School of Water Resources and Environment, China University of Geosciences (Beijing), 29 Xue Yuan Road, Haidian District, Beijing 100083, China; Department of Chemistry, Keio University, 3-14-1 Hiyoshi, Yokohama 223-8522, Japan.
Department of Chemistry, Keio University, 3-14-1 Hiyoshi, Yokohama 223-8522, Japan.
Chemosphere. 2018 Nov;210:524-530. doi: 10.1016/j.chemosphere.2018.07.039. Epub 2018 Jul 11.
The electrochemical nitrate reduction by using boron-doped diamond (BDD) and copper (Cu) electrodes was investigated at various potentials. Product selectivity of nitrate reduction was strongly dependent on the applied potential for both electrodes. The highest selectivity of nitrogen gas production was obtained at -2.0 V (vs. Ag/AgCl) by using a BDD electrode with a faradaic efficiency as high as 45.2%. Compared with Cu electrode, nitrate reduction on BDD electrode occurred at more positive potential, and the production of nitrogen gas was larger. The transformation of surface-adsorbed nitrate into molecular nitrogen would be accelerated on BDD electrode with hindering nitrite production. In addition, low concentration of surface-adsorbed hydrogen on the BDD would also retard the ammonia generation, leading to increase in the selectivity of nitrogen gas formation. Meanwhile, BDD electrode could hinder the hydrogen evolution reaction, which enhanced the efficiency for nitrate reduction and decreased energy consumption. BDD electrode has excellent stability to remain better performance for reducing nitrate during electrolysis without any variation of surface morphology or chemical components.
采用掺硼金刚石(BDD)和铜(Cu)电极在不同电位下研究了电化学硝酸盐还原。两种电极的硝酸盐还原产物选择性强烈依赖于施加的电位。使用 BDD 电极在-2.0 V(相对于 Ag/AgCl)时可获得最高的氮气选择性,法拉第效率高达 45.2%。与 Cu 电极相比,BDD 电极上的硝酸盐还原发生在更正的电位下,氮气的产量更大。BDD 电极上表面吸附的硝酸盐向氮气的转化会加速,从而抑制亚硝酸盐的生成。此外,BDD 上表面吸附的低浓度氢气也会阻碍氨的生成,从而提高氮气形成的选择性。同时,BDD 电极可以抑制析氢反应,从而提高硝酸盐还原效率,降低能耗。BDD 电极具有出色的稳定性,在电解过程中不会改变表面形态或化学组成,从而保持更好的硝酸盐还原性能。