Fe, P Heteronuclear Catalytic Pairs with Hydrogen Bonding Regulated the Oxygen Reduction Reaction Kinetics for an Ultrastable Oxygen Depolarized Cathode.
basic_science · Level V
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- Record sourced from PubMed, PMID 41217778.
- Also identified by DOI 10.1021/acsnano.5c15715.
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Abstract
The rational design of efficient oxygen reduction reaction (ORR) catalysts with maximized atom utilization is essential for advancing the oxygen depolarized cathode technology. Here, we report atomically dispersed Fe, P heteronuclear catalytic pairs on hierarchical porous carbon, in which the hydrogen bond between Fe, P catalytic pairs and ORR intermediates significantly enhances the adsorption/desorption kinetics and lowers the rate-determining step barrier of OH* desorption. Thus, Fe,P/HPC delivers an alkaline ORR performance with a half-wave potential (<i>E</i><sub>1/2</sub>) of 0.92 V and retains ∼90% of the initial activity even after 150 h operation. In addition, Fe,P/HPC achieves an <i>E</i><sub>1/2</sub> of 0.74 V in 0.1 M HClO<sub>4</sub>. The Fe,P/HPC-based aqueous Zn-air battery (A-ZAB) achieves a high power density of 262 mW cm<sup>-2</sup> and exhibits enhanced stability, sustaining a minimal voltage gap over 2800 h of constant-current cycling. Moreover, the quasi-solid-state Zn-air battery (QSS-ZAB) delivers a large open-circuit voltage of 1.52 V, while maintaining a cycling stability for over 95 h at 0.5, 1, and 2 mA cm<sup>-2</sup>, respectively. In the chlor-alkali process, the Fe,P/HPC||RuO<sub>2</sub> electrolyzer enables a large current density of 300 mA cm<sup>-2</sup> at 1.66 V and maintains stability over 110 h. The present work pioneers the designing and construction of atomic-level heteronuclear catalysts for practical and durable cathode.