邻苯二甲酸二甲酯在三维多孔钛基掺硼金刚石薄膜电极上的电催化氧化行为

doi:10.7503/cjcu20150069

高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (8): 1606.doi: 10.7503/cjcu20150069

邻苯二甲酸二甲酯在三维多孔钛基掺硼金刚石薄膜电极上的电催化氧化行为

梁龙琪, 黄卫民(), 林海波

吉林大学化学学院, 长春130012

收稿日期:2015-01-20 出版日期:2015-08-10 发布日期:2015-07-17
作者简介:联系人简介: 黄卫民, 男, 博士, 副教授, 主要从事电化学研究. E-mail:huangwm@jlu.edu.cn
基金资助:
国家自然科学基金(批准号: 21273097 )、吉林省重大科技攻关招标项目(批准号: 20130204003GX)和电分析化学国家重点实验室开放课题(2013)资助

Electrochemical Oxidation of Dimethyl Phthalate on Porous Titanium Based Boron-dopped Diamond Electrode^†

LIANG Longqi, HUANG Weimin^*(), LIN Haibo

College of Chemistry, Jilin University, Changchun 130012, China

Received:2015-01-20 Online:2015-08-10 Published:2015-07-17
Contact: HUANG Weimin E-mail:huangwm@jlu.edu.cn
Supported by:
† Supported by the National Natural Science Foundation of China(No.21273097), the Science Foundation of Jilin Province, China(No.20130204003GX) and the Open Fund of the State Key Laboratory of Electroanalytical Chemistry, China(2013)

摘要/Abstract

摘要：

以邻苯二甲酸二甲酯(DMP)作为模型污染物, 研究了不同结构的钛基体对掺硼金刚石薄膜(Ti/BDD)电极电催化性能的影响. 结果表明, 三维多孔电极为氧化还原反应提供了更多的反应活性位点, 表现出更快的电子传递速率. 通过循环伏安法和线性扫描法验证了DMP在BDD电极上的电催化氧化行为属于直接电氧化过程, 且在低浓度下近似为一级反应, DMP浓度较高时会在BDD电极表面发生成膜现象. 在不同浓度的DMP溶液中使用平板Ti/BDD电极及多孔Ti/BDD电极进行直接电催化氧化时, DMP的电催化氧化过程与理论推断一致; 多孔电极由于其电活性面积的优势在COD和DMP的去除方面均优于平板电极.

关键词: 三维多孔钛基体, 掺硼金刚石薄膜电极, 邻苯二甲酸二甲酯, 电催化氧化

Abstract:

The effect of structure of the titanium substrate on the electrocatalytic activity of boron-dopped diamond film(BDD) electrode was studied with dimethyl phthalate(DMP) as an organic pollutant mode. 3D porous Ti/BDD electrode can provide more reactive sites for the electrochemical reaction and has faster electron transfer rate compared with planar Ti/BDD electrode. The electrooxidation behavior of DMP on BDD electrodes is direct oxidation based on the results of cyclic voltammetry and liner sweep curves and presented pseudo first-order kinetic at low DMP concentration. Meanwhile, the formation of polymer film was observed at high DMP concentration. Due to the high active area, 3D porous Ti/BDD electrode revealed superior performance in the direct electrooxidation of DMP. In terms of chemical oxygen demand(COD) and removal rate when employing different concentrations of DMP, the experimental results on planar Ti/BDD and 3D-Ti/BDD electrodes coincided with the theory proposed.

Key words: Three-dimensional porous titanium substrate, Boron-doped diamond film electrode, Dimethyl phthalate, Electrochemical oxidation

中图分类号:

O646

TrendMD:

梁龙琪, 黄卫民, 林海波. 邻苯二甲酸二甲酯在三维多孔钛基掺硼金刚石薄膜电极上的电催化氧化行为. 高等学校化学学报, 2015, 36(8): 1606.

LIANG Longqi, HUANG Weimin, LIN Haibo. Electrochemical Oxidation of Dimethyl Phthalate on Porous Titanium Based Boron-dopped Diamond Electrode^†. Chem. J. Chinese Universities, 2015, 36(8): 1606.

图/表 6

Fig.1 Cyclic voltammograms of planar Ti/BPP electrode(A) and porous Ti/BDD electrode(B) in 1 mol/L KCl solution with different concentrations of [Fe(CN)6]3-/4-Concentration of [Fe(CN)6]3-/4-/(mol·L-1): a. 5; b. 10; c. 20; d. 30.

Fig.2 Cyclic voltammograms of planar Ti/BDD electrodes at scan rate of 100 mV/s in 0.5 mol/L H2SO4 containing 100 mg/L DMPa. The 1st cycle; b. the 5th cycle.

Fig.3 Linear sweep voltammograms of a planar Ti/BDD electrode in 0.5 mol/L H2SO4 solution containing 100 mg/L DMP at different scan rates(A) and the relationship between response current density and square root of scan rate(B)The scan rates are 20, 100, 200, 400, 600, 800 and 1000 mV/s with the direction of the arrow.

Fig.4 Linear sweep voltammograms of planar Ti/BDD electrode in 0.5 mol/L H2SO4 solution containing different concentrations of DMP(A) and relationship between response current density and DMP concentration(B)The concentration of DMP is 15, 20, 25, 30, 35 and 40 mmol/L with the direction of the arrow.

Fig.5 Change of COD value during the degradation of DMP at planar Ti/BDD(A) and porous Ti/BDD anodes(B)Concentration of DMP/(mg·L-1): a. 20; b. 40; c.60.

Fig.6 Change of concentration of DMP during degradation using planar Ti/BDD(A) and porous Ti/BDD anodes(B)Concentration of DMP/(mg·L-1): a. 20; b. 40; c.60.The insets show the relationship between value of ln(c0/ct) and time.

参考文献 25

[1]	Giam C. S., Chan H. S., Neff. G. S., Atlas E. L., Science, 1978, 199(4327), 419—421
[2]	Baikova S. V., Samsonova A. S., Aleshchenkova Z. M., Shcherbina A. N., Eurasian Soil Sci., 1999, 32, 701—704
[3]	Hou Y. N., Qu J. H., Zhan X., Liu H. J., J. Environ. Sci., 2009, 21, 1321—1328
[4]	Yin X. T., Xu Q., Wu S. Y., Wang M., Gu Z. Z., Chem. J. Chinese Universities, 2010, 31(4), 690—695
	(殷雪琰, 许茜, 吴淑燕, 王敏, 顾忠泽. 高等学校化学学报, 2010, 31(4), 690—695)
[5]	Wolf C., Lanbright C., Mann P., Price M., Cooper R. L., Ostby J., Gray L. E., Toxicol. Ind. Health, 1999, 15(1/2), 94—118
[6]	Zacharewski T. R., Meek M. D., Clemons J. H., Wu Z. F., Fielden M. R., Matthews J. B., Toxicolo. Sci., 1998, 46(2), 282—293
[7]	Jobling S., Reynolds T., White R., Parker M. G., Sumper J. P., Environ.Health Persp., 1995, 103(6), 582—587
[8]	Stales C. A., Peterson D. R., Parkerton T. F., Adams W. J., Chemosphere, 1997, 35(4), 667—749
[9]	Rodgers J. D., Jedral W., Bunce N. J., Enviro. Sci. Tech., 1999, 33(9), 1453—1457
[10]	Wu M. H., Liu N., Xu G., Ma J., Tang L., Wang L., Fu H. Y., Radiat. Phys. Chem., 2011, 80(3), 420—425
[11]	Torres R. A., Torres W., Periger P., Pulgarin C., Chemosphere, 2003, 50(1), 97—104
[12]	Brillas E., Boye B., Sires J., Garrido J. A., Rodriguez R. M., Arias C., Cabot P., Chemosphere, 2004, 49(25), 4487—4496
[13]	Chen X., Chen G., Gao F., Yue L. P., Environ. Sci. Technol., 2003, 37, 5021—5026
[14]	Iniesta J., Michaud P. A., Panizza M., Cerisola G., Aldaz A., Comninellis C., Electrochim. Acta, 2001, 46(23), 3573—3578
[15]	Rodrigo M. A., Michaud P. A., Duo I., Panizza M., Cerisola G., J. Electrochem. Soc., 2001, 148(5), D60—D64
[16]	Panizza M., Michaud P. A., Cerosola G., Comninellis C., J. Electroanal. Chem., 2001, 507(1/2), 206—214
[17]	Canizares P., Saez C., Lobato J., Rodrigo M. A., Ind. Eng. Chem. Res., 2004, 43(9), 1944—1951
[18]	Montilla F., Michaud P. A., Morallon E., Vazquez J. L., Comninellis C., Electrochim. Acta, 2002, 47(21), 3509—3513
[19]	Canizares P., Garcia-Gomez J., Lobato J., Rodrigo M. A., Ind. Eng. Chem. Res., 2003, 42(5), 956—962
[20]	Braga N. A., Baldan M. R., Ferreira N. G. J. Mater. Sci., 2012, 47, 23—40
[21]	Canizares P., Saez C., Lobato J., Paz R., Rodrigo M. A., J. Electroche. Soc., 2007, 154, E37—E44
[22]	Panizza M., Cerisola G., Electrochim. Acta, 2005, 51, 191—199
[23]	Li H., Zhu X., Jiang Y., Ni J., Chemosphere, 2010, 80, 845—851
[24]	Souzad F., Saez C., Canizares P., Motheo D. A., Rodrigo M., J. Chem. Tech. Biotech., 2014, 89, 282—289
[25]	Vazquez-Gomez L., Battisti D. A., Ferro S., Cerro M., Reyna S., Clean-Soil, Air Water, 2012, 40, 408—415

邻苯二甲酸二甲酯在三维多孔钛基掺硼金刚石薄膜电极上的电催化氧化行为

Electrochemical Oxidation of Dimethyl Phthalate on Porous Titanium Based Boron-dopped Diamond Electrode^†

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邻苯二甲酸二甲酯在三维多孔钛基掺硼金刚石薄膜电极上的电催化氧化行为

Electrochemical Oxidation of Dimethyl Phthalate on Porous Titanium Based Boron-dopped Diamond Electrode†

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Electrochemical Oxidation of Dimethyl Phthalate on Porous Titanium Based Boron-dopped Diamond Electrode^†