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<p>Ni single-atom catalysts have been widely explored for CO<sub>2</sub> reduction, however, their practical application is often hampered by complex synthesis and instability at high current densities. In this context, well-dispersed nickel nanoparticles present a compelling alternative, offering both facile fabrication and robust performance. Herein, a hierarchical catalyst comprising nickel nanoparticles encapsulated within a nitrogen-doped carbon shell on a hollow-rod carbon substrate (denoted as Ni<sub>NP</sub>-BCN@C) was designed. The hollow-rod architecture maximizes the exposure of nickel nanoparticles as active sites, while the nitrogen-doped carbon shell effectively modulates the electronic environment of the metallic Ni, suppressing the competing hydrogen evolution reaction and promoting CO<sub>2</sub> activation. The catalyst exhibits exceptional CO<sub>2</sub>-to-CO conversion, with a Faradaic efficiency exceeding 90% at −0.83 V <i>vs.</i> RHE in an H-cell and remarkable stability over 32 h. When evaluated in a flow-cell configuration, it achieves a CO Faradaic efficiency &gt; 98% at a current density of 300 mA·cm<sup>−2</sup>, corresponding to a high turnover frequency of ∼93,579 h<sup>−1</sup>. <i>In situ</i> Fourier transform infrared spectroscopy revealed intensified bands for key intermediates (*COOH and COO<sup>−</sup>), confirming enhanced CO<sub>2</sub> adsorption and activation. This work showcases a scalable and efficient catalyst design, highlighting the synergy between structural engineering and electronic modulation for advanced CO<sub>2</sub> electroreduction.</p>

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Engineering highly-exposed nickel nanoparticles within a nitrogen-doped carbon matrix for efficient CO2 electroreduction to CO

  • 期刊论文

  • 发表日期：

    2026年4月2日

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  • Can Yang,
  • Bingyuan Dai,
  • Minxuan Wang,
  • Hui Xu,
  • Hongbing Zheng,
  • Cheng Ma,
  • Licheng Ling,
  • Jitong Wang

摘要

Ni single-atom catalysts have been widely explored for CO2 reduction, however, their practical application is often hampered by complex synthesis and instability at high current densities. In this context, well-dispersed nickel nanoparticles present a compelling alternative, offering both facile fabrication and robust performance. Herein, a hierarchical catalyst comprising nickel nanoparticles encapsulated within a nitrogen-doped carbon shell on a hollow-rod carbon substrate (denoted as NiNP-BCN@C) was designed. The hollow-rod architecture maximizes the exposure of nickel nanoparticles as active sites, while the nitrogen-doped carbon shell effectively modulates the electronic environment of the metallic Ni, suppressing the competing hydrogen evolution reaction and promoting CO2 activation. The catalyst exhibits exceptional CO2-to-CO conversion, with a Faradaic efficiency exceeding 90% at −0.83 V vs. RHE in an H-cell and remarkable stability over 32 h. When evaluated in a flow-cell configuration, it achieves a CO Faradaic efficiency > 98% at a current density of 300 mA·cm−2, corresponding to a high turnover frequency of ∼93,579 h−1. In situ Fourier transform infrared spectroscopy revealed intensified bands for key intermediates (*COOH and COO−), confirming enhanced CO2 adsorption and activation. This work showcases a scalable and efficient catalyst design, highlighting the synergy between structural engineering and electronic modulation for advanced CO2 electroreduction.