Vapor deposition strategy for implanting isolated Fe sites into papermaking nanofibers-derived N-doped carbon aerogels for liquid Electrolyte-/All-Solid-State Zn-Air batteries.

Single-atom catalysts (SACs), with precisely controlled metal atom distribution and adjustable coordination architecture, have gained intensive concerns as efficient oxygen reduction reaction (ORR) electrocatalysts in Zn-air batteries (ZAB). The attainment of a monodispersed state for metallic atoms anchored on the carbonaceous substrate remains the foremost research priority; however, the persistent challenges lie in the relatively weak metal-support interactions and the instability of captured single atom active sites. Furthermore, in order to achieve rapid transport of O and other reactive substances within the carbon matrix, manufacturing SACs based on multi-stage porous carbon substrates is highly anticipated. Here, we propose a methodology for the fabrication of carbon aerogels (CA)-supported SACs utilizing papermaking nanofibers, which incorporates advanced strategies for N-atom self-doping, defect/vacancy introduction, and single-atom interface engineering. Specifically, taking advantages of using green and energy-efficient feedstocks, combining with a direct pore-forming template volatilization and chemical vapor deposition approach, we successfully developed N-doped carbon aerogels immobilized with separated iron sites (Fe-SAC@N/CA-Cd). The obtained Fe-SAC@N/CA-Cd exhibited substantially large specific surface area (S = 1173 m/g) and a multi-level pore structure, which can effectively mitigate the random aggregation of Fe atoms during pyrolysis. As a result, it demonstrated appreciable activity and stability in catalyzing the ORR progress (E = 0.88 V, E = 0.96 V). Furthermore, the assembled liquid electrolyte-state Zn-air batteries (LES-ZAB) and all-solid-state Zn-air battery (ASS-ZAB) also provides encouraging performance, with a peak power density of 169 mW cm for LES-ZAB and a maximum power density of 124 mW cm for ASS-ZAB.