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<p>The coordination-directed strategy for fabricating customizable functional metal-organic frameworks (MOFs) offers a promising yet underexplored approach to optimizing their physicochemical properties for target applications. This work exploited the tunable characteristics of MOF structures to successfully synthesize a novel ternary MOF-on-MOF heterostructure (ZIF-67@MOF-74@PBA). The hybrid materials, composed of distinct components, enhance the structural integrity of the MOFs. The pyrolysis-derived bimetallic CoFeP nanoparticles anchored onto hierarchically porous carbon nanomaterials feature hollow structures with high site exposure, <i>in situ</i> grown CNTs that promote efficient mass and charge transport, and synergistic effects from multiple transition metals. The catalyst demonstrates excellent hydrogen evolution reaction (HER) activity (<i>η</i><sub>10</sub> = 107 mV), oxygen evolution reaction (OER) activity (<i>η</i><sub>10</sub> = 231 mV), and overall water splitting performance (1.544 V at 10 mA cm<sup>−2</sup>) in 1.0 M KOH, with remarkable long-term stability. Apparent activation energy measurements and density functional theory calculations confirm that the <i>in situ</i> integration of bimetals and phosphorus doping enhances O–O coupling in the OER and improves hydrogen adsorption/desorption in the HER, thereby optimizing overall catalytic efficiency. This synthesis strategy provides valuable insights and a new approach for the flexible design and practical application of multi-level MOF-on-MOF systems as high-performance electrocatalysts.</p>

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Coordination-directed ternary MOF-on-MOF-derived bimetal phosphide-carbon nanomaterials for efficient overall water splitting

  • 期刊论文

  • 发表日期：

    2025年6月3日

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  • Haoran Wang,
  • Jie Liu,
  • Huijie Ni,
  • Xusheng Wang,
  • Xiangou Zhu,
  • Qipeng Li,
  • Jinjie Qian

摘要

The coordination-directed strategy for fabricating customizable functional metal-organic frameworks (MOFs) offers a promising yet underexplored approach to optimizing their physicochemical properties for target applications. This work exploited the tunable characteristics of MOF structures to successfully synthesize a novel ternary MOF-on-MOF heterostructure (ZIF-67@MOF-74@PBA). The hybrid materials, composed of distinct components, enhance the structural integrity of the MOFs. The pyrolysis-derived bimetallic CoFeP nanoparticles anchored onto hierarchically porous carbon nanomaterials feature hollow structures with high site exposure, in situ grown CNTs that promote efficient mass and charge transport, and synergistic effects from multiple transition metals. The catalyst demonstrates excellent hydrogen evolution reaction (HER) activity (η10 = 107 mV), oxygen evolution reaction (OER) activity (η10 = 231 mV), and overall water splitting performance (1.544 V at 10 mA cm−2) in 1.0 M KOH, with remarkable long-term stability. Apparent activation energy measurements and density functional theory calculations confirm that the in situ integration of bimetals and phosphorus doping enhances O–O coupling in the OER and improves hydrogen adsorption/desorption in the HER, thereby optimizing overall catalytic efficiency. This synthesis strategy provides valuable insights and a new approach for the flexible design and practical application of multi-level MOF-on-MOF systems as high-performance electrocatalysts.