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April 4, 2023Nature Communications538 citationsOpen Access

Regulating electronic states of nitride/hydroxide to accelerate kinetics for oxygen evolution at large current density

PZPanlong ZhaiCWChen WangYZYuanyuan Zhao

Key Points

  • To design an efficient transition metal electrocatalyst array that accelerates oxygen evolution reaction kinetics and maintains stability at high industrial current densities.
  • Synthesized hierarchical bimetal nitride/hydroxide (NiMoN/NiFe LDH) arrays as a model catalyst system.
  • Tracked dynamic structure evolution, charge transport, and reaction kinetics using in-situ electrochemical spectroscopy and operando electrochemical impedance spectroscopy.
  • Analyzed the underlying reaction mechanisms through combined experimental measurements and theoretical calculations.
  • The activated NiMoN/NiFe LDH electrocatalyst achieved an industrial current density of 1000 mA cm⁻² at an overpotential of 266 mV.
  • The catalyst maintained steady oxygen evolution performance over 250 hours of continuous operation.
  • Mechanistic investigations confirmed accelerated reaction kinetics operating via a lattice oxygen oxidation pathway facilitated by optimized heterointerfaces.

Abstract

Rational design efficient transition metal-based electrocatalysts for oxygen evolution reaction (OER) is critical for water splitting. However, industrial water-alkali electrolysis requires large current densities at low overpotentials, always limited by intrinsic activity. Herein, we report hierarchical bimetal nitride/hydroxide (NiMoN/NiFe LDH) array as model catalyst, regulating the electronic states and tracking the relationship of structure-activity. As-activated NiMoN/NiFe LDH exhibits the industrially required current density of 1000 mA cm-2 at overpotential of 266 mV with 250 h stability for OER. Especially, in-situ electrochemical spectroscopic reveals that heterointerface facilitates dynamic structure evolution to optimize electronic structure. Operando electrochemical impedance spectroscopy implies accelerated OER kinetics and intermediate evolution due to fast charge transport. The OER mechanism is revealed by the combination of theoretical and experimental studies, indicating as-activated NiMoN/NiFe LDH follows lattice oxygen oxidation mechanism with accelerated kinetics. This work paves an avenue to develop efficient catalysts for industrial water electrolysis via tuning electronic states.

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Cite This Study

Zhai et al. (2023) studied this question.

synapsesocial.com/papers/69dbc2db387cf70698688a1ahttps://doi.org/10.1038/s41467-023-37091-x
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