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Tuning the N Coordination Environment of Ir Single-Atom-Catalyst for Highly Efficient ORR and OER: A Computational Study

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Abstract

Modulating the coordination environments of single-atom catalysts (SAC) holds great potential to improve their catalytic activity in electrocatalysis. In this work, by means of comprehensive density functional theory computations, we systematically explored the catalytic performance of single Ir atom with different coordination environments for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Our results showed that the introduction of nitrogen atoms can improve the catalytic activity of IrC4 for ORR and OER. Especially, IrN4 can be used as ORR and OER bifunctional electrocatalysts with the overpotentials (ηORR = 0.36 V and ηOER = 0.55 V). Interestingly, some descriptors, including energy descriptor (ΔGOH*), structure descriptor (φ), and d-band center (εd), can well explain the high catalytic activity of IrN4 towards ORR/OER. Our findings not only provide new insights into the development of efficient ORR and OER bifunctional electrocatalysts, but also open a new door to boost the catalytic performance of SACs.

Graphical Abstract

IrN4 was identified as efficient bifunctional catalyst for ORR and OER by exploring different N coordination environments through comprehensive density functional theory calculations, which is attributed to the ideal φ value and the d-band center near the Fermi energy level.

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Acknowledgements

This work was financially supported by the Harbin Normal University Science and Technology Innovation Climbing Program Funding Project (XKB202212).

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  1. Harbin Vocational College of Science and Technology, Harbin, 150300, Heilongjiang, China

    Ying Zhu

  2. College of Chemistry and Chemical Engineering, and Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin, 150025, China

    Zhongxu Wang

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Zhu, Y., Wang, Z. Tuning the N Coordination Environment of Ir Single-Atom-Catalyst for Highly Efficient ORR and OER: A Computational Study. Catal Lett 154, 2464–2474 (2024). https://doi.org/10.1007/s10562-023-04490-0

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