State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing, 100875, PR China; School of Mechanical Engineering and Birck Nanotechnology Center, Purdue University, West Lafayette, IN, 47907, USA.
State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing, 100875, PR China.
Chemosphere. 2021 Jul;274:129706. doi: 10.1016/j.chemosphere.2021.129706. Epub 2021 Jan 23.
Electrocatalysis is emerging as a promising alternative to bacterial denitrification for removing nitrate and ammonia from sewage. The technology is highly efficient and robust in actual wastewater treatment scenarios; however, there may be the generation of harmful intermediates (such as nitrite) on the traditional cathode material. In this study, we demonstrated that TiO nanotube arrays can be used as an effective cathode to reduce nitrate to ammonia without generation of nitrite. Alongside this, the addition of chloride ions in the solution can further oxidize ammonia to N. We looked into the key factors influencing the electrocatalytic denitrification, including the current density (2-10 mA/cm), initial pH values (3-11), and types of anions (HCO, Cl, SO). The results showed that 90.8% of nitrate and 59.4% of total nitrogen could be removed in 1.5 h under optimal conditions, with degradation kinetic constants of 1.61 h and 0.79 h, respectively. Furthermore, we investigated the formation of intermediate products and explored the electrocatalytic denitrification mechanism: (a) the surface oxygen vacancies and high specific surface area of TiO nanotube arrays electrode promote the reduction of nitrate to ammonia and N; (b) the active chlorine generated at the anode surface can effectively oxidize ammonium to N.
电催化技术作为一种替代细菌反硝化的方法,在去除污水中的硝酸盐和氨方面正逐渐崭露头角。该技术在实际废水处理场景中具有高效、稳定的特点;然而,在传统阴极材料上可能会产生有害的中间产物(如亚硝酸盐)。在本研究中,我们证明了 TiO 纳米管阵列可用作有效的阴极,可将硝酸盐还原为氨,而不会生成亚硝酸盐。此外,溶液中氯离子的添加可以进一步将氨氧化为 N。我们研究了影响电催化反硝化的关键因素,包括电流密度(2-10 mA/cm)、初始 pH 值(3-11)和阴离子类型(HCO、Cl、SO)。结果表明,在最佳条件下,硝酸盐和总氮的去除率分别达到 90.8%和 59.4%,降解动力学常数分别为 1.61 h 和 0.79 h。此外,我们还研究了中间产物的形成,并探讨了电催化反硝化的机理:(a)TiO 纳米管阵列电极的表面氧空位和高比表面积促进了硝酸盐向氨和 N 的还原;(b)阳极表面生成的活性氯可有效将铵氧化为 N。