Electrochemical reduction of nitrate on boron-doped diamond electrodes: Effects of surface termination and boron-doping level

被引:45
作者
Kuang, Peijing [1 ,2 ,3 ]
Natsui, Keisuke [3 ]
Feng, Chuanping [4 ]
Einaga, Yasuaki [3 ,5 ]
机构
[1] Dalian Minzu Univ, Key Lab Biotechnol & Bioresources Utilizat, Minist Educ, 18 Liaohe Rd West, Dalian 116600, Peoples R China
[2] Dalian Minzu Univ, Coll Environm & Resources, Dalian 116600, Peoples R China
[3] Keio Univ, Dept Chem, 3-14-1 Hiyoshi, Yokohama, Kanagawa 2238522, Japan
[4] China Univ Geosci Beijing, Sch Water Resources & Environm, 29 Xue Yuan Rd, Beijing 100083, Peoples R China
[5] JST ACCEL, 3-14-1 Hiyoshi, Yokohama, Kanagawa 2238522, Japan
关键词
Nitrate reduction; Surface termination; Boron-doping level; Nitrogen gas selectivity; Investigation of mechanism; IMPEDANCE SPECTROSCOPY; OXIDATION; BEHAVIOR; GROUNDWATER; HYDROGEN; NITRITE; WATER;
D O I
10.1016/j.chemosphere.2020.126364
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study is among the first to systematically study the electrochemical reduction of nitrate on boron-doped diamond (BDD) films with different surface terminations and boron-doping levels. The highest nitrate reduction efficiency was 48% and the highest selectivity in the production of nitrogen gas was 44.5%, which were achieved using a BDD electrode with a hydrogen-terminated surface and a B/C ratio of 1.0%. C-H bonds served as the anchor points for attracting NO anions close to the electrode surface, and thus accelerating the formation of NO3(ads)-. Compared to oxygen termination, hydrogen-terminated BDD exhibited higher electrochemical reactivity for reducing nitrate, resulting from the formation of shallow acceptor states and small interfacial band bending. The hydrophobicity of the hydrogen-terminated BDD inhibited water electrolysis and the subsequent adsorption of atomic hydrogen, leading to increased selectivity in the production of nitrogen gas. A BDD electrode with a boron-doping level of 1.0% increased the density of acceptor states, thereby enhancing the conductivity and promoting the formation of C-H bonds after the cathodic reduction pretreatment leading to the direct reduction of nitrate. (C) 2020 Elsevier Ltd. All rights reserved.
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页数:11
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