Cascade protection strategy for anchoring atomic FeN3 sites within defect-rich wood carbon aerogel for high-performance Zn-air batteries and versatile application
Jiaojiao Sun, Mengxia Shen, A. Jun Chang, Chanjuan Liang, Chuanyin Xiong, Chen Hou, Jinbao Li, Pengbo Wang, Jiayin Li, Jianfeng Huang
Abstract
The emergence of metal-nitrogen-carbon single atom catalysts (M-N-C SACs) has revolutionized the field of cathode materials in zinc-air battery (ZAB) devices. Nevertheless, accurately regulating the metal–carbon support interactions and the metal coordination centers at the atomic scale remains pivotal scientific challenges for enhancing their intrinsic catalytic activity. Besides, the carbon substrate materials commonly in the powder form entail essential dependence on extra binders or carbon cloths, hindering the development of self-supported M-N-C SACs for practical electrochemical devices. In this study, we employed the natural wood and implemented an effective cascade protection strategy to achieve a multi-level porous wood-derived carbon-supported Fe single atom catalyst (MPWC-FeSA) with atomically dispersed Fe-N 3 sites, abundant defects, hierarchical porous network structure, and robust mechanical properties. Density functional theory calculations confirm that vacancy defects improve the electronic environment surrounding the FeN 3 active sites in MPWC-FeSA, resulting in a low overpotential for the oxygen reduction reaction (ORR). The MPWC-FeSA exhibited exceptional ORR performance when utilized in the assembled liquid-state Zinc Air Batteries (LZABs) and quasi-solid-state devices for diverse application scenarios. This study offers novel prospects for transforming wood biomass into the self-supported electrode materials, as well as opens up effective avenues in achieving atomic economy.