“…This persistent shift corroborates the enduring stability of the Cu vacancies throughout the cycling process, underscoring the sustained presence of Cu vacancies in the catalyst. Our two-electrode device surpassed all previously reported performances in electrocatalytic nitrate reduction to ammonia 47 – 49 . Fig.…”
Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array electrode generated by in-situ electrochemical reduction, exhibiting superior performance in the electrochemical nitrate reduction reaction benefitting from the triple synergistic modulation. Notably, the defect-rich Cu nanowire array electrode delivers current density ranging from 50 to 1100 mA cm−2 across wide nitrate concentrations (1–100 mM) with Faradaic efficiency over 90%. Operando Synchrotron radiation Fourier Transform Infrared Spectroscopy and theoretical calculations revealed that the defective Cu sites can simultaneously enhance nitrate adsorption, promote water dissociation and suppress hydrogen evolution. A two-electrode system integrating nitrate reduction reaction in industrial wastewater with glycerol oxidation reaction achieves current density of 550 mA cm−2 at −1.4 V with 99.9% ammonia selectivity and 99.9% nitrate conversion with 100 h stability, demonstrating outstanding practicability.
“…This persistent shift corroborates the enduring stability of the Cu vacancies throughout the cycling process, underscoring the sustained presence of Cu vacancies in the catalyst. Our two-electrode device surpassed all previously reported performances in electrocatalytic nitrate reduction to ammonia 47 – 49 . Fig.…”
Nitrate can be electrochemically degraded to produce ammonia while treating sewage while it remains grand challenge to simultaneously realize high Faradaic efficiency and production rate over wide-range concentrations in real wastewater. Herein, we report the defect-rich Cu nanowire array electrode generated by in-situ electrochemical reduction, exhibiting superior performance in the electrochemical nitrate reduction reaction benefitting from the triple synergistic modulation. Notably, the defect-rich Cu nanowire array electrode delivers current density ranging from 50 to 1100 mA cm−2 across wide nitrate concentrations (1–100 mM) with Faradaic efficiency over 90%. Operando Synchrotron radiation Fourier Transform Infrared Spectroscopy and theoretical calculations revealed that the defective Cu sites can simultaneously enhance nitrate adsorption, promote water dissociation and suppress hydrogen evolution. A two-electrode system integrating nitrate reduction reaction in industrial wastewater with glycerol oxidation reaction achieves current density of 550 mA cm−2 at −1.4 V with 99.9% ammonia selectivity and 99.9% nitrate conversion with 100 h stability, demonstrating outstanding practicability.
“…Ammonia is a significant chemical with a wide range of applications in agriculture, textiles, plastics, and pharmaceuticals, etc. − However, industrial NH 3 is synthesized from hydrogen and nitrogen (N 2 ) by the Haber–Bosch method under high temperature (∼400 °C) and pressure (20 MPa), which requires large installations with high input costs and concentrated production. − Recently, from the perspective of environmental friendliness and energy efficiency, the utilization of renewable energy for NH 3 synthesis from N 2 , NO 3 – and nitrite (NO 2 – ) under mild conditions has attracted extensive attention to the alternative Haber–Bosch process, whereas the low water solubility of N 2 and the high bond energy of NN (941 kJ mol –1 ) limit the improvement of the NH 3 yield rate. − Notably, NO 3 – is water-soluble and can be readily reduced by breaking the low bond energy of the NO (204 kJ mol –1 ), which is deemed as a perfect nitrogen source to replace N 2 for the electrochemical synthesis of NH 3 . − Thus, a strategy for the electrochemical reduction of NO 3 – containing wastewater to valuable NH 3 products by renewable electric energy under mild conditions is proposed (Scheme ). Despite these advantages, electrochemical nitrate reduction reaction (NO 3 RR) still faces many challenges due to its sluggish reaction dynamics of the eight-electron transfer (NO 3 – + 6H 2 O + 8e – → NH 3 + 9OH – ) and the byproducts during the complex reduction pathways, which reduce the yield rate and selectivity. − In addition, the hydrogen evolution reaction (HER) competes with the NO 3 RR, which hinders the Faradaic efficiency (FE). − Therefore, it is quite urgent to rationally design and construct electrocatalysts with high catalytic activity and selectivity for NO 3 RR, regarded as an alluring policy with broad prospects …”
“…[26][27][28] Regrettably, the persistent lack of electroactive sites remains a critical challenge that requires urgent attention in the context of electrocatalytic green ammonia synthesis. 29,30 Herein, we present a one-step plasma engraving strategy for the modification of Co 3 O 4 nanorods, resulting in remarkably enriched surface oxygen vacancies (V-Co 3 O 4 ). The plasma engraving of Co 3 O 4 significantly boosted ammonia yield across all potentials, exhibiting a notable increase of up to 67.9% at −0.48 V vs. RHE, for instance.…”
Section: Introductionmentioning
confidence: 99%
“…26–28 Regrettably, the persistent lack of electroactive sites remains a critical challenge that requires urgent attention in the context of electrocatalytic green ammonia synthesis. 29,30…”
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