High-Density Accessible Iron Single-Atom Catalyst for Durable and Temperature-Adaptive Laminated Zinc-Air Batteries

Abstract

Designing single-atom catalysts (SACs) with high density of accessible sites by improving metal loading and sites utilization is a promising strategy to boost the catalytic activity, but remains challenging. Herein, a high site density (SD) iron SAC (D-Fe-N/C) with 11.8 wt.% Fe-loading is reported. The in situ scanning electrochemical microscopy technique attests that the accessible active SD and site utilization of D-Fe-N/C reach as high as 1.01 × 10²¹ site g⁻¹ and 79.8%, respectively. Therefore, D-Fe-N/C demonstrates superior oxygen reduction reaction (ORR) activity in terms of a half-wave potential of 0.918 V and turnover frequency of 0.41 e site⁻¹ s⁻¹. The excellent ORR property of D-Fe-N/C is also demonstrated in the liquid zinc-air batteries (ZABs), which exhibit a high peak power density of 306.1 mW cm⁻² and an ultra-long cycling stability over 1200 h. Moreover, solid-state laminated ZABs prepared by presetting an air flow layer show a high specific capacity of 818.8 mA h g⁻¹, an excellent cycling stability of 520 h, and a wide temperature-adaptive from −40 to 60 °C. This work not only offers possibilities by improving metal-loading and catalytic site utilization for exploring efficient SACs, but also provides strategies for device structure design toward advanced ZABs.