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<p>High-entropy alloys (HEAs) have shown great promise in the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) due to their tunable composition and unique physical and chemical properties. However, the role of HEAs in CO<sub>2</sub>RR and the underlying reaction mechanism remain underexplored, particularly through <i>in situ</i> techniques. In this work, we investigate the mechanism of CO<sub>2</sub> reduction on AuAgCuPdPt HEAs using <i>in situ</i> Raman spectroscopy and attenuated total reflectance Fourier-transform infrared (ATR-FTIR) spectroscopy to reveal key intermediates and reaction pathways. Our results demonstrate that within the potential window of −0.2 to −0.7 V vs. reversible hydrogen electrode (RHE), the AuAgCuPdPt HEAs efficiently reduce CO<sub>2</sub> to CO, achieving a Faradaic efficiency (FE) for CO greater than 90%, with a peak FE of 96.5% at −0.3 V vs. RHE. The CO<sub>2</sub><sup>−</sup> intermediate was observed at low potentials, revealing the reaction pathway in the CO<sub>2</sub> reduction process. Additionally, <i>in situ</i> ATR-FTIR results suggest that the introduction of an appropriate amount of Pt metal not only promotes water dissociation to generate protonic hydrogen, but also facilitates the desorption of *CO intermediates. The kinetic isotope effect of hydrogen-deuterium (H-D) confirms that water dissociation acts as a key proton donor in CO<sub>2</sub>RR. Furthermore, the catalyst of AuAgCuPdPt HEAs was applied as cathodes in a Zn-CO<sub>2</sub> battery, achieving 90.23% FE for CO and a power density of 3.474 mW cm<sup>−2</sup>. This study provides new insights into the mechanistic understanding of CO<sub>2</sub> reduction and underscores the importance of <i>in situ</i> spectroscopic techniques for advancing the design of efficient electrocatalysts for CO<sub>2</sub> conversion.</p>

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Pt-optimized AuAgCuPdPt high-entropy alloys for selective CO2 reduction and high-performance Zn-CO2 battery

  • 期刊论文

  • 发表日期：

    2025年11月11日

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  • Li Li,
  • Zengqiang Gao,
  • Wenjing Kang,
  • Yi Feng,
  • Man Hou,
  • Pengfei Yin,
  • Hui Liu,
  • Zhicheng Zhang

摘要

High-entropy alloys (HEAs) have shown great promise in the CO2 reduction reaction (CO2RR) due to their tunable composition and unique physical and chemical properties. However, the role of HEAs in CO2RR and the underlying reaction mechanism remain underexplored, particularly through in situ techniques. In this work, we investigate the mechanism of CO2 reduction on AuAgCuPdPt HEAs using in situ Raman spectroscopy and attenuated total reflectance Fourier-transform infrared (ATR-FTIR) spectroscopy to reveal key intermediates and reaction pathways. Our results demonstrate that within the potential window of −0.2 to −0.7 V vs. reversible hydrogen electrode (RHE), the AuAgCuPdPt HEAs efficiently reduce CO2 to CO, achieving a Faradaic efficiency (FE) for CO greater than 90%, with a peak FE of 96.5% at −0.3 V vs. RHE. The CO2− intermediate was observed at low potentials, revealing the reaction pathway in the CO2 reduction process. Additionally, in situ ATR-FTIR results suggest that the introduction of an appropriate amount of Pt metal not only promotes water dissociation to generate protonic hydrogen, but also facilitates the desorption of *CO intermediates. The kinetic isotope effect of hydrogen-deuterium (H-D) confirms that water dissociation acts as a key proton donor in CO2RR. Furthermore, the catalyst of AuAgCuPdPt HEAs was applied as cathodes in a Zn-CO2 battery, achieving 90.23% FE for CO and a power density of 3.474 mW cm−2. This study provides new insights into the mechanistic understanding of CO2 reduction and underscores the importance of in situ spectroscopic techniques for advancing the design of efficient electrocatalysts for CO2 conversion.