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<p>A series of ∼20 nm intermetallic Pd<sub>3</sub>Pb nanocubes with tunable surface Pb exposure were synthesized via a facile one-step solvothermal approach, providing an ideal system to investigate the way in which the surface configurations of Pb-rich (Pd<sub>3</sub>Pb/Pb), Pd-rich (Pd<sub>3</sub>Pb/Pd), and standard Pd<sub>3</sub>Pb nanocubes influence the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) mainly through the ligand effect while excluding geometric influences. Electrochemical measurement results indicate that the Pd<sub>3</sub>Pb/Pb catalyst delivered outstanding C1+ selectivity, achieving a high Faradaic efficiency of 96.88% at −0.72 V (vs. RHE), significantly outperforming the Pd<sub>3</sub>Pb/Pd (39.86%) and standard Pd<sub>3</sub>Pb (81.75%) counterparts. <i>In situ</i> FTIR together with DFT calculations further elucidated that Pb incorporation can modulate the electronic structure of Pd via p-d hybridization, leading to the upshift of the d-band center. This will, in return, strengthen the intermediate adsorption ability and lower the energy barriers of the C1+ pathways while effectively suppressing the competing hydrogen evolution reaction. This work establishes a precise surface engineering paradigm of intermetallic nanocrystals for designing high-performance electrocatalysts.</p>

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Precise modulation of surface Pb-rich intermetallic Pd3Pb nanocubes for efficient electrocatalytic CO2 reduction

  • 期刊论文

  • 发表日期：

    2026年3月10日

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  • Junjie Li,
  • Liang Ji,
  • Lei Li,
  • Xiao Li,
  • Xingqiao Wu,
  • Hui Zhang,
  • Deren Yang

摘要

A series of ∼20 nm intermetallic Pd3Pb nanocubes with tunable surface Pb exposure were synthesized via a facile one-step solvothermal approach, providing an ideal system to investigate the way in which the surface configurations of Pb-rich (Pd3Pb/Pb), Pd-rich (Pd3Pb/Pd), and standard Pd3Pb nanocubes influence the CO2 reduction reaction (CO2RR) mainly through the ligand effect while excluding geometric influences. Electrochemical measurement results indicate that the Pd3Pb/Pb catalyst delivered outstanding C1+ selectivity, achieving a high Faradaic efficiency of 96.88% at −0.72 V (vs. RHE), significantly outperforming the Pd3Pb/Pd (39.86%) and standard Pd3Pb (81.75%) counterparts. In situ FTIR together with DFT calculations further elucidated that Pb incorporation can modulate the electronic structure of Pd via p-d hybridization, leading to the upshift of the d-band center. This will, in return, strengthen the intermediate adsorption ability and lower the energy barriers of the C1+ pathways while effectively suppressing the competing hydrogen evolution reaction. This work establishes a precise surface engineering paradigm of intermetallic nanocrystals for designing high-performance electrocatalysts.