FeN<sub>4</sub>S<sub>1</sub> Single-Atom Sites Anchored on Three-Dimensional Porous Carbon for Highly Efficient and Durable Oxygen Electrocatalysis.
basic_science · Level V
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- Record sourced from PubMed, PMID 39528350.
- Also identified by DOI 10.1021/acsnano.4c15410.
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Abstract
Precisely designing asymmetric active centers and exploring their electronic regulation effects to prepare efficient bifunctional single-atom catalysts (SACs) is important for boosting the practical applications of zinc-air batteries (ZABs). Herein, an effective strategy has been developed by introducing an axial S atom to the FeN<sub>4</sub> active center, simultaneously assisted by pyrolyzing the graphene oxide (GO) sheathed zeolitic-imidazolate framework-8 (ZIF8) composite and constructing a three-dimensional (3D) porous framework with abundant FeN<sub>4</sub>S<sub>1</sub> moieties. This structure can accelerate the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) kinetics owing to the modulated electronic redistribution and <i>d</i>-band center with a reduced energy barrier. The optimal S-Fe-NC/rGO showcases a lower voltage gap (Δ<i>E</i>) of 0.64 V between both the ORR and OER half-wave potentials at 10 mA cm<sup>-2</sup>, highlighting the excellent bifunctional activities. The assembled S-Fe-NC/rGO rechargeable liquid ZABs deliver a power density of 154.05 mW·cm<sup>-2</sup> and a desirable durability of >900 h. More importantly, the corresponding flexible solid-state ZABs exhibit considerable foldability.