Reactive Separation of Ammonia from Wastewater Nitrate via Molecular Electrocatalysis
Reactive Separation of Ammonia from Wastewater Nitrate via Molecular Electrocatalysis
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通过分子电催化反应分离废水硝酸盐中的氨
DOI：
10.1021/acs.estlett.3c00205
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发表时间：
2023
影响因子：
10.9
通讯作者：
Tarpeh, William A.
中科院分区：
文献类型：
--
作者：
Liu, Matthew J.;Miller, Dean M.;Tarpeh, William A.
氨捕集选择性电化学法将硝酸盐转化为氨，既可修复硝酸盐污染的废水，又可补充Haber-Bosch合成氨生产。均相分子催化剂在废水处理以及更广泛的反应分离过程中仍未得到充分开发。尽管分子催化剂的反应活性是可调的，但有两个障碍阻碍了它们在废水硝酸盐处理和氨回收方面的广泛应用。第一个障碍是缺乏关于硝酸盐还原分子催化剂在真实废水中的反应活性和选择性的报道。第二个障碍是需要分离催化剂、催化产物和处理后的废水。在这项研究中，我们在几种配置中使用电化学汽提作为反应分离单元过程来解决实施的两个障碍。使用均相分子硝酸盐还原催化剂Co(DIM)，我们证明了城市污水处理厂二级出水中硝酸盐的脱除率为70%，氨的选择性为98.5%，从而产生了高纯度的氨产品(硫酸铵)。这些实验构成了分子催化还原真实废水中硝酸盐的新演示，并突出了在反应分离中的电化学工程机会，以评估废水资源。这项工作推动了环境研究朝着联合国清洁水可持续发展目标(SDG 6)和负责任的消费和生产(SDG 12)的方向发展。
Selective electrochemical conversion of nitrate to ammonia with ammonia capture can simultaneously remediate nitrate-polluted wastewater and supplement Haber-Bosch ammonia production. Homogeneous molecular catalysts remain underexplored in wastewater treatment and, more generally, in reactive separation processes. Despite the tunable reactivity of molecular catalysts, two barriers prevent their widespread implementation for wastewater nitrate treatment and ammonia recovery. The first barrier is the lack of reports of reaction activity and selectivity of nitrate reduction molecular catalysts in real wastewaters. The second barrier is the need to separate the catalyst, catalytic product, and treated wastewater. In this study, we employ electrochemical stripping in several configurations as a reactive separation unit process to address both barriers to implementation. Using the homogeneous molecular nitrate reduction catalyst Co(DIM), we demonstrate >70% removal of nitrate from municipal wastewater treatment plant secondary effluent with >98.5% selectivity to ammonia, leading to the generation of a high-purity ammonia product (ammonium sulfate). These experiments constitute a novel demonstration of molecular catalysis for nitrate reduction in real wastewater and highlight electrochemical engineering opportunities in reactive separations to valorize wastewater resources. This work advances environmental research toward United Nations Sustainable Development Goals (SDGs) for Clean Water (SDG 6) and Responsible Consumption and Production (SDG 12).
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