Activation of Hydrogen Peroxide by Activated Carbon Fibers Coupled with Fe(Ⅲ)-Citrate for Degradation of Dyes at Neutral pH
Received date: 2013-08-07
Online published: 2013-10-14
Supported by
Project supported by the State Key Program of National Natural Science of China (No. 51133006), the National Natural Science Foundation of China (Nos. 51003096, 51103133), Science Foundation of Zhejiang Sci-Tech University (No. 1001803-Y) and Textile Vision Science & Education Fund.
The development of a pH-tolerant Fenton-like catalyst is a active and challenging project in the field of environmental catalysis. In this work, an efficient Fenton-like catalytic fibers (Cit-Fe@ACFs) with pH-tolerance has been prepared by an extremely simple impregnation method. First, activated carbon fibers (ACFs) were impregnated into a nitric acid solution at 25 ℃ for 24 h to obtain acidified ACFs, and then immersed in a sodium citrate solution at 25 ℃ for 2 h, which was taken out to put into ferric chloride solution at 25 ℃ for 2 h. The treated ACFs were rinsed with distilled water and dried at room temperature to obtain the Cit-Fe@ACFs. Cit-Fe@ACFs exhibited efficient catalytic activity for the activation of hydrogen peroxide at neutral pH to degrade dyes, including reactive, acid, and basic dyes, etc. The UV-vis spectroscopy showed that reactive brilliant red M-3BE (RR M-3BE) was eliminated completely in 15 min (Cit-Fe@ACFs: 12 g/L; H2O2: 60 mmol/L; RR M-3BE: 5×10-5 mol/L; pH 7; T=50 ℃). Moreover, the catalyst presented excellent regeneration capability and sustained catalytic ability in these experiments. Importantly, the Cit-Fe@ACFs/H2O2 catalytic system exhibited remarkable catalytic activity across a wider pH range (2～10) and the values of apparent rate constant (kapp) were greater than 0.320 min-1, which was efficient to expand the pH range for the traditional Fenton reaction. Various scavengers and probe compounds (n-butanol, benzoquinone) combined with electron paramagnetic resonance (EPR) spectroscopy were used to identify the active species involved in the catalytic system. The results revealed that the hydroxyl radicals (·OH) and superoxide radical (HO2·) may be responsible for the degradation of dyes. This paper discusses a possible catalytic oxidation mechanism in the Cit-Fe@ACFs/H2O2 system, which may be a feasible approach for the elimination of widely existing pollutants.
Key words： activated carbon fibers; ferric citrate; Fenton-like; catalytic fibers; dyes
Wang Lie, Yao Yuyuan, Sun Lijie, Lü Wangyang, Chen Wenxing . Activation of Hydrogen Peroxide by Activated Carbon Fibers Coupled with Fe(Ⅲ)-Citrate for Degradation of Dyes at Neutral pH[J]. Acta Chimica Sinica, 2013 , 71(12) : 1633 -1638 . DOI: 10.6023/A13080832
[1] Zhou, X.; Lan, J.; Liu, G.; Deng, K.; Yang, Y.; Nie, G.; Yu, J.; Zhi, L. Angew. Chem., Int. Ed. 2012, 51, 178.
[2] Ayoub, K.; van Hullebusch, E. D.; Cassir, M.; Bermond, A. J. Hazard. Mater. 2010, 178, 10.
[3] Jiang, H.; Wang, Q.; Li, J.; Wang, Q.; Li, Z. Acta Chim. Sinica 2012, 70, 2173. (姜洪泉, 王巧凤, 李井申, 王庆元, 李振宇, 化学学报, 2012, 70, 2173).
[4] Ma, J.; Song, W.; Chen, C.; Ma, W.; Zhao, J.; Tang, Y. Environ. Sci. Technol. 2005, 39, 5810.
[5] Nam, S.; Renganathan, V.; Tratnyek, P. Chemosphere 2001, 45, 59.
[6] Joonseon, J.; Jeyong, Y. Water Res. 2005, 39, 2893.
[7] Huang, W.; Brigante, M.; Wu, F.; Mousty, C.; Hanna, K.; Mailhot, G. Environ. Sci. Technol. 2013, 47, 1952.
[8] Silva, M R. A.; Trovo, A. G.; Nogueira, R. F. P. J. Photochem. Photobiol. A 2007, 191, 187.
[9] Schmidt, C.; Fleig, M.; Sacher, F.; Brauch, H. Environ. Pollut. 2004, 131, 107.
[10] Dean, J. A. Lange's Chemistry Handbook, 13th ed., Science Press, Beijing, 1991, Chapter 5.5. (Dean, J. A. 兰氏化学手册, 第十三版, 科学出版社, 北京, 1991, Chapter 5.5.).
[11] Feng, X.; Wang, Z.; Chen, Y.; Tao, T.; Wu, F.; Zuo, Y. Ind. Eng. Chem. Res. 2012, 51, 7007.
[12] Guo, J.; Du, Y.; Lan, Y.; Mao, J. J. Hazard. Mater. 2011, 186, 2083.
[13] Chen, M.; Ma, W.; Li, J.; Huang, Y.; Zhao, J. Environ. Sci. Technol. 2004, 38, 1569.
[14] Gonzalez-Olmos, R.; Holzer, F.; Kopinke, F.; Georgi, A. Appl. Catal. A: General 2011, 398, 44.
[15] Martínez, F.; Pariente, M.; ángel, J.; Melero, J.; Rubalcaba, A. J. Chem. Technol. Biotechnol. 2012, 87, 880.
[16] Ramirez, J.; Vicente, M.; Madeira, L. Appl. Catal. B: Environ. 2010, 98, 10.
[17] Filipa, D.; Francisco, J. M.; Luis, M. M. Appl. Catal. B: Environ. 2013, 129, 264.
[18] Gergo, M.; Frank, P. Z.; Josep, F.; Agustí, F.; Azael, F. J. Environ. Manage. 2012, 102, 148.
[19] Lu, W.; Chen, W.; Li, N.; Xu, M.; Yao, Y. Appl. Catal. B: Environ. 2009, 87, 146.
[20] Yao, Y.; Wang, L.; Sun, L.; Zhu, S.; Huang, Z.; Mao, Y.; Lu, W.; Chen, W. Chem. Eng. Sci. 2013, 101, 424.
[21] Chen, J.; Zhu, L. Catal. Today 2007, 126, 463.
[22] Rodríguez, A.; Ovejero, G.; Sotelo, J.; Mestanza, M.; García, J. Ind. Eng. Chem. Res. 2010, 49, 498.
[23] Xu, L.; Wang, J. Environ. Sci. Technol. 2012, 46, 10145.
[24] Zhou, L.; Song, W.; Chen, Z.; Yin, G. Environ. Sci. Technol. 2013, 47, 3833.
/
| 〈 |
|
〉 |
