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Atomically dispersed iron doped-MOF-derived carbon with high iron loading and nitrogen content for the oxygen reduction reaction via a cage-confinement strategy shows excellent catalytic performance.

Rational design and facile synthesis of highly active and stable electrocatalysts for oxygen reduction reaction (ORR) are crucial in the field of metal-air batteries. Here, we present a facile two-stage thermal synthesis of Fe-N codoped porous carbon (Fe-N/C) with abundant Fe-N x active sites and mesopores from Fe-doped ZIF-8 precursors. The first-stage preheating treatment of the Fe-doped ZIF-8 precursors before the second-stage carbonization is the key to boost the coordination between the doped Fe and N-containing ligands, which contributes to a higher N content and more Fe-N x sites in the final carbonized product. Besides, the preheating and Fedoping both affect the morphology, porous structure, and catalytic performance of the fabricated Fe-N/C. The optimized Fe-N/C catalyst exhibits an outstanding ORR catalytic performance with a half-wave potential of 0.88 V and limiting current density of 6.0 mA cm −2 in 0.1 M KOH. A Mg-air battery assembled with a neutral electrolyte using the optimized Fe-N/C catalyst as the cathode exhibits an excellent power density of 72 mW cm −2 at 0.72 V. This developed two-stage synthesis strategy is facile, and the preheating stage could be integrated into any carbonization process as an intermediate step for the fabrication of various metal, N codoped carbon materials with enhanced electrocatalytic performance.

Fundamental kinetics of the V2+/V3+ of vanadium redox flow battery (VRFB) are still not well understood despite tremendous efforts in improving the sluggish kinetics of V2+/V3+. This article first reveals the rate‐determining step in the electrochemical oxidation of V2+ to V3+ by exploring the reaction kinetics. Thereafter, TiB2 with abundant electron‐deficient sites, which possesses a strong electron‐accepting ability, is demonstrated to improve the rate‐determining step of V2+/V3+ by enhancing the electron transfer from V2+ to the electrode. The mechanism of TiB2 for boosting V2+/V3+ kinetics is also unraveled by analyzing the reaction order. VRFB with the electron‐deficient TiB2 demonstrates a remarkable enhancement in the electrochemical performance, exhibiting an excellent rate performance from 70 to 300 mA cm−2. The energy efficiency is improved by 14.06% compared to the cell with the pristine electrode at 150 mA cm−2 for 300 cycles. This study is critical for not only proposing the promising electron‐deficient catalyst in VRFB application but also promoting fundamental understanding and offering a design strategy for achieving superior performance electrocatalysts in VRFB.

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