe1Co2N7O1 supported on a nitrogen-doped carbon matrix (Fe1Co2/NC). Its performance is boosted by the orbital hybridization between Fe and Co atoms, which alters the d band centers to push the activity (half-wave potential of 0.94 V in alkaline and 0.88 V in acid conditions) and stability boundaries to a high level. The optimized metal-adsorbate interactions and strengthened metal − N bonding in Fe1Co2N7O1 are responsible for the competitive activity and stability. Furthermore, rechargeable and flexible quasi-solid-state zinc-air batteries using this catalyst achieve high power density (282.7 mW cm−2 and 95.8 mW cm−2) and high operational stability, and are therefore more energy-efficient than commercial catalysts. Our findings underscore the importance of atomic editing for designing low-nuclearity catalysts. The development of advanced electrocatalysts with high efficiency and longevity is essential to alleviate the energy crisis. Here, the authors report an atomic editing strategy to access atomically dispersed, heteronuclear triatomic Fe and Co sites to endow improved activity and stability.