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在三相界面处通过电子转移和相转移反应偶联实现硝酸盐中电化学选择性氨提取。

Electrochemically Selective Ammonia Extraction from Nitrate by Coupling Electron- and Phase-Transfer Reactions at a Three-Phase Interface.

机构信息

School of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266033, P. R. China.

Department of Civil and Environmental Engineering, New Jersey Institute of Technology, Newark, New Jersey 07102, United States.

出版信息

Environ Sci Technol. 2021 Aug 3;55(15):10684-10694. doi: 10.1021/acs.est.0c08552. Epub 2021 Jul 14.

Abstract

As an attractive alternative to the Haber-Bosch process, an electrochemical process for nitrate (NO) reduction to ammonia (NH) has made great strides in the development of advanced electrocatalysts to suppress the unavoidable H evolution reaction (HER) and side production of N. However, isochronous NH separation and recovery from the mother liquor, especially wastewaters, are awfully neglected in state-of-the-art electrochemical systems. Here, we designed electrochemical three-phase interfaces constructed by a CoP cathode and a flat-sheet gas membrane to achieve NO reduction to ammonia and simultaneous NH recovery in the form of (NH)SO from wastewaters. The partial current density for ammonia yield and its recovery rate were 37.3 mA cm and 306 g NH-N m day, respectively, accompanying 100% NO removal and 99.7% NH extraction. By favoring the originally unfavored side reaction HER, it served as the driving force for NH separation from the wastewater through gas stripping and membrane separation at the three-phase interfaces. Unexpectedly, the timely NH separation could also promote the reduction of NO to ammonia due to the release of much more active sites. From these, we envision that the present electrochemical process can be routinely employed as an effective strategy to address energy and environmental issues with NH recovery from NO wastewater.

摘要

作为哈伯-博施法的一种有吸引力的替代方法,电化学硝酸盐(NO)还原为氨(NH)的过程在开发先进的电催化剂以抑制不可避免的析氢反应(HER)和副产物 N 的产生方面取得了重大进展。然而,从母液(特别是废水)中同步分离和回收氨在最先进的电化学系统中却被严重忽视。在这里,我们设计了由 CoP 阴极和平面片状气体膜构成的电化学三相界面,以实现从废水中将 NO 还原为氨,并以(NH)SO 的形式同时回收 NH。氨的生成和回收的部分电流密度分别为 37.3 mA cm 和 306 g NH-N m day,伴随 100% 的 NO 去除和 99.7% 的 NH 萃取。通过有利于原本不受青睐的析氢反应 HER,它作为通过三相界面的气体汽提和膜分离从废水中分离 NH 的驱动力。出乎意料的是,由于释放出更多的活性位点,及时的 NH 分离也可以促进 NO 还原为氨。由此可见,目前的电化学过程可以作为一种从 NO 废水中回收 NH 的有效策略,用于解决能源和环境问题。

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