Regulating the spin state of triple-atom catalysts for improved oxygen electrocatalysis in zinc-air batteries at subzero temperature
Year: 2025
Type: article
Abstract: Triple-atom catalysts (TACs), building upon dual-atom catalysts, have demonstrated exceptional catalytic activity toward oxygen reduction reaction (ORR). Nevertheless, advancing the catalytic activity of TACs for application in low-temperature (Low-T) energy conversion devices remains a formidable challenge, primarily limited by the slow capture efficiency of oxygen reactants at catalytic sites. In this work, utilizing Fe-Fe double atomic pairs as a foundational research model, we plant the CoN4 site adjacent to activate them to construct efficient ORR electrocatalysts (named as Fe2/Co-NHCS) featuring the Fe2N5+CoN4 tri-atomic structure. The adjacent CoN4 site can optimize the spin state of the Fe-Fe double atomic pairs from low to medium spin with ${ {t}_{{2g}^{4}}} $ ${ {e}_{{g}^{1}} }$ 3d-electron configuration, which makes the catalysts bind with oxygen reactants more readily to complete ORR process. As anticipated, the Fe2/Co-NHCS achieved a high half-wave potential of 0.92 V. Moreover, the flexible Zn-air batteries powered by Fe2/Co-NHCS deliver a large peak power density of 57.3 mW cm-2 and brilliant charge-discharge stability over 150 stable cycles at -40°C. This research advances ORR electrocatalysts by modulating the electron spin states at diatomic Fe sites, paving a viable route for expanding the application range of ZABs in low-temperature environment.
Source: The Innovation Materials
Authors: Canhui Zhang, Zhuangzhuang He, Li Qiao, Xu Liu, Kaiyue Chen, Xingkun Wang, Jian Zhou, Lei Chu, Guanghui Wang, Minghua Huang, Heqing Jiang
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: diamond
OpenAlex ID: W4410279563