Abstract
La–Ce–MCM-41 was directly synthesized by a hydrothermal method and applied as heterogeneous catalyst for the ozonation process of para chlorobenzoic-acid (pCBA). La3+ and Ce3+ were successfully incorporated into the framework of MCM-41 and the formation of degradation products (p-chlorophenol, p-dihydroxybenzene, maleic acid and oxalic acid) were monitored qualitatively using gas chromatography–mass spectrometer and high performance liquid chromatography. Due to the synergy of bimetal and the fast degradation of accumulated intermediates, total organic carbon (TOC) removal efficiency was significantly improved (92 %) in La–Ce–MCM-41/O3 process compared with ozonation (40 %) at identical reaction condition. The presence of tert-butanol (TBA) in La–Ce–MCM-41/O3 process indicated that the oxidation of pCBA was mainly due to the function of hydroxyl radicals in the liquid bulk, and a plausible degradation pathway was proposed. TOC removal slightly decreased from 90 to 86 % after La–Ce–MCM-41 being re-utilized three times, which illustrated that La–Ce–MCM-41 was an efficient of promising catalyst for ozonation of pCBA.
Similar content being viewed by others
References
B. Langlais, D.A. Reckhow, D.R. Brink, Ozone in water treatment: application and engineering (Lewis Publisher, Chelsea, 1991)
M. Ernst, F. Lurot, J.C. Schrotter, Appl. Catal. B: Environ. 47, 15–25 (2004)
B. Legube, N.K.V. Leitner, Catal. Today 53, 61–72 (1999)
B. Kasprzyk-Horderna, M. Ziółekb, J. Nawrockia, Appl. Catal. B: Environ. 46, 639–669 (2003)
Y. Huang, C. Cui, D. Zhang, L. Li, D. Pan, Chemosphere 119, 295–301 (2015)
J. Nawrocki, B. Kasprzyk-Hordern, Appl. Catal. B: Environ. 99, 27–42 (2010)
S.S. Lin, M.D. Gurol, Water Sci. Technol. 34, 57–64 (1996)
R. Huang, H. Yan, L. Li, D. Deng, Y. Shu, Q. Zhang, Appl. Catal. B: Environ. 106, 264–271 (2011)
J. Bing, L. Li, B. Lan, G. Liao, J. Zeng, Q. Zhang, X. Li, Appl. Catal. B: Environ. 115–116, 16–24 (2012)
R. Andreozzi, A. Insola, V. Caprio, R. Marotta, V. Tufano, Appl. Catal. A: Gen. 138, 75–81 (1996)
C. Cooper, R. Burch, Water Res. 33, 3695–3700 (1999)
F.P. Logemann, J.H.J. Annee, Water Sci. Technol. 35, 353–360 (1997)
R. Gracia, S. Cortés, J. Sarasa, P. Ormad, J.L. Ovelleiro, Ozone Sci. Eng. 22, 461–471 (2000)
Z. Pan, J. Zeng, B. Lan, L. Li, J. Adv. Oxid. Technol. 18, 139–146 (2015)
S. Imamura, A. Doi, S. Ishida, Ind. Eng. Chem. Prod. Res. Dev. 24, 75–80 (1985)
S. Imamura, M. Nakamura, N. Kawabata, J. Yoshida, S. Ishida, Ind. Eng. Chem. Prod. Res. Dev. 25, 34–37 (1986)
C.T. Kresge, M.E. Leonowicz, W.J. Roth, J.C. Vartuli, J.S. Beck, Nature 359, 710–712 (1992)
J.S. Beck, J.C. Vartuli, W.J. Roth, M.E. Leonowicz, C.T. Kresge, K.D. Schmitt, C.T.W. Chu, D.H. Olson, E.W. Sheppard, J. Am. Chem. Soc. 114, 10834–10843 (1992)
W. Huang, J.N. Kuhn, C.K. Tsung, Y. Zhang, S.E. Habas, P. Yang, G.A. Somorjai, Nano Lett. 8, 2027–2034 (2008)
D. Zhao, J. Sun, Q. Li, G.D. Stucky, Chem. Mater. 12, 275–279 (2000)
X. Chen, S. Wang, J. Zhuang, M. Qiao, K. Fan, H. He, J. Catal. 227, 419–427 (2004)
G. Liu, M. Hou, T. Wu, T. Jiang, H. Fan, G. Yang, B. Han, Phys. Chem. Chem. Phys. 13, 2062–2068 (2011)
Z. Ma, S. Dai, Nano. Res. 4, 3–32 (2011)
X. Yang, D. Chen, S. Liao, H. Song, Y. Li, Z. Fu, Y. Su, J. Catal. 291, 36–43 (2012)
R. Huang, J. Liu, L. Li, Q. Zhang, L. Zeng, P. Lu, Chin. Chem. Lett. 22, 683–686 (2011)
H. Yan, P. Lu, Z. Pan, X. Wang, Q. Zhang, L. Li, J. Mol. Catal. A: Chem. 377, 57–64 (2013)
J. Bing, X. Wang, B. Lan, G. Liao, Q. Zhang, L. Li, Sep. Purif. Technol. 118, 479–486 (2013)
B. Lan, R. Huang, L. Li, H. Yan, G. Liao, X. Wang, Q. Zhang, Chem. Eng. J. 219, 346–354 (2013)
Y. He, F. Grieser, M. Ashokkumar, J. Phys. Chem. A 115, 6582–6588 (2011)
P.C.C. Faria, D.C.M. Monteiro, J.J.M. Órfão, M.F.R. Pereira, Chemosphere 74, 818–824 (2009)
R. Huang, B. Lan, Z. Chen, H. Yan, Q. Zhang, J. Bing, L. Li, Chem. Eng. J. 180, 19–24 (2012)
R.C. Martins, R.M. Quinta-Ferreira, Appl. Catal. B: Environ. 90, 268–277 (2009)
M. Kuosa, J. Kallas, Chem. Eng. Process. 48, 1212–1221 (2009)
M. Pera-Titus, V. García-Molin, M.A. Baños, J. Giménez, S. Esplugas, Appl. Catal. B: Environ. 47, 219–256 (2004)
J. Ma, M. Sui, T. Zhang, C. Guan, Water Res. 39, 779–786 (2005)
Q. Sun, L. Li, H. Yan, X. Hong, K.S. Hui, Z. Pan, Chem. Eng. J. 242, 348–356 (2014)
C.P. Huang, C. Dong, Z. Tang, Waste Manag. 13, 361–377 (1993)
R. Andreozzi, V. Caprioa, A. Insola, R. Marotta, Catal. Today 53, 51–59 (1999)
J. Ma, N.J.D. Graham, Water Res. 34, 3822–3828 (2000)
S. Tong, W. Liu, W. Leng, Q. Zhang, Chemosphere 50, 1359–1364 (2003)
M. Sánchez-Polo, J. Rivera-Utrilla, U.V. Gunten, Water Res. 40, 3375–3384 (2006)
G. Praline, B.E. Koel, R.L. Hance, H.I. Lee, J.M. White, J. Electron. Spectrosc. 21, 17–30 (1980)
Q. Zhao, Y. Xu, Y. Li, T. Jiang, C. Li, H. Yin, Appl. Surf. Sci. 255, 9425–9429 (2009)
M. Boutros, F. Launay, A. Nowicki, T. Onfroy, V. Herledan-Semmer, A. Roucoux, A. Gédéon, J. Mol. Catal. A: Chem. 259, 91–98 (2006)
W. Zhan, G. Lu, Y. Guo, Y. Guo, Y. Wang, J. Rare Earth 26, 59–65 (2008)
F. Delanoë, B. Acedo, N.K.V. Leitner, B. Legube, Appl. Catal. B: Environ. 29, 315–325 (2007)
Acknowledgments
The authors are grateful for the financial support from the National Natural Science Foundation of China (Contract No. 20977036), the Science and Technology Office of Guangdong Province (Contract No. 2010B030900006) and the National High-Tech Research and Development Program (Contract No. 2013AA06A305), the South China Normal University graduate student innovation fund in 2014 (Contract No. 2014bsxm11).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Pan, Z., Zeng, J. & Li, L. Efficient degradation of para-chlorobenzoic acid in water by catalytic ozonation with La–Ce–MCM-41. J Porous Mater 23, 619–628 (2016). https://doi.org/10.1007/s10934-015-0116-5
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10934-015-0116-5