掺氮金刚石电极性能及其氧化降解硝基苯研究

doi:10.15541/jim20170290

无机材料学报 ›› 2018, Vol. 33 ›› Issue (5): 565-569.DOI: 10.15541/jim20170290 CSTR: 32189.14.10.15541/jim20170290

所属专题：电催化研究

掺氮金刚石电极性能及其氧化降解硝基苯研究

严世胜¹, 彭鸿雁¹, 赵志斌¹, 潘孟美¹, 羊大立¹, 阿金华¹, 叶国林¹, 王崇太², 郭心玮²

海南师范大学 1. 物理与电子工程学院;2. 化学与化工学院, 海口 571158

收稿日期:2017-06-08 修回日期:2017-10-02 出版日期:2018-05-20 网络出版日期:2018-04-26
作者简介:严世胜(1972-), 男, 副教授. E-mail: 605840548@qq.com
基金资助:
国家自然科学基金(51262007);海南省自然科学基金(617104, 20165196)

Nitrogen-doped Diamond Electrode Property and Anodic Catalytic Degradation of Nitrobenzene

YAN Shi-Sheng¹, PENG Hong-Yan¹, ZHAO Zhi-Bin¹, PAN Meng-Mei¹, YANG Da-Li¹, A Jin-Hua¹, YE Guo-Lin¹, WANG Chong-Tai², GUO Xin-Wei²

1. School of Physics and Electronic Engineering, Hainan Normal University, Haikou 571158, China;
2. School of Chemistry and Chemical Engineering, Hainan Normal University, Haikou 571158, China

Received:2017-06-08 Revised:2017-10-02 Published:2018-05-20 Online:2018-04-26
About author:YAN Shi-Sheng. E-mail: 605840548@qq.com
Supported by:
National Natural Science Foundation of China (51262007);Natural Science Foundation of Hainan Province (617104, 20165196)

摘要/Abstract

摘要：

采用热阴极直流辉光等离子体化学气相沉积法制备亚微米晶氮掺杂金刚石膜(NDD), 采用SEM分析样品的表面形貌, 分别用Hall测试和循环伏安法测试氮掺杂金刚石电极的电学和电化学性能。实验结果表明, 当氮气流量低于30 sccm时, 膜的电导率随氮气流量的增大略有提高; 氮气流量继续增大则电导率迅速下降, 电导率最大为5.091 S/cm。氮掺杂金刚石电极具有较好的伏安性能, 在酸性、中性和碱性介质中均具有较宽的电位窗口和较低的背景电流。以硝基苯为目标污染物测试NDD材料作为阳极氧化降解的电催化性能。在0.1 mol/L Na₂SO₄溶液的支持电解质中, 以氮掺杂金刚石为阳极降解0.5 mmol/L的硝基苯, 反应时间300 min, 硝基苯的降解率达到94%, 化学需氧量(COD)去除率约68%。

关键词: 热阴极直流辉光等离子体化学气相沉积, 掺氮亚微米晶金刚石电极, 电催化氧化, 硝基苯降解

Abstract:

A series of nitrogen-doped diamond (NDD) film electrodes were synthesis by hot cathode direct current plasma chemical vapor deposition (HCDCPCVD) method with varied ratio CH₄/H₂/N₂ gas mixture. Morphologies of diamond films were characterized by SEM. Electrical and electrochemical properties of nitrogen-doped diamond electrodes were characterized by Hall test and cyclic voltammetry. The results show that when the nitrogen flow rate is less than 30 sccm, the conductivity of the film increases slightly with the increase of the nitrogen flow rate. As the nitrogen flow rate continues to increase, the conductivity decreases rapidly, showing the maximum electro- conductibility of 5.091 S/cm. The nitrogen-doped diamond electrode has good voltammetric performance with a wide potential window and a low background current in acidic, neutral and alkaline media. Properties of anodic oxidation degradation of nitrogen-doped diamond electrodes were tested using nitrobenzene as target pollutant. In the supporting electrolyte of 0.1 mol/L Na₂SO₄ solution, 0.5 mmol/L nitrobenzene is decomposed using the nitrogen- doped diamond as anode. After reaction for 300 min, degradation rate of the nitrobenzene reaches 94%, and COD (Chemical Oxygen Demand) removal rate is about 68%.

Key words: hot cathode direct current glow plasma chemical vapor deposition, nitrogen-doped submicron-crystalline diamond electrode, electrocatalytic oxidation, nitrobenzene degradation

中图分类号:

O646

严世胜, 彭鸿雁, 赵志斌, 潘孟美, 羊大立, 阿金华, 叶国林, 王崇太, 郭心玮. 掺氮金刚石电极性能及其氧化降解硝基苯研究[J]. 无机材料学报, 2018, 33(5): 565-569.

YAN Shi-Sheng, PENG Hong-Yan, ZHAO Zhi-Bin, PAN Meng-Mei, YANG Da-Li, A Jin-Hua, YE Guo-Lin, WANG Chong-Tai, GUO Xin-Wei. Nitrogen-doped Diamond Electrode Property and Anodic Catalytic Degradation of Nitrobenzene[J]. Journal of Inorganic Materials, 2018, 33(5): 565-569.

图/表 6

图1 不同氮气流量下制备的掺氮亚微米晶金刚石膜的SEM照片

Fig.1 SEM images of diamond films deposited at different N2 flux rates(a) 0 sccm; (b) 10 sccm; (c) 20 sccm; (d) 30 sccm; (e) 40 sccm; (f) 50 sccm

图2 掺氮亚微米晶金刚石膜电导率随氮气流量变化曲线

Fig. 2 Electrical conductivity of diamond films deposited at different N2 flux rates

图3 不同氮流量制备NDD电极循环伏安图(0.1 mol/L Na2SO4; 扫速100 mV∙s-1)

Fig. 3 Cyclic voltammogram of the NDD electrodes deposited at different N2 flux rates (0.1 mol/L Na2SO4; scan rate: 100 mV∙s-1)(b) 10 sccm; (c) 20 sccm; (d) 30 sccm; (e) 40 sccm; (f) 50 sccm

图4 样品c在不同电解质溶液中的循环伏安图

Fig. 4 Cyclic voltammogram of sample c electrode in different electrolytic solutions at scan rate of 100 mV/s(1) 0.1 mol/L Na2SO4-NaHSO4, pH 2.2; (2) 0.1 mol/L Na2SO4, pH 7.0; (3) 0.1 mol/L Na2CO3-NaHCO3, pH 9.4

图5 硝基苯在NDD电极(样品c, d, e)上的阳极催化降解曲线

Fig. 5 Anodically catalyzed degradation curves of NB at NDD electrodes (sample c, d, e)(0.1 mol/L Na2SO4 solution. [NB]=0.5 mmol/L, E=2.8 V)

图6 样品c电解过程中溶液COD的变化曲线

Fig. 6 Anodically catalyzed degradation curve of COD at electrode of sample c

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掺氮金刚石电极性能及其氧化降解硝基苯研究

Nitrogen-doped Diamond Electrode Property and Anodic Catalytic Degradation of Nitrobenzene

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