Chinese Journal of Catalysis ›› 2024, Vol. 61: 192-204.DOI: 10.1016/S1872-2067(24)60030-6

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Constructing amorphous/crystalline NiFe-MOF@NiS heterojunction catalysts for enhanced water/seawater oxidation at large current density

Xianbiao Hou,1, Chen Yu,1, Tengjia Ni, Shucong Zhang, Jian Zhou, Shuixing Dai, Lei Chu*(), Minghua Huang*()   

  1. School of Materials Science and Engineering, Ocean University of China, Qingdao 266100, Shandong, China
  • Received:2024-01-21 Accepted:2024-03-26 Online:2024-06-18 Published:2024-06-20
  • Contact: * E-mail: chulei@ouc.edu.cn (L. Chu), huangminghua@ouc.edu.cn (M. Huang).
  • About author:

    1Contributed equally to this work.

  • Supported by:
    National Natural Science Foundation of China(52261145700);National Natural Science Foundation of China(22279124);Natural Science Foundation of Shandong Province(ZR2022ZD30);Qingdao New Energy Shandong Laboratory Open Project(QNESL OP202307);Fundamental Research Funds for the Central Universities(202262010)

Abstract:

Developing metal-organic frameworks (MOF) based catalysts with high activity and chlorine corrosion resistance is of paramount importance for seawater oxidation at large current density. Herein, we report a heterogeneous structure coupling NiFe-MOF nanoparticles with NiS nanosheets onto Ni foam (denoted as the NiFe-MOF@NiS/NF) via the mild strategy involving sulfur-modified corrosion and electrodeposition treatment. The constructed amorphous/crystalline interfaces could not only facilitate the adequate infiltration of electrolyte and release of O2 bubbles at large current densities, but also significantly improve the charge transfer from NiFe-MOF to NiS and the adsorption/desorption capacity of oxygen intermediates. Intriguingly, during oxygen evolution reaction process, the sulfate film formed by the self-reconstruction could remarkably inhibit the adsorption of Cl- ions on the catalyst surface in the seawater electrolytes. Benefiting from the robust corrosion resistance, unique amorphous/crystalline interfaces, and the charge redistribution, the well-designed NiFe-MOF@NiS/NF exhibits the low overpotential of 346 and 355 mV under a high current density of 500 mA cm-2 in alkaline water and seawater electrolytes, respectively. More importantly, the as-fabricated NiFe-MOF@NiS/NF demonstrates prolonged stability and durability, lasting over 600 h at a current density of 100 mA cm-2 in both electrolytes. This study enriches the understanding of electronic structure modulation and chlorine corrosion resistance in seawater, providing broad prospects for designing advanced MOF-based catalysts.

Key words: Metal-organic framework, Amorphous/crystalline heterointerface, Electrocatalyst, Water/seawater oxidation, Large current density