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<p>Electrocatalytic NO<sub>3</sub><sup>−</sup> reduction (eNO3RR) is a sustainable method for purification of NO<sub>3</sub><sup>−</sup> wastewater and NH<sub>3</sub> recovery. Cu-based catalysts are promising for eNO3RR, but insufficient active hydrogen (*H) supply and *NO<sub>2</sub> poison of active sites have hindered their performance, and the catalytic mechanism remains ambiguous. Here, we report oxide-derived copper nanosheet arrays (OD-Cu NSs) with residual lattice oxygen and lattice strains to enhance NH<sub>3</sub> synthesis from eNO3RR. It is efficient for NH<sub>3</sub> synthesis with high Faradaic efficiencies of 88.7-99.7% and maximum NH<sub>3</sub> yield of 6.20 mmol·h<sup>−1</sup>·cm<sup>−2</sup> at neutral solution, 10-140 mM NO<sub>3</sub><sup>−</sup> and 50-1500 mA·cm<sup>−2</sup>. Experimental and theoretical results reveal that lattice oxygen regulates the electronic structure of OD-Cu NSs and promotes *NO<sub>2</sub> conversion, while lattice strain enhances *H generation from water dissociation, resulting in the good performance for NH<sub>3</sub> synthesis. The applicability of OD-Cu NSs is proved by the high recovery of ammonia compound from eNO3RR.</p>

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Insights into lattice oxygen and strains of oxide-derived copper for ammonia electrosynthesis from nitrate

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月11日

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  • Qinyue Wu,
  • Xinfei Fan,
  • Bing Shan,
  • Liang Qi,
  • Xie Quan,
  • Yanming Liu

摘要

Electrocatalytic NO3− reduction (eNO3RR) is a sustainable method for purification of NO3− wastewater and NH3 recovery. Cu-based catalysts are promising for eNO3RR, but insufficient active hydrogen (*H) supply and *NO2 poison of active sites have hindered their performance, and the catalytic mechanism remains ambiguous. Here, we report oxide-derived copper nanosheet arrays (OD-Cu NSs) with residual lattice oxygen and lattice strains to enhance NH3 synthesis from eNO3RR. It is efficient for NH3 synthesis with high Faradaic efficiencies of 88.7-99.7% and maximum NH3 yield of 6.20 mmol·h−1·cm−2 at neutral solution, 10-140 mM NO3− and 50-1500 mA·cm−2. Experimental and theoretical results reveal that lattice oxygen regulates the electronic structure of OD-Cu NSs and promotes *NO2 conversion, while lattice strain enhances *H generation from water dissociation, resulting in the good performance for NH3 synthesis. The applicability of OD-Cu NSs is proved by the high recovery of ammonia compound from eNO3RR.