Electrocatalytic Upcycling of Nitrate Wastewater into an Ammonia Fertilizer via an Electrified Membrane
Electrocatalytic Upcycling of Nitrate Wastewater into an Ammonia Fertilizer via an Electrified Membrane
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DOI：
10.1021/acs.est.1c08442
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发表时间：
2022-08-16
影响因子：
11.4
通讯作者：
Zhang, Wen
中科院分区：
文献类型：
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作者：
Gao, Jianan;Shi, Ning;Zhang, Wen
电化学上循环废水中的氮，如硝酸盐（NO3-）和亚硝酸盐（NO2-）成为氨肥料是一个有前途的，但具有挑战性的研究课题，在资源回收和废水处理。本研究提出了一种由CuO@Cu泡沫和聚四氟乙烯（PTFE）膜制成的带电膜，用于将NO3-还原为氨（NH3）并将NH3上循环为（NH 4）（2）SO 4，即一种液体肥料。在阴极膜上，在63.8 +/- 4.4 mAmiddotcm（-2）的分电流密度下，实现了无外加酸/碱消耗的成对电解过程，运行5 h后，进料（150 mM NO3-）中NO3-的去除率为99.9%，NH3的回收率为99.5%。在哈伯-博施法中，氨的回收率和能耗分别为3100 +/- 91 g-（NH 4）（2）SO（4）middotm（-2）middotd（-1）和21.8 +/- 3.8 kWhmiddotkg（-1）-（NH 4）（2）SO（4），几乎超过了工业氨生产成本。密度泛函理论（DFT）计算揭示了Cu 2+到Cu（1+）的原位电化学转化为NO3-还原为NH3提供了高度动态的活性物种。这种带电膜过程被证明可以实现协同的硝酸盐去污和养分回收，具有持久的催化活性和稳定性。
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)(2)SO4, 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 mAmiddotcm(-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)(2)SO(4)middotm(-2)middotd(-1) and 21.8 +/- 3.8 kWhmiddotkg(-1)-(NH4)(2)SO4, 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 Cu(1+ )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.