<p>Electrochemical nitrate reduction (NO<sub>3</sub>RR) enables the conversion of nitrate into value-added NH<sub>3</sub> under ambient conditions, providing a promising solution for addressing environmental issues while simultaneously producing useful chemicals. However, the efficiency and selectivity of the NO<sub>3</sub>RR are still limited by the complex multi-electron transfer process and competitive hydrogen evolution reaction. Herein, a pulse electrolysis strategy based on an AgCu bimetallic telluride nanowire catalyst (denoted as CuAgTe NWs) was developed, in which the NO<sub>3</sub>RR is decomposed into two distinct tandem reduction processes: “NO<Stack> <sub>3</sub> <sup>−</sup> </Stack> → NO<Stack> <sub>2</sub> <sup>−</sup> </Stack>” and “NO<Stack> <sub>2</sub> <sup>−</sup> </Stack> → NH<sub>3</sub>”. Experimental and theoretical studies reveal that the introduction of Ag significantly increases the onset potential for NO<Stack> <sub>2</sub> <sup>−</sup> </Stack> generation and also reduces the energy barrier for hydrogenation on Cu, thereby achieving nitrite enrichment at higher potentials and subsequent rapid conversion at low potentials. As expected, the CuAgTe NWs exhibited excellent NO<sub>3</sub>RR performance, with an ammonia Faradaic efficiency of 98.3% and yield rate of 8.296 mg h<sup>−1</sup> cm<sup>−2</sup>. This study provides new insights for the development of efficient tandem catalysis protocols for the NO<sub>3</sub>RR.</p>

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Tandem catalysis facilitates nitrate-to-ammonia electroreduction on AgCu telluride nanowires

  • Zhenyang Meng,
  • Shixian Wang,
  • Yong Li,
  • Yu Fan,
  • Xiang Yu,
  • Xue Wang,
  • Xiaotian Guo,
  • Yecan Pi,
  • Huan Pang

摘要

Electrochemical nitrate reduction (NO3RR) enables the conversion of nitrate into value-added NH3 under ambient conditions, providing a promising solution for addressing environmental issues while simultaneously producing useful chemicals. However, the efficiency and selectivity of the NO3RR are still limited by the complex multi-electron transfer process and competitive hydrogen evolution reaction. Herein, a pulse electrolysis strategy based on an AgCu bimetallic telluride nanowire catalyst (denoted as CuAgTe NWs) was developed, in which the NO3RR is decomposed into two distinct tandem reduction processes: “NO 3 → NO 2 ” and “NO 2 → NH3”. Experimental and theoretical studies reveal that the introduction of Ag significantly increases the onset potential for NO 2 generation and also reduces the energy barrier for hydrogenation on Cu, thereby achieving nitrite enrichment at higher potentials and subsequent rapid conversion at low potentials. As expected, the CuAgTe NWs exhibited excellent NO3RR performance, with an ammonia Faradaic efficiency of 98.3% and yield rate of 8.296 mg h−1 cm−2. This study provides new insights for the development of efficient tandem catalysis protocols for the NO3RR.