Boosting oxygen evolution reaction performance <i>via</i> metal defect-induced lattice oxygen redox reactions on spinel oxides

Zheng, Jingxuan; Wang, Zhuozhi; Meng, Dapeng; Guo, Junxin; Wang, Zhao

doi:10.1039/d3ta01385e

J. Mater. Chem. A

2023

DOI: 10.1039/d3ta01385e

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Boosting oxygen evolution reaction performance via metal defect-induced lattice oxygen redox reactions on spinel oxides

Jingxuan Zheng

Zhuozhi Wang

Dapeng Meng

et al.

Abstract: High-performance and low-cost oxygen evolution reaction (OER) catalysts are essential for sustainable energy-to-hydrogen conversion. Defect engineering has been extensively used to optimize the structure and performance of catalysts. Metal defects...

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Cited by 10 publications

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Lattice Oxygen Redox Mechanisms in the Alkaline Oxygen Evolution Reaction

Ren,

Zhai,

Yang

et al. 2024

Adv Funct Materials

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Understanding of fundamental mechanism and kinetics of the oxygen evolution reaction (OER) is pivotal for designing efficient OER electrocatalysts owing to its key role in electrochemical energy conversion devices. In the past few years, the lattice oxygen oxidation mechanism (LOM) arising from the anodic redox chemistry has attracted significant attention as it involves a direct O─O coupling and thus bypasses thermodynamic limitations in the traditional adsorbate evolution mechanism (AEM). Transition metal‐based oxyhydroxides are generally acknowledged as the real catalytic phase in alkaline media. In particular, their low‐dimensional layered structures offer sufficient structural flexibility to trigger the LOM. Herein, a comprehensive overview is provided for recent advances in anion redox from LOM‐based electrocatalysts. Based on analyses of electronic structure of electrocatalysts and LOM, a strategy is proposed to activate LOM. Possible identification techniques for corroboration of the oxygen redox are also reviewed. In addition, the structural reconstruction process induced by the LOM is focused and the importance of multiple in situ/operando characterizations is highlighted to unveil the structural and chemical origins of the LOM. To conclude, a prospect on the remaining challenges and future opportunities for LOM electrocatalysts is presented.

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Lattice Oxygen Redox Mechanisms in the Alkaline Oxygen Evolution Reaction

Ren,

Zhai,

Yang

et al. 2024

Adv Funct Materials

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Defect Engineering for Enhanced Electrocatalytic Oxygen Reaction on Transition Metal Oxides: The Role of Metal Defects

Zheng,

Meng,

Guo

et al. 2024

Advanced Materials

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Metal defect engineering is a highly effective strategy for addressing the prevalent high overpotential issues associated with transition metal oxides functioning as dual‐function commercial oxygen reduction reaction/ oxygen evolution reaction catalysts for increasing their activity and stability. However, the high formation energy of metal defects poses a challenge to the development of strategies to precisely control the selectivity during metal defect formation. We used density functional theory calculations to demonstrate that altering the pathway of metal defect formation released metal atoms as metal chlorides, which effectively reduced the formation energy of defects. The metal defects on the monometallic metal oxide surface (Mn, Fe, Co, and Ni) are selectively produced using chlorine plasma. The characterization and density functional theory calculations reveal that catalytic activity is enhanced owing to electronic delocalization induced by metal defects, which reduces the theoretical overpotential. Notably, ab initio molecular dynamics calculations, ex‐situ XPS, and in‐situ ATR‐SEIRAS suggested that metal defects effectively improved the adsorption of reactive species on active sites and enhanced the efficiency of product desorption, thereby boosting catalytic performance.This article is protected by copyright. All rights reserved

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Enhancing Oxygen Evolution Reaction Performance: Electrochemical Activation of the Biphasic CoNi/Zn(Fe,Al,Cr)₂O₄ via Controlled Aluminum Leaching Facilitated Surface Reconstruction

Chen,

Xu,

Jiang

et al. 2023

Advanced Energy Materials

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Given that the oxygen evolution reaction (OER) faces challenges due to its sluggish kinetics, development of efficient and robust OER catalytic electrodes is critical for reducing the cost of hydrogen production through electrochemical water splitting. In this study, a biphasic CoNi/Zn(Fe,Al,Cr)2O4 coating, characterized by a densely organized stalagmite‐like microarray structure, is deposited on a commercial pure titanium plate, creating an exceptionally effective OER catalytic electrode. The formation of numerous metal/spinel oxide heterogeneous interfaces is demonstrated to enhance its electron transfer ability and conductivity. At high potentials, aluminum leaching and lattice oxygen consumption can facilitate deep surface reconstruction of highly active Fe‐doped CoNiOOH phase inducing electrochemical activation, further optimizing thermodynamic barrier of the fundamental reaction step. Ultimately, this electrode showcases exceptional OER catalytic performance (low overpotential of 248 and 335 mV to deliver the current density of 10 and 100 mA cm−2) compared to commercial IrO2 catalyst (overpotential of ≈310 mV at 10 mA cm−2). Moreover, it demonstrates high current stability sustaining a current density of 500 mA cm−2 for 100 h. This work deepens the comprehension of the surface reconstruction process in OER and, more broadly, introduces a new avenue for designing and enhancing the performance of catalytic materials.

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Boosting oxygen evolution reaction performance via metal defect-induced lattice oxygen redox reactions on spinel oxides

Abstract: High-performance and low-cost oxygen evolution reaction (OER) catalysts are essential for sustainable energy-to-hydrogen conversion. Defect engineering has been extensively used to optimize the structure and performance of catalysts. Metal defects...

Cited by 10 publications

References 74 publications

Lattice Oxygen Redox Mechanisms in the Alkaline Oxygen Evolution Reaction

Lattice Oxygen Redox Mechanisms in the Alkaline Oxygen Evolution Reaction

Defect Engineering for Enhanced Electrocatalytic Oxygen Reaction on Transition Metal Oxides: The Role of Metal Defects

Enhancing Oxygen Evolution Reaction Performance: Electrochemical Activation of the Biphasic CoNi/Zn(Fe,Al,Cr)₂O₄ via Controlled Aluminum Leaching Facilitated Surface Reconstruction

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Boosting oxygen evolution reaction performance via metal defect-induced lattice oxygen redox reactions on spinel oxides

Abstract: High-performance and low-cost oxygen evolution reaction (OER) catalysts are essential for sustainable energy-to-hydrogen conversion. Defect engineering has been extensively used to optimize the structure and performance of catalysts. Metal defects...

Cited by 10 publications

References 74 publications

Lattice Oxygen Redox Mechanisms in the Alkaline Oxygen Evolution Reaction

Lattice Oxygen Redox Mechanisms in the Alkaline Oxygen Evolution Reaction

Defect Engineering for Enhanced Electrocatalytic Oxygen Reaction on Transition Metal Oxides: The Role of Metal Defects

Enhancing Oxygen Evolution Reaction Performance: Electrochemical Activation of the Biphasic CoNi/Zn(Fe,Al,Cr)2O4 via Controlled Aluminum Leaching Facilitated Surface Reconstruction

Contact Info

Product

Resources

About

Enhancing Oxygen Evolution Reaction Performance: Electrochemical Activation of the Biphasic CoNi/Zn(Fe,Al,Cr)₂O₄ via Controlled Aluminum Leaching Facilitated Surface Reconstruction