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Research Article

Surface reconstruction and structural transformation of two-dimensional Ni-Fe MOFs for oxygen evolution in seawater media

Liyuan Xiao1,§, Xue Bai1,§, Jingyi Han1, Tianmi Tang1, Siyu Chen1, Hui Qi2, Changmin Hou3, Fuquan Bai4( ), Zhenlu Wang1( ), Jingqi Guan1( )
Institute of Physical Chemistry, College of Chemistry, Jilin University, Changchun 130021, China
The Second Hospital of Jilin University, Changchun 130021, China
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, College of Chemistry, Changchun 130023, China

§ Liyuan Xiao and Xue Bai contributed equally to this work.

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Graphical Abstract

Ni-Fe metal-organic framework nanosheets on nickel foam (Ni3Fe-TPA/NF, TPA = terephthalic acid) shows low η10 of 189, 192, and 265 mV for the oxygen evolution reaction (OER) in 1 M KOH, in 0.5 M NaCl + 1 M KOH, and in seawater + 1 M KOH, respectively. During the OER, surface reconstruction and structural transformation occurred, and active Ni3FeOOH species with more oxygen vacancies were in-situ generated on the Ni3Fe-TPA/NF.

Abstract

As a four-electron transfer reaction, oxygen evolution reaction (OER) is limited by large overpotential and slow kinetics. Here, we in-situ synthesized two-dimensional (2D) Ni-Fe metal-organic framework nanosheets on nickel foam (NixFe-TPA/NF, TPA = terephthalic acid) for oxygen evolution in alkaline and alkaline seawater electrolytes. In 1 M KOH, Ni3Fe-TPA/NF shows a low overpotential (η10) of 189 mV at 10 mA·cm−2 and an ultra-low overpotential of only 260 mV at 500 mA·cm−2. In alkaline seawater, Ni3Fe-TPA/NF still provides impressive OER performance, with an η10 of 265 mV. In-situ Raman characterization results show that the phase transition occurs during the OER, and Ni3FeOOH with more oxygen vacancies is in-situ formed, reducing the OER energy barrier. Density functional theory (DFT) reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining step. In addition, the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER activity. Therefore, the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

Keywords

density functional theory (DFT) calculationNi3FeOOHoxygen evolution reactionseawater electrolysissurface reconstruction

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Nano Research
Volume 17 Issue 4,
April 2024
Pages 2429-2437
DOI: 10.1007/s12274-023-6088-x
Cite this article:
Xiao L, Bai X, Han J, et al. Surface reconstruction and structural transformation of two-dimensional Ni-Fe MOFs for oxygen evolution in seawater media. Nano Research, 2024, 17(4): 2429-2437. https://doi.org/10.1007/s12274-023-6088-x
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Received: 03 July 2023
Revised: 29 July 2023
Accepted: 13 August 2023
Published: 07 September 2023
© Tsinghua University Press 2023
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