Coupling nitrate capture with ammonia production through bifunctional redox-electrodes.
Coupling nitrate capture with ammonia production through bifunctional redox-electrodes.
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DOI：
10.1038/s41467-023-36318-1
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发表时间：
2023-02-14
影响因子：
16.6
通讯作者：
Su, Xiao
中科院分区：
文献类型：
--
作者：
Kim, Kwiyong;Zagalskaya, Alexandra;Ng, Jing Lian;Hong, Jaeyoung;Alexandrov, Vitaly;Pham, Tuan Anh;Su, Xiao
硝酸盐是工农业活动中普遍存在的水体污染物。与此同时，硝酸盐转化为氨通过将污染物稳定为无碳能量载体和基本化学原料，为氮循环所面临的环境和能源挑战提供了一种有吸引力的解决方案。由于硝酸盐的稀释浓度，质量传输限制是将硝酸盐从水流有效转化为氨的关键障碍。在这里，我们开发了双功能电极，将硝酸盐选择性氧化还原电吸附剂（聚苯胺）与电催化剂（钴氧化物）结合，用于硝酸盐转化为铵。我们证明了协同反应分离硝酸盐，通过单独的电化学控制。可以实现大于70 mg/g的电化学可逆硝酸盐吸收，电子结构计算和光谱测量提供了对氢键对硝酸盐选择性的潜在作用的深入了解。使用含有稀硝酸盐（0.27 mM）的农业瓷砖排水，我们证明了双功能电极可以实现8倍的硝酸盐浓度，24倍的铵生产率提高（108.1 ug h−1 cm−2），以及与稀流中的直接电催化相比，能量效率提高>10倍。我们的研究为模块化硝酸盐修复和氨生产的完全电气化反应分离途径提供了一种通用策略。将硝酸盐捕获与转化为铵相结合是有吸引力的，因为它结合了污染物修复和化学生产。在这里，作者设计了一个双功能氧化还原电极，以实现在一个单一的电化学电池中的硝酸盐铵的反应分离。
Nitrate is a ubiquitous aqueous pollutant from agricultural and industrial activities. At the same time, conversion of nitrate to ammonia provides an attractive solution for the coupled environmental and energy challenge underlying the nitrogen cycle, by valorizing a pollutant to a carbon-free energy carrier and essential chemical feedstock. Mass transport limitations are a key obstacle to the efficient conversion of nitrate to ammonia from water streams, due to the dilute concentration of nitrate. Here, we develop bifunctional electrodes that couple a nitrate-selective redox-electrosorbent (polyaniline) with an electrocatalyst (cobalt oxide) for nitrate to ammonium conversion. We demonstrate the synergistic reactive separation of nitrate through solely electrochemical control. Electrochemically-reversible nitrate uptake greater than 70 mg/g can be achieved, with electronic structure calculations and spectroscopic measurements providing insight into the underlying role of hydrogen bonding for nitrate selectivity. Using agricultural tile drainage water containing dilute nitrate (0.27 mM), we demonstrate that the bifunctional electrode can achieve a 8-fold up-concentration of nitrate, a 24-fold enhancement of ammonium production rate (108.1 ug h−1 cm−2), and a >10-fold enhancement in energy efficiency when compared to direct electrocatalysis in the dilute stream. Our study provides a generalized strategy for a fully electrified reaction-separation pathway for modular nitrate remediation and ammonia production. Coupling nitrate capture with conversion to ammonium is attractive because it combines pollutant remediation and chemical production. Here, the authors design a bifunctional redox-electrode to achieve the reactive separation of nitrate to ammonium in a single electrochemical cell.
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影响因子：
16.6
作者：
He W;Zhang J;Dieckhöfer S;Varhade S;Brix AC;Lielpetere A;Seisel S;Junqueira JRC;Schuhmann W
通讯作者：
Schuhmann W
影响因子：
16.6
作者：
Gao, Qiang;Pillai, Hemanth Somarajan;Huang, Yang;Liu, Shikai;Mu, Qingmin;Han, Xue;Yan, Zihao;Zhou, Hua;He, Qian;Xin, Hongliang;Zhu, Huiyuan
通讯作者：
Zhu, Huiyuan
影响因子：
15.1
作者：
Chauhan, Rohit;Srivastava, Vimal Chandra
通讯作者：
Srivastava, Vimal Chandra
影响因子：
3.7
作者：
Jeon, Tae Hwa;Wu, Zhen-Yu;Wang, Haotian
通讯作者：
Wang, Haotian
影响因子：
15.1
作者：
Cheng, H;Scott, K;Christensen, PA
通讯作者：
Christensen, PA