Intermittent electrolysis enabling the enhanced efficiency and stability for nitrate reduction

IF 19.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem Pub Date : 2025-05-13 DOI:10.1016/j.chempr.2025.102591

Limin Wu, Libing Zhang, Jiaqi Feng, Shunhan Jia, Ruhan Wang, Xinning Song, Xiaodong Ma, Qinggong Zhu, Xinchen Kang, Qingli Qian, Xiaofu Sun, Buxing Han

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Abstract

Catalyst deactivation is a common issue in catalysis, which restricts its practical applications. Nitrate electroreduction using copper (Cu) catalysts offers an eco-friendly NH₃ production route. However, the NH₃ selectivity and activity decline significantly due to Cu surface reconstruction and compositional changes during electrolysis. Herein, an intermittent reduction strategy is proposed to maintain high efficiency and stability of Cu₂O for NO₃⁻ to NH₃ through applying an alternating on/off electrolysis. The high Faradaic efficiency (FE) (≥90%) and current density (≥110 mA cm⁻²) were maintained at least 200 h, which improved the cycle stability by 40 times compared with relay electrolysis. Detailed experimental studies and theoretical calculations manifest that the composition and structure of Cu catalyst could be recovered periodically via intermittent electrolysis, which facilitated NO₃⁻ adsorption, moderated ∗NO₂ coverage, and balanced ∗H production/consumption, leading to high selectivity toward NH₃ in long-term electrolysis. Further investigation showed that this strategy could also be extended to other Cu-based catalysts.

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间歇电解提高了硝酸还原的效率和稳定性

催化剂失活是催化过程中常见的问题，制约了催化剂的实际应用。使用铜（Cu）催化剂的硝酸电还原提供了一种环保的NH3生产路线。然而，由于电解过程中Cu的表面重构和组分的变化，NH3的选择性和活性显著下降。本文提出了一种间歇还原策略，通过交替开/关电解来保持Cu2O将NO3−转化为NH3的高效率和稳定性。与继电器电解相比，在至少200 h内保持了较高的法拉第效率（FE）（≥90%）和电流密度（≥110 mA cm−2），循环稳定性提高了40倍。详细的实验研究和理论计算表明，通过间歇电解可以周期性地恢复Cu催化剂的组成和结构，促进NO3−吸附，减缓∗NO2覆盖，平衡∗H的产生/消耗，从而在长期电解中对NH3具有高选择性。进一步的研究表明，该策略也可以推广到其他铜基催化剂。

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来源期刊

Chem Environmental Science-Environmental Chemistry

CiteScore

32.40

自引率

1.30%

发文量

281

期刊介绍： Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.