In-situ electrochemical upcycling ammonia from wastewater-level nitrate with a natural hematite electrode: Regulation, performance, and application

Xing Wu, Zhenhui Song, Zhigong Liu, Xi Tang, Fubing Yao, Feiping Zhao, Xiaobo Min, Chong-Jian Tang
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Abstract

Electrochemical reduction of nitrate (NORR) to ammonia (NH/NH) offers promising prospects for NO treatment. However, this process still suffers from NH causing secondary pollution and catalyst deactivation in high-concentration NO wastewater. Herein, a high-performance system comprising a hematite (α-FeO) electrode and a water-resistant membrane achieved 97.6 % NO removal and 81.6 % NH as (NH)SO recovery at wastewater-level NO. The system exhibited an energy consumption of 62.2 kWh·Kg and a Faradaic efficiency of 85.9 %. spectroscopy and electrochemical measurements revealed that α-FeO acted as both an electron transfer mediator for reducing NO to NO and an active center for NH formation via NO/Fe(Ⅱ) redox. Density functional theory calculations identified *HNO to *NO as potential-determining step of NORR. Natural hematite-based system exhibited 74.8 % total inorganic nitrogen removal and 77.1 % NH recovery for actual photovoltaic wastewater. This study provides insights into the development of electrochemical systems for resourcefully treating NO-containing wastewater.
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利用天然赤铁矿电极从废水硝酸盐中就地电化学回收氨:调节、性能和应用
将硝酸盐(NORR)电化学还原为氨(NH/NH)为氮氧化物处理提供了广阔的前景。然而,在高浓度氮废水处理过程中,该工艺仍存在 NH 造成二次污染和催化剂失活的问题。在本文中,一个由赤铁矿(α-FeO)电极和防水膜组成的高性能系统实现了 97.6% 的 NO 去除率和 81.6% 的 NH(NH)SO 回收率。该系统的能耗为 62.2 kWh-Kg,法拉第效率为 85.9%。光谱和电化学测量显示,α-FeO 既是将 NO 还原成 NO 的电子转移介质,也是通过 NO/Fe(Ⅱ)氧化还原形成 NH 的活性中心。密度泛函理论计算确定 *HNO 到 *NO 是 NORR 的电位决定步骤。天然赤铁矿系统对实际光伏废水的无机氮总去除率为 74.8%,NH 回收率为 77.1%。这项研究为开发资源化处理含氮废水的电化学系统提供了启示。
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