| 引用本文: | 张云澍,丁晶,高庆伟,王琨,赵庆良.Ti4O7多孔膜电极降解橙黄Ⅱ的效果与催化机制[J].哈尔滨工业大学学报,2022,54(2):31.DOI:10.11918/202103056 |
| ZHANG Yunshu,DING Jing,GAO Qingwei,WANG Kun,ZHAO Qingliang.Effect and mechanism of Ti4O7 porous membrane electrode for orange Ⅱ degradation[J].Journal of Harbin Institute of Technology,2022,54(2):31.DOI:10.11918/202103056 |
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| 摘要: |
| 为开发高效、低成本的电催化氧化系统,在制备Ti4O7多孔膜电极的基础上构建穿流-电催化氧化系统,采用X-射线衍射、压汞法、电子顺磁共振波谱等对Ti4O7多孔膜电极进行表征,分析穿流和非穿流模式下橙黄Ⅱ的电催化降解动力学,探究穿流模式下管道压力、电流密度、初始污染物浓度和溶液pH对橙黄Ⅱ电催化降解的影响,验证Ti4O7多孔膜电极的循环稳定性和电催化机制。结果表明:Ti4O7多孔膜电极具有晶体纯度高、比表面积高(10.18 m2/g)、孔径分布集中(0.1~1.0 μm)、析氧电位高(2.2 V vs. SHE)等特点;穿流模式可以增强污染物向电极表面的液相传质,进而加速污染物的电催化降解,穿流模式下橙黄Ⅱ的降解率可达91.03%,电流效率为88.77%;穿流模式下,管道压力、电流密度与橙黄Ⅱ的电催化降解速率呈正相关,不同初始质量浓度的橙黄Ⅱ(10~50 mg/L)在穿流模式下均可以被有效降解,最适pH为3~7;Ti4O7多孔膜电极具有良好的循环稳定性,·OH和SO-4·是Ti4O7多孔膜电极电催化过程中最重要的氧化剂。 |
| 关键词: 电化学高级氧化 Ti4O7多孔膜电极 液相传质 橙黄Ⅱ 动力学 |
| DOI：10.11918/202103056 |
| 分类号:X703.1 |
| 文献标识码:A |
| 基金项目:国家自然科学基金(6,4)； 中国博士后科学基金(2018M643198) |
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| Effect and mechanism of Ti4O7 porous membrane electrode for orange Ⅱ degradation |
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ZHANG Yunshu1,DING Jing2,GAO Qingwei2,WANG Kun2,ZHAO Qingliang2
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（1.School of Environment and Architecture, University of Shanghai for Science and Technology, Shanghai 200093, China; 2.School of Environment, Harbin Institute of Technology, Harbin 150090, China）
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| Abstract: |
| To develop an efficient and low-cost electrochemical oxidation system, a flow-through electrochemical oxidation process was designed based on a Ti4O7 porous membrane electrode. The material properties of the Ti4O7 porous membrane electrode were analyzed by X-ray diffraction, mercury intrusion, and electron paramagnetic resonance spectroscopy. The degradation kinetics of orange II in flow-through and non-flow-through electrochemical oxidation modes were analyzed. The effects of pipeline pressure, current density, initial pollutant concentration, and solution pH on the electrochemical oxidation of orange II in the flow-through mode were investigated. The cycling stability of the Ti4O7 porous membrane electrode was tested, and the catalytic mechanism of the Ti4O7 porous membrane electrode was revealed. Results showed that the Ti4O7 porous membrane electrode had high crystal purity, high specific surface area (10.18 m2/g), concentrated pore size distribution (0.1-1.0 μm), and high oxygen evolution potential (2.2 V vs. SHE). The flow-through electrochemical oxidation mode could enhance the liquid-phase mass transfer of pollutants to the electrode surface, accelerating the electrooxidation of pollutants. The degradation rate of orange Ⅱ in flow-through electrochemical oxidation mode was 91.03% and the current efficiency was 88.77%. In the flow-through mode, the pipeline pressure and current density had positive correlation with the degradation rate of orange Ⅱ. Orange Ⅱ with different initial concentrations (10-50 mg/L) could all be effectively degraded in the flow-through electrochemical oxidation mode, with the optimum pH ranging between 3 and 7. The cycling stability of the Ti4O7 porous membrane electrode was high. ·OH and SO-4· were the main oxidants in the electrochemical oxidation process of Ti4O7 porous membrane electrode. |
| Key words: electrochemical advanced oxidation process Ti4O7 porous membrane electrode liquid-phase mass transfer orange Ⅱ kinetics |
