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Efficient conversion of low-concentration nitrate sources into ammonia on a Ru-dispersed Cu nanowire electrocatalyst
Nature Nanotechnology ( IF 38.3 ) Pub Date : 2022-05-02 , DOI: 10.1038/s41565-022-01121-4
Feng-Yang Chen 1 , Zhen-Yu Wu 1 , Srishti Gupta 2 , Daniel J Rivera 2 , Sten V Lambeets 3 , Stephanie Pecaut 1 , Jung Yoon Timothy Kim 1 , Peng Zhu 1 , Y Zou Finfrock 4 , Debora Motta Meira 5 , Graham King 5 , Guanhui Gao 6 , Wenqian Xu 7 , David A Cullen 8 , Hua Zhou 7 , Yimo Han 9 , Daniel E Perea 10 , Christopher L Muhich 2, 11 , Haotian Wang 1, 9, 12
Affiliation  

Electrochemically converting nitrate ions, a widely distributed nitrogen source in industrial wastewater and polluted groundwater, into ammonia represents a sustainable route for both wastewater treatment and ammonia generation. However, it is currently hindered by low catalytic activities, especially under low nitrate concentrations. Here we report a high-performance Ru-dispersed Cu nanowire catalyst that delivers an industrial-relevant nitrate reduction current of 1 A cm–2 while maintaining a high NH3 Faradaic efficiency of 93%. More importantly, this high nitrate-reduction catalytic activity enables over a 99% nitrate conversion into ammonia, from an industrial wastewater level of 2,000 ppm to a drinkable water level <50 ppm, while still maintaining an over 90% Faradaic efficiency. Coupling the nitrate reduction effluent stream with an air stripping process, we successfully obtained high purity solid NH4Cl and liquid NH3 solution products, which suggests a practical approach to convert wastewater nitrate into valuable ammonia products. Density functional theory calculations reveal that the highly dispersed Ru atoms provide active nitrate reduction sites and the surrounding Cu sites can suppress the main side reaction, the hydrogen evolution reaction.



中文翻译:

在Ru分散的Cu纳米线电催化剂上将低浓度硝酸盐源高效转化为氨

将硝酸根离子(工业废水和受污染地下水中广泛分布的氮源)电化学转化为氨是废水处理和氨生成的可持续途径。然而,目前它受到低催化活性的阻碍,特别是在低硝酸盐浓度下。在这里,我们报告了一种高性能的 Ru 分散铜纳米线催化剂,该催化剂可提供 1 A cm –2的工业相关硝酸盐还原电流,同时保持高 NH 3法拉第效率为93%。更重要的是,这种高硝酸盐还原催化活性能够将超过 99% 的硝酸盐转化为氨,从 2,000 ppm 的工业废水水平到 <50 ppm 的饮用水水平,同时仍保持超过 90% 的法拉第效率。将硝酸盐还原流出物流与空气汽提工艺相结合,我们成功地获得了高纯度固体 NH 4 Cl 和液体 NH 3溶液产品,这为将废水硝酸盐转化为有价值的氨产品提供了一种实用的方法。密度泛函理论计算表明,高度分散的Ru原子提供了活性硝酸盐还原位点,而周围的Cu位点可以抑制主要副反应,即析氢反应。

更新日期:2022-05-02
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