通过带电膜将硝酸盐废水电催化升级为氨肥,Environmental Science & Technology

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通过带电膜将硝酸盐废水电催化升级为氨肥
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2022-07-21 , DOI: 10.1021/acs.est.1c08442
Jianan Gao _{1,

2} , Ning Shi ₁ , Yifan Li ₁ , Bo Jiang ₁ , Taha Marhaba ₂ , Wen Zhang ₂

Affiliation

_{将硝酸盐（NO 3}^-）和亚硝酸盐（NO ₂^- ）等废水氮电化学升级为氨肥是资源回收和废水处理领域一个有前途但具有挑战性的研究课题。本研究介绍了一种由 CuO@Cu 泡沫和聚四氟乙烯 (PTFE) 膜制成的带电膜，用于将 NO ₃^–还原为氨 (NH ₃ ) 并将 NH ₃升级为(NH ₄ ) ₂ SO ₄利用。^{在 63.8 ± 4.4 mA·cm –2}的部分电流密度下实现了无外部酸碱消耗的配对电解过程在阴极膜上，在运行 5 小时后去除了进料（150 mM NO ₃^{- ）中 99.9% 的 NO}₃^{- ，NH}₃回收率为 99.5%。回收率和能耗分别为 3100 ± 91 g-(NH ₄ ) ₂ SO ₄ ·m ^–2 ·d ^–1和 21.8 ± 3.8 kWh·kg ^–1 -(NH ₄ ) ₂ SO ₄，几乎超过了Haber-Bosch 工艺中的工业氨生产成本。密度泛函理论 (DFT) 计算揭示了Cu ²⁺原位电化学转化为 Cu^{1+为 NO}₃^–还原为 NH ₃提供了高度动态的活性物质。这种带电膜工艺被证明可以实现协同的硝酸盐净化和养分回收，并具有持久的催化活性和稳定性。

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Electrocatalytic Upcycling of Nitrate Wastewater into an Ammonia Fertilizer via an Electrified Membrane

Electrochemically upcycling wastewater nitrogen such as nitrate (NO₃^–) and nitrite (NO₂^–) into an ammonia fertilizer is a promising yet challenging research topic in resource recovery and wastewater treatment. This study presents an electrified membrane made of a CuO@Cu foam and a polytetrafluoroethylene (PTFE) membrane for reducing NO₃^– to ammonia (NH₃) and upcycling NH₃ into (NH₄)₂SO₄, a liquid fertilizer for ready-use. A paired electrolysis process without external acid/base consumption was achieved under a partial current density of 63.8 ± 4.4 mA·cm^–2 on the cathodic membrane, which removed 99.9% NO₃^– in the feed (150 mM NO₃^–) after a 5 h operation with an NH₃ recovery rate of 99.5%. A recovery rate and energy consumption of 3100 ± 91 g-(NH₄)₂SO₄·m^–2·d^–1 and 21.8 ± 3.8 kWh·kg^–1-(NH₄)₂SO₄, respectively, almost outcompete the industrial ammonia production cost in the Haber–Bosch process. Density functional theory (DFT) calculations unraveled that the in situ electrochemical conversion of Cu²⁺ into Cu¹⁺ provides highly dynamic active species for NO₃^– reduction to NH₃. This electrified membrane process was demonstrated to achieve synergistic nitrate decontamination and nutrient recovery with durable catalytic activity and stability.

更新日期：2022-07-21

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