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<p>Electrochemical nitrate (NO<sub>3</sub><sup>−</sup>) reduction reaction (eNO<sub>3</sub>RR) to ammonia (NH<sub>3</sub>) provides a promising route for both water conservation and green ammonia synthesis. Although various catalysts were designed for the eNO<sub>3</sub>RR and great achievements have been achieved, it is still a challenge to realize selective eNO<sub>3</sub>RR to NH<sub>3</sub> at low concentration for the competing hydrogen evolution reaction (HER) and poor mass transfer of NO<sub>3</sub><sup>−</sup>. Herein, we designed a tandem catalyst of Pd nanoparticle loaded Cu<sub>2</sub>O hierarchical nanofiber (Pd-Cu<sub>2</sub>O) to improve eNO<sub>3</sub>RR performance at low nitrate concentration. The Pd-Cu<sub>2</sub>O shows a faraday efficiency (FE) of 95.80% and an ammonia selectivity of 97.34% at a comparatively low applied potential of −0.15&#xa0;V versus RHE with low concentration. Besides, it exhibits excellent nitrate removal effects, the residual concentration of nitrate–N was only 7.22&#xa0;ppm at −0.15&#xa0;V. Electrochemical characterizations indicate that the abundant secondary heterojunction structures and the tandem effects of Pd-Cu<sub>2</sub>O synergistically accelerate the transfer and conversion of NO<sub>3</sub><sup>−</sup> and improve the dynamic of eNO<sub>3</sub>RR at low concentration. Furthermore, the operando electrochemical impedance spectroscopy (EIS) and density functional theory (DFT) calculations suggested the tandem effects of Pd-Cu<sub>2</sub>O improved the adsorption of NO<sub>3</sub><sup>−</sup> and *H and thus promoted the dynamics of eNO<sub>3</sub>RR at low concentration. The findings highlight the tandem effects of Pd-Cu<sub>2</sub>O and provide an effective strategy for designing electrocatalysts that can be applied to low concentration and low applied potential conditions.</p> Graphical abstract <p></p>

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A Cu2O-Pd dual active sites tandem catalyst enables efficient nitrate reduction to ammonia at low concentration

  • 期刊论文

  • 发表日期：

    2025年4月16日

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  • Meng-Yuan Yue,
  • Ya-Fei Liu,
  • You-Hai Cao,
  • Ya-Ru Jiang,
  • Kai-Zheng Dong,
  • Qi-Hui Yuan,
  • Yi-Jing Wang

摘要

Electrochemical nitrate (NO3−) reduction reaction (eNO3RR) to ammonia (NH3) provides a promising route for both water conservation and green ammonia synthesis. Although various catalysts were designed for the eNO3RR and great achievements have been achieved, it is still a challenge to realize selective eNO3RR to NH3 at low concentration for the competing hydrogen evolution reaction (HER) and poor mass transfer of NO3−. Herein, we designed a tandem catalyst of Pd nanoparticle loaded Cu2O hierarchical nanofiber (Pd-Cu2O) to improve eNO3RR performance at low nitrate concentration. The Pd-Cu2O shows a faraday efficiency (FE) of 95.80% and an ammonia selectivity of 97.34% at a comparatively low applied potential of −0.15 V versus RHE with low concentration. Besides, it exhibits excellent nitrate removal effects, the residual concentration of nitrate–N was only 7.22 ppm at −0.15 V. Electrochemical characterizations indicate that the abundant secondary heterojunction structures and the tandem effects of Pd-Cu2O synergistically accelerate the transfer and conversion of NO3− and improve the dynamic of eNO3RR at low concentration. Furthermore, the operando electrochemical impedance spectroscopy (EIS) and density functional theory (DFT) calculations suggested the tandem effects of Pd-Cu2O improved the adsorption of NO3− and *H and thus promoted the dynamics of eNO3RR at low concentration. The findings highlight the tandem effects of Pd-Cu2O and provide an effective strategy for designing electrocatalysts that can be applied to low concentration and low applied potential conditions.

Graphical abstract