<p>The microstructure and composition of electrocatalysts play a crucial role in determining their oxygen evolution reaction (OER) performance. Herein, we report a controlled self-template synthesis of hollow CoNiFe Prussian blue analogues (PBAs) and their phosphide derivatives with enhanced OER activity. Cobalt-nickel basic acetates with tunable metal ratios were first synthesized via a solvothermal method, followed by anion exchange with potassium hexacyanoferrate to form CoNiFe-PBAs, and subsequent phosphorization to obtain hollow CoNiFe phosphides (CoNiFe-PBA-Ps). Among these, the Co<sub>3</sub>Ni<sub>1</sub>Fe composition exhibits an optimal combination of reduced particle size and hollow architecture, resulting in more exposed active sites and increased electrolyte accessibility. The final Co<sub>3</sub>Ni<sub>1</sub>Fe-PBA-P displays a low overpotential of 273 mV at 10 mA cm<sup>−2</sup> and a Tafel slope of 59 mV dec<sup>−1</sup>, outperforming other Co<sub><i>x</i></sub>Ni<sub><i>y</i></sub>Fe-PBA-Ps and many reported Co, Ni, Fe-based electrocatalysts. DFT calculations confirm that the improved activity stems from the lower energy barriers of the key OER intermediates. This work provides a versatile strategy to design multi-metallic hollow nanostructures with small particle size, offering new insights into the development of high-performance electrocatalysts.</p>

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Controlled self-template synthesis of CoNiFe-PBA hollow structure with enhanced electrocatalytic oxygen evolution reaction activity

  • Songtao Zhang,
  • Yong Chen,
  • Tao Pan,
  • Ying Wei,
  • Yong Li,
  • Zixia Lin,
  • Yecan Pi,
  • Shuai Cao,
  • Yijian Tang,
  • Yongbin Hu,
  • Mingbo Zheng,
  • Huan Pang

摘要

The microstructure and composition of electrocatalysts play a crucial role in determining their oxygen evolution reaction (OER) performance. Herein, we report a controlled self-template synthesis of hollow CoNiFe Prussian blue analogues (PBAs) and their phosphide derivatives with enhanced OER activity. Cobalt-nickel basic acetates with tunable metal ratios were first synthesized via a solvothermal method, followed by anion exchange with potassium hexacyanoferrate to form CoNiFe-PBAs, and subsequent phosphorization to obtain hollow CoNiFe phosphides (CoNiFe-PBA-Ps). Among these, the Co3Ni1Fe composition exhibits an optimal combination of reduced particle size and hollow architecture, resulting in more exposed active sites and increased electrolyte accessibility. The final Co3Ni1Fe-PBA-P displays a low overpotential of 273 mV at 10 mA cm−2 and a Tafel slope of 59 mV dec−1, outperforming other CoxNiyFe-PBA-Ps and many reported Co, Ni, Fe-based electrocatalysts. DFT calculations confirm that the improved activity stems from the lower energy barriers of the key OER intermediates. This work provides a versatile strategy to design multi-metallic hollow nanostructures with small particle size, offering new insights into the development of high-performance electrocatalysts.