Citation: XU Xiangyu, LIAO Yanqing, SUN Jianchuan, WANG Xuhui, CHEN Shuaiqi, LV Zhi, SONG Jiaqing. Removal of Fluorides from Aqueous Solutions Using Fresh and Regenerated Activated Alumina[J]. Acta Physico-Chimica Sinica, ;2019, 35(3): 317-326. doi: 10.3866/PKU.WHXB201805021 shu

Removal of Fluorides from Aqueous Solutions Using Fresh and Regenerated Activated Alumina

State Key Laboratory of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China

Corresponding author: SONG Jiaqing, songjq@126.com
Received Date: 23 March 2018
Revised Date: 25 April 2018
Accepted Date: 25 April 2018
Available Online: 2 March 2018
Fund Project: The project was supported from Shanghai Key Laboratory of Green Chemistry and Chemical Processes, East China Normal University, China (H2016107)Shanghai Key Laboratory of Green Chemistry and Chemical Processes, East China Normal University, China H2016107

Fluoride contamination of water is a problem worldwide and has caused great concern. Our study focused on the removal of fluorides from aqueous solutions using newly prepared and regenerated activated alumina. To obtain a suitable adsorbent, industrial boehmite was calcined from 573 K to 1473 K and the sample was characterized. The X-ray diffraction patterns showed that the sample was transformed to γ-alumina (activated alumina) at temperatures from 773 K to 1173 K, and the BET dates showed that the specific surface area of the sample decreased gradually from the temperature of 773 K to 1173 K. In our study, the activated alumina calcined from 773 K to 973 K was selected as the defluoridation adsorbent, and dynamic adsorption was employed for the removal of fluorides from aqueous solutions. The breakthrough curves demonstrated that the adsorption capacity of the adsorbent decreased with increasing calcination temperature. To investigate the effect of initial fluoride concentration on the adsorption capacity, 15 mg·L^-1, 20 mg·L^-1, and 25 mg·L^-1 fluoride solutions were selected as the initial aqueous fluoride solution. As a result, the capacity of the adsorbent increased gradually with the increase in the initial fluoride concentration. In order to improve the capacity, we also studied the regeneration process in our experiment. When the activated alumina was saturated by the fluorides, it was regenerated with a NaOH solution (pH = 13.0, 13.3, 13.5) and activated with a HCl solution (0.1 mol·L^-1). By a comparison of the five desorption and Al³⁺ dissolution rates during the regeneration process, it was determined that the NaOH solution with pH 13.0 was the most suitable desorption agent. An analysis of the nitrogen adsorption-desorption isotherm showed that its sharpness was almost unchanged after regeneration, which indicated that the pore structure of the adsorbent was not destroyed during this process. The change in the specific surface area and isoelectric point for the five-times regenerated adsorbent were important impact factors for fluoride adsorption. The specific surface area of the regenerated adsorbent increased, and the study of the zeta potential demonstrated that the isoelectric point also increased after regeneration. To observe the adsorption effect of regenerated activated alumina, we performed an adsorption experiment after each regeneration. The breakthrough curves demonstrated that the regenerated activated alumina exhibited faster saturation and increased adsorption capacity compared to fresh activated alumina. To elucidate the adsorption mechanism, IR spectroscopy was employed to characterize the O―H band of the adsorbent. The change in the Al―O―H content of the activated alumina during regeneration was the main factor impacting the fluoride adsorption capacity of the activated alumina.
- Defluoridation,
- Regeneration,
- Activated alumina,
- Breakthrough curve,
- Zeta potential
1. [1]
  WHO. Guidelines for Drinking-Water Quality, 4th ed.; WHO Press: Geneva, Switzerland, 2011.
2. [2]
  Tor, A.; Danaoglu, N.; Arslan, G.; Cengeloglu, Y. J. Hazard. Mater. 2009, 164 (1), 271. doi: 10.1016/j.jhazmat.2008.08.011 doi: 10.1016/j.jhazmat.2008.08.011
3. [3]
  Samarghandi, M. R.; Khiadani, M.; Foroughi, M.; Nasab, H. Z. Environ. Sci. Pollut. Res. 2016, 23 (1), 887. doi: 10.1007/s11356-015-5293-x doi: 10.1007/s11356-015-5293-x
4. [4]
  Yi, Q.; Ge, L.; Cheng, Y.; Dong, H.; Liu, K.; Zhang, J.; Yue, C. J. Groundwater Sci. Eng. 2015, 3 (2), 176.
5. [5]
  Jagtap, S.; Yenkie, M. K.; Labhsetwar, N.; Rayalu, S. Chem. Rev. 2012, 112 (4), 2454. doi: 10.1021/cr2002855 doi: 10.1021/cr2002855
6. [6]
  Sivasankar, V. S. Surface Modified Carbons as Scavengers for Fluoride from Water; Springer: Switzerland; 2016.
7. [7]
  Chinnakoti, P.; Chunduri, A. L. A.; Vankayala, R. K.; Patnaik, S.; Kamisetti, V. Appl. Water Sci. 2017, 7 (5), 2413. doi: 10.1007/s13201-016-0437-9 doi: 10.1007/s13201-016-0437-9
8. [8]
  Duan, Y.; Wang, C.; Li, X.; Xu, W. J. Water Health. 2014, 12 (4), 715. doi: 10.2166/wh.2014.016 doi: 10.2166/wh.2014.016
9. [9]
  Zhu, B.; Jia, Y.; Jin, Z.; Sun, B.; Luo, T.; Kong, L.; Liu, J. RSC Adv. 2015, 5 (103), 84389. doi: 10.1039/C5RA15619J doi: 10.1039/C5RA15619J
10. [10]
  Arora, M.; Maheshwari, R. C.; Jain, S. K.; Gupta, A. Desalination 2004, 170 (2), 105. doi: 10.1016/j.desal.2004.02.096 doi: 10.1016/j.desal.2004.02.096
11. [11]
  Amor, Z.; Bariou, B.; Mameri, N.; Taky, M.; Nicolas, S.; Elmidaoui, A. Desalination 2001, 133 (3), 215. doi: 10.1016/S0011-9164(01)00102-3 doi: 10.1016/S0011-9164(01)00102-3
12. [12]
  Hichour, M.; Persin, F. O.; Sandeaux, J.; Gavach, C. Sep. Purif. Technol. 1999, 18 (1), 1. doi: 10.1016/S1383-5866(99)00042-8 doi: 10.1016/S1383-5866(99)00042-8
13. [13]
  Nasr, A. B.; Charcosset, C.; Amar, R. B.; Walha, K. J. Fluorine Chem. 2013, 150, 92. doi: 10.1016/j.jfluchem.2013.01.021 doi: 10.1016/j.jfluchem.2013.01.021
14. [14]
  Ghosh, D.; Medhi, C. R.; Purkait, M. K. Chemosphere 2008, 73 (9), 1393. doi: 10.1016/j.chemosphere.2008.08.041 doi: 10.1016/j.chemosphere.2008.08.041
15. [15]
  Meenakshi, S.; Viswanathan, N. J. Colloid Interface Sci. 2007, 308 (2), 438. doi: 10.1016/j.jcis.2006.12.032 doi: 10.1016/j.jcis.2006.12.032
16. [16]
  Loganathan, P.; Vigneswaran, S.; Kandasamy, J.; Naidu, R. J. Hazard. Mater. 2013, 248-249, 1. doi: 10.1016/j.jhazmat.2012.12.043 doi: 10.1016/j.jhazmat.2012.12.043
17. [17]
  Habuda-Stanić, M.; Ravančić, M.; Flanagan, A. Materials 2014, 7 (9), 6317. doi: 10.3390/ma7096317 doi: 10.3390/ma7096317
18. [18]
  Maliyekkal, S. M.; Sharma, A. K.; Philip, L. Water Res. 2006, 40 (19), 3497. doi: 10.1016/j.watres.2006.08.007 doi: 10.1016/j.watres.2006.08.007
19. [19]
  Mondal, P.; George, S. Rev. Environ. Sci. Bio/Technol. 2015, 14 (2), 195. doi: 10.1007/s11157-014-9356-0 doi: 10.1007/s11157-014-9356-0
20. [20]
  Fawell, J.; Bailey, K.; Chilton, J.; Dahi, E.; Fewtrell, L.; Magara, Y. Fluoride in Drinking-Water; WHO Press: Geneva, Switzerland, 2006.
21. [21]
  Wang, S.; Ma, Y.; Shi, Y.; Gong, W. J. Chem. Technol. Biotechnol. 2009, 84 (7), 1043. doi: 10.1002/jctb.2131 doi: 10.1002/jctb.2131
22. [22]
  Dash, K.; Hareesh, U. S.; Johnson, R.; Arunachalam, J. Water Pract. Technol. 2010, 5 (3), 1. doi: 10.2166/WPT.2010.061 doi: 10.2166/WPT.2010.061
23. [23]
  Gong, W.; Qu, J.; Liu, R.; Lan, H. Chem. Eng. J. 2012, 189-190, 126. doi: 10.1016/j.cej.2012.02.041 doi: 10.1016/j.cej.2012.02.041
24. [24]
  Deng, S. B.; Yu, G. Environmental Adsorption Material and Its Application Principle; Science Press: Beijing, 2012.
25. [25]
  Prabhu, S. M.; Subaramanian, M.; Meenakshi, S. Chem. Eng. J. 2016, 283, 1081. doi: 10.1016/j.cej.2015.08.005 doi: 10.1016/j.cej.2015.08.005
26. [26]
  Liu, R.; Gong, W.; Lan, H.; Gao, Y.; Liu, H.; Qu, J. Chem. Eng. J. 2011, 175, 144. doi: 10.1016/j.cej.2011.09.083 doi: 10.1016/j.cej.2011.09.083
27. [27]
  Gai, W.; Deng, Z.; Shi, Y. RSC Adv. 2015, 5 (102), 84223. doi: 10.1039/C5RA14706A doi: 10.1039/C5RA14706A
28. [28]
  Jia, Y.; Zhu, B.; Jin, Z.; Sun, B.; Luo, T.; Yu, X.; Kong, L.; Liu, J. J. Colloid Interface Sci. 2015, 440, 60. doi: 10.1016/j.jcis.2014.10.069 doi: 10.1016/j.jcis.2014.10.069
29. [29]
  Nur, T.; Loganathan, P.; Nguyen, T. C.; Vigneswaran, S.; Singh, G.; Kandasamy, J. Chem. Eng. J. 2014, 247, 93. doi: 10.1016/j.cej.2014.03.009 doi: 10.1016/j.cej.2014.03.009
30. [30]
  Niu, B. J.; Ding, W. M.; Dang, D. Appl. Mech. Mater. Trans Technol. Pub. 2013, 316, 653. doi: 10.1109/ICETCE.2012.508 doi: 10.1109/ICETCE.2012.508
31. [31]
  Ghorai, S.; Pant, K. K. Sep. Purif. Technol. 2005, 42 (3), 265. doi: 10.1016/j.seppur.2004.09.001 doi: 10.1016/j.seppur.2004.09.001
32. [32]
  Ghorai, S.; Pant, K. K. Chem. Eng. J. 2004, 98 (1-2), 165. doi: 10.1016/j.cej.2003.07.003 doi: 10.1016/j.cej.2003.07.003
33. [33]
  Kumar, E.; Bhatnagar, A.; Kumar, U.; Sillanpää, M. J. Hazard. Mater. 2011, 186 (2-3), 1042. doi: 10.1016/j.jhazmat.2010.11.102 doi: 10.1016/j.jhazmat.2010.11.102
34. [34]
  Mohan, S.; Singh, D. K.; Kumar, V.; Hasan, S. H. J. Fluor. Chem. 2017, 194, 40. doi: 10.1016/j.jfluchem.2016.12.014 doi: 10.1016/j.jfluchem.2016.12.014
35. [35]
  Sing, K. Pure Appl. Chem. 1984, 57 (4), 603. doi: 10.1351/pac198557040603 doi: 10.1351/pac198557040603
36. [36]
  Jin, Z.; Jia, Y.; Luo, T.; Kong, L.; Sun, B.; Shen, W.; Meng, F.; Liu, J. Appl. Surf. Sci. 2015, 357, 1080. doi: 10.1016/j.apsusc.2015.09.127 doi: 10.1016/j.apsusc.2015.09.127
37. [37]
  Tangsir, S.; Hafshejani, L. D.; Lähde, A.; Maljanen, M.; Hooshmand, A.; Naseri, A. A.; Moazed, H.; Jokiniemi, J.; Bhatnagar, A. Chem. Eng. J. 2016, 288, 198. doi: 10.1016/j.cej.2015.11.097 doi: 10.1016/j.cej.2015.11.097
38. [38]
  Jia, Y.; Zhu, B.; Zhang, K.; Jin, Z.; Sun, B.; Luo, T.; Yu, X.; Kong, L.; Liu, J. Chem. Eng. J. 2015, 268, 325. doi: 10.1016/j.cej.2015.01.080 doi: 10.1016/j.cej.2015.01.080
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