Please wait a minute...
Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2014, Vol. 8 Issue (2) : 169-179    https://doi.org/10.1007/s11783-013-0533-0
RESEARCH ARTICLE
Simultaneous removal of arsenate and fluoride from water by Al-Fe (hydr)oxides
Junlian QIAO1, Zimin CUI2, Yuankui SUN1, Qinghai HU1, Xiaohong GUAN1()
1. State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
2. State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China
 Download: PDF(391 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

Al-Fe (hydr)oxides with different Al/Fe molar ratios (4∶1, 1∶1, 1∶4, 0∶1) were prepared using a co-precipitation method and were then employed for simultaneous removal of arsenate and fluoride. The 4Al:Fe was superior to other adsorbents for removal of arsenate and fluoride in the pH range of 5.0–9.0. The adsorption capacity of the Al-Fe (hydr)oxides for arsenate and fluoride at pH 6.5±0.3 increased with increasing Al content in the adsorbents. The linear relationship between the amount of OH released from the adsorbent and the amount of arsenate or fluoride adsorbent by 4Al:Fe indicated that the adsorption of arsenate and fluoride by Al-Fe (hydr)oxides was realized primarily through quantitative ligand exchange. Moreover, there was a very good correlation between the surface hydroxyl group densities of Al-Fe (hydr)oxides and their adsorption capacities for arsenate or fluoride. The highest adsorption capacity for arsenate and fluoride by 4Al:Fe is mainly ascribed to its highest surface hydroxyl group density besides its largest pHpzc. The dosage of adsorbent necessary to remove arsenate and fluoride to meet the drinking water standard was mainly determined by the presence of fluoride since fluoride was generally present in groundwater at much higher concentration than arsenate.

Keywords Al-Fe (hydr)oxides      groundwater      adsorption      hydroxyl group      ligand exchange     
Corresponding Author(s): Xiaohong GUAN   
Issue Date: 01 April 2014
 Cite this article:   
Junlian QIAO,Zimin CUI,Yuankui SUN, et al. Simultaneous removal of arsenate and fluoride from water by Al-Fe (hydr)oxides[J]. Front. Environ. Sci. Eng., 2014, 8(2): 169-179.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-013-0533-0
https://academic.hep.com.cn/fese/EN/Y2014/V8/I2/169
Fig.1  XRD patterns of the Al-Fe binary (hydr)oxides and pure Fe (hydr)oxides (a) 4Al:Fe; (b) Al:Fe; (c) Al:4Fe; (d) Fe
Fig.2  SEM-EDAX analysis of the Al-Fe binary (hydr)oxides and pure Fe (hydr)oxides: (a) 4Al:Fe; (b) Al:Fe; (c) Al:4Fe; (d) Fe
Fig.3  Influence of pH on arsenate adsorption by the Al-Fe binary (hydr)oxides and pure Fe (hydr)oxides without (a) or with (b) the presence of fluoride (initial As(V) = 5?mg·L−1, initial F = 20?mg·L−1, adsorbent dose= 0.2?g·L−1)
Fig.4  Influence of pH on fluoride adsorption by the Al-Fe binary (hydr)oxides and pure Fe (hydr)oxides without (a) or with (b) the presence of arsenate (Initial F = 20?mg·L−1, initial As(V) = 5?mg·L−1, adsorbent dose= 0.5?g·L−1)
Fig.5  Influence of 4Al:Fe adsorbent dosage on simultaneous removal of arsenate and fluoride as a function of pH (a) Removal efficiency of As(V); (b) Removal efficiency of F (initial As(V) = 5?mg·L−1, initial F = 20?mg·L−1, adsorbent dose= 0.2 or 0.5?g·L−1, ionic strength= 0.01?mol·L−1)
concentration of F/(mg·L−1) adsorbent Langmuir isotherm Freundlich isotherm
Qmax /(mg·g−1) k /(L·mg−1) R2 KF n R2
0?mg·L−1 4Al:Fe 71.43 9.33 0.9865 93.88 1.83 0.6334
Al:Fe 52.08 4.26 0.9809 33.70 2.91 0.5211
Al:4Fe 43.48 12.10 0.9976 32.03 3.46 0.7725
Fe 27.32 6.39 0.9979 19.68 4.54 0.7733
20?mg·L−1 4Al:Fe 42.92 1.87 0.9759 21.29 2.27 0.8677
Al:Fe 32.26 2.12 0.9907 16.13 2.81 0.8891
Al:4Fe 30.49 8.41 0.9953 19.24 3.45 0.8387
Fe 28.65 4.65 0.9897 18.36 4.23 0.8730
Tab.1  Model isotherm constant of arsenate adsorption by Al-Fe binary (hydr)oxides
Fig.6  Adsorption isotherm of arsenate on Al-Fe binary (hydr)oxides or Fe (hydr)oxides (a) in the absence or (b) in the presence of fluoride. The dots are experimental data. The solid lines and the dotted lines are the results fitted by Langmuir isotherm and Freundlich isotherm, respectively. (initial As(V) = 0−15?mg·L−1, initial F = 0 or 20?mg·L−1, adsorbent dose= 0.2?g·L−1, initial pH= 6.0, final pH= 6.5±0.3)
Fig.7  Adsorption isotherm of fluoride on Al-Fe binary (hydr)oxides or Fe (hydr)oxides (a) in the absence and (b) in the presence of arsenate. The dots are experimental data. The solid lines and the dotted lines are the results fitted by Langmuir isotherm and Freundlich isotherm, respectively. (initial F = 0−50?mg·L−1, initial As(V) = 0 or 5?mg·L−1, adsorbent dose= 0.5?g·L−1, initial pH= 6.0, final pH= 6.5±0.3)
concentration of As(V)/( mg·L−1) adsorbent Langmuir isotherm Freundlich isotherm
Qmax /(mg·g−1) k /(L·mg−1) R2 KF n R2
0?mg·L−1 4Al:Fe 45.87 0.28 0.9936 15.02 3.14 0.9705
Al:Fe 35.09 0.37 0.9927 16.11 4.67 0.9648
Al:4Fe 16.42 0.73 0.9940 7.98 4.42 0.8179
Fe 4.96 0.06 0.9275 0.63 2.09 0.8423
5?mg·L−1 4Al:Fe 47.62 0.20 0.9729 13.30 2.94 0.9948
Al:Fe 26.11 0.35 0.9935 12.25 5.08 0.9629
Al:4Fe 16.47 0.19 0.9553 5.30 3.52 0.9119
Fe 2.67 0.02 0.3169 0.06 1.04 0.3787
Tab.2  Model isotherm constant of fluoride adsorption by Al-Fe binary (hydr)oxides
Fig.8  (a) Correlation between the amount of surface hydroxyl groups released from 4Al:Fe and the amount of fluoride or arsenate removed by 4Al:Fe at pH 7.0; (b) correlation between the adsorption capacity of various Al-Fe binary (hydr)oxides and pure Fe (hydr)oxides for arsenate or fluoride with their surface hydroxyl group densities
1 S Chouhan, S J S Flora. Arsenic and fluoride: two major ground water pollutants. Indian Journal of Experimental Biology, 2010, 48(7): 666–678
pmid: 20929051
2 C X Wu, X L Gu, Y M Ge, J H Zhang, J D Wang. Effects of high fluoride and arsenic on brain biochemical indexes and learning-memory in rats. Fluoride, 2006, 39(4): 274–279
3 M Amini, K C Abbaspour, M Berg, L Winkel, S J Hug, E Hoehn, H Yang, C A Johnson. Statistical modeling of global geogenic arsenic contamination in groundwater. Environmental Science & Technology, 2008, 42(10): 3669–3675
https://doi.org/10.1021/es702859e pmid: 18546706
4 M Amini, K Mueller, K C Abbaspour, T Rosenberg, M Afyuni, K N Møller, M Sarr, C A Johnson. Statistical modeling of global geogenic fluoride contamination in groundwaters. Environmental Science & Technology, 2008, 42(10): 3662–3668
https://doi.org/10.1021/es071958y pmid: 18546705
5 M A Armienta, N Segovia. Arsenic and fluoride in the groundwater of Mexico. Environmental Geochemistry and Health, 2008, 30(4): 345–353
https://doi.org/10.1007/s10653-008-9167-8 pmid: 18335171
6 Y L Tang, X H Guan, T Z Su, N Y Gao, J M Wang. Fluoride adsorption onto activated alumina: modeling the effects of pH and some competing ions. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2009, 337(1–3): 33–38
https://doi.org/10.1016/j.colsurfa.2008.11.027
7 C Warren, W G Burgess, M G Garcia. Hydrochemical associations and depth profiles of arsenic and fluoride in Quaternary loess aquifers of northern Argentina. Mineralogical Magazine, 2005, 69(5): 877–886
https://doi.org/10.1180/0026461056950295
8 Y Wang, S L Shvartsev, C Su. Genesis of arsenic/fluoride-enriched soda water: a case study at Datong, northern China. Applied Geochemistry, 2009, 24(4): 641–649
https://doi.org/10.1016/j.apgeochem.2008.12.015
9 A Farooqi, H Masuda, N Firdous. Toxic fluoride and arsenic contaminated groundwater in the Lahore and Kasur districts, Punjab, Pakistan and possible contaminant sources. Environmental Pollution, 2007, 145(3): 839–849
https://doi.org/10.1016/j.envpol.2006.05.007 pmid: 16777300
10 A Farooqi, H Masuda, M Kusakabe, M Naseem, N Firdous. Distribution of highly arsenic and fluoride contaminated groundwater from east Punjab, Pakistan, and the controlling role of anthropogenic pollutants in the natural hydrological cycle. Geochemical Journal, 2007, 41(4): 213–234
https://doi.org/10.2343/geochemj.41.213
11 A Farooqi, H Masuda, R Siddiqui, M Naseem. Sources of arsenic and fluoride in highly contaminated soils causing groundwater contamination in Punjab, Pakistan. Archives of Environmental Contamination and Toxicology, 2009, 56(4): 693–706
https://doi.org/10.1007/s00244-008-9239-x pmid: 18937006
12 M L Gomez, M T Blarasin, D E Martinez. Arsenic and fluoride in a loess aquifer in the central area of Argentina. Environmental Geology, 2009, 57(1): 143–155
https://doi.org/10.1007/s00254-008-1290-4
13 P L Smedley, M Zhang, G Zhang, Z Luo. Mobilisation of arsenic and other trace elements in fluviolacustrine aquifers of the Huhhot Basin, Inner Mongolia. Applied Geochemistry, 2003, 18(9): 1453–1477
https://doi.org/10.1016/S0883-2927(03)00062-3
14 G Q Wang, Y Z Huang, B Y Xiao, X C Qian, H Yao, Y Hu, Y L Gu, C Zhang, K T Liu. Toxicity from water containing arsenic and fluoride in Xinjiang. Fluoride, 1997, 30(2): 81–84
15 C Zhu, G Bai, X Liu, Y Li. Screening high-fluoride and high-arsenic drinking waters and surveying endemic fluorosis and arsenism in Shaanxi Province in western China. Water Research, 2006, 40(16): 3015–3022
https://doi.org/10.1016/j.watres.2006.06.026 pmid: 16904724
16 MHPRC. Standards for Dinking Water Quality. Beijing: Ministry of Health of the People’s Republic of China, 2007.
17 R Devi, E Alemayehu, V Singh, A Kumar, E Mengistie. Removal of fluoride, arsenic and coliform bacteria by modified homemade filter media from drinking water. Bioresource Technology, 2008, 99(7): 2269–2274
https://doi.org/10.1016/j.biortech.2007.05.002 pmid: 17596936
18 T B Mlilo, L R Brunson, D A Sabatini. Arsenic and fluoride removal using simple materials. Journal of Environmental Engineering, 2010, 136(4): 391–398
https://doi.org/10.1061/(ASCE)EE.1943-7870.0000154
19 M Pinon-Miramontes, R G Bautista-Margulis, A Perez-Hernandez. Removal of arsenic and fluoride from drinking water with cake alum and a polymeric anionic flocculent. Fluoride, 2003, 36(2): 122–128
20 A P Padilla, H Saitua. Performance of simultaneous arsenic, fluoride and alkalinity (bicarbonate) rejection by pilot-scale nanofiltration. Desalination, 2010, 257(1–3): 16–21
https://doi.org/10.1016/j.desal.2010.03.022
21 X Zhao, B Zhang, H Liu, J Qu. Simultaneous removal of arsenite and fluoride via an integrated electro-oxidation and electrocoagulation process. Chemosphere, 2011, 83(5): 726–729
https://doi.org/10.1016/j.chemosphere.2011.01.055 pmid: 21392815
22 A M Ingallinella, V A Pacini, R G Fernández, R M Vidoni, G Sanguinetti. Simultaneous removal of arsenic and fluoride from groundwater by coagulation-adsorption with polyaluminum chloride. Journal of Environmental Science and Health Part A, 2011, 46(11): 1288–1296
pmid: 21879862
23 S Deng, H Liu, W Zhou, J Huang, G Yu. Mn-Ce oxide as a high-capacity adsorbent for fluoride removal from water. Journal of Hazardous Materials, 2011, 186(2–3): 1360–1366
https://doi.org/10.1016/j.jhazmat.2010.12.024 pmid: 21208743
24 Y F Pan, C T Chiou, T F Lin. Adsorption of arsenic(V) by iron-oxide-coated diatomite (IOCD). Environmental Science and Pollution Research International, 2010, 17(8): 1401–1410
https://doi.org/10.1007/s11356-010-0325-z pmid: 20383794
25 Z Ren, G Zhang, J P Chen. Adsorptive removal of arsenic from water by an iron-zirconium binary oxide adsorbent. Journal of Colloid and Interface Science, 2011, 358(1): 230–237
https://doi.org/10.1016/j.jcis.2011.01.013 pmid: 21440898
26 K Biswas, S K Saha, U C Ghosh. Adsorption of fluoride from aqueous solution by a synthetic Iron(III)-Aluminum(III) mixed oxide. Industrial & Engineering Chemistry Research, 2007, 46(16): 5346–5356
https://doi.org/10.1021/ie061401b
27 H J Hong, W Farooq, J S Yang, J W Yang. Preparation and evaluation of Fe-Al binary oxide for arsenic removal: comparative study with single metal oxides. Separation Science and Technology, 2010, 45(12–13): 1975–1981
https://doi.org/10.1080/01496395.2010.493790
28 Y Masue, R H Loeppert, T A Kramer. Arsenate and arsenite adsorption and desorption behavior on coprecipitated aluminum:iron hydroxides. Environmental Science & Technology, 2007, 41(3): 837–842
https://doi.org/10.1021/es061160z pmid: 17328191
29 M G Sujana, S Anand. Iron and aluminium based mixed hydroxides: a novel sorbent for fluoride removal from aqueous solutions. Applied Surface Science, 2010, 256(23): 6956–6962
https://doi.org/10.1016/j.apsusc.2010.05.006
30 M G Sujana, G Soma, N Vasumathi, S Anand. Studies on fluoride adsorption capacities of amorphous Fe/Al mixed hydroxides from aqueous solutions. Journal of Fluorine Chemistry, 2009, 130(8): 749–754
https://doi.org/10.1016/j.jfluchem.2009.06.005
31 H Tamura, A Tanaka, K Mita, R Furuichi. Surface hydroxyl site densities on metal oxides as a measure for the ion-exchange capacity. Journal of Colloid and Interface Science, 1999, 209(1): 225–231
https://doi.org/10.1006/jcis.1998.5877 pmid: 9878157
32 A Jain, K P Raven, R H Loeppert. Arsenite and arsenate adsorption on ferrihydrite: surface charge reduction and net OH − release stoichiometry. Environmental Science & Technology, 1999, 33(8): 1179–1184
https://doi.org/10.1021/es980722e
33 U Schwertmann, R M Taylor. Iron Oxides. In: J B Dixon, eds. Minerals in Soil Environments. Madison WI: Soil Science Society of America, 1989
34 X Krokidis, P Raybaud, A E Gobichon, B Rebours, P Euzen, H Toulhoat. Theoretical study of the dehydration process of boehmite to gamma-alumina. Journal of Physical Chemistry B, 2001, 105(22): 5121–5130
https://doi.org/10.1021/jp0038310
35 Y T Liu, D Hesterberg. Phosphate bonding on noncrystalline Al/Fe-hydroxide coprecipitates. Environmental Science & Technology, 2011, 45(15): 6283–6289
https://doi.org/10.1021/es201597j pmid: 21714572
36 X H Guan, J M Wang, C C Chusuei. Removal of arsenic from water using granular ferric hydroxide: macroscopic and microscopic studies. Journal of Hazardous Materials, 2008, 156(1–3): 178–185
https://doi.org/10.1016/j.jhazmat.2007.12.012 pmid: 18206296
37 Y H Li, S G Wang, A Y Cao, D Zhao, X F Zhang, C L Xu, Z K Luan, D B Ruan, J Liang, D H Wu, B Q Wei. Adsorption of fluoride from water by amorphous alumina supported on carbon nanotubes. Chemical Physics Letters, 2001, 350(5–6): 412–416
https://doi.org/10.1016/S0009-2614(01)01351-3
38 S George, P Pandit, A B Gupta. Residual aluminium in water defluoridated using activated alumina adsorption—modeling and simulation studies. Water Research, 2010, 44(10): 3055–3064
https://doi.org/10.1016/j.watres.2010.02.028 pmid: 20231028
39 M Mohapatra, K Rout, P Singh, S Anand, S Layek, H C Verma, B K Mishra. Fluoride adsorption studies on mixed-phase nano iron oxides prepared by surfactant mediation-precipitation technique. Journal of Hazardous Materials, 2011, 186(2–3): 1751–1757
https://doi.org/10.1016/j.jhazmat.2010.12.076 pmid: 21232851
40 W Stumm, J J Morgan. Aquatic Chemistry: Chemical Equilibria and Rates in Natural Waters, 3rd ed. New York: John Wiley & Sons, Inc, 1996
41 V Kumar, N Talreja, D Deva, N Sankararamakrishnan, A Sharma, N Verma. Development of bi-metal doped micro- and nano multi-functional polymeric adsorbents for the removal of fluoride and arsenic(V) from wastewater. Desalination, 2011, 282SI: 27–38
https://doi.org/10.1016/j.desal.2011.05.013
42 X H Guan. Adsorption of phosphates and organic acids on aluminum hydroxide in aquatic environment-mechanisms and interactions. Dissertation for the Doctoral Degree. Hong Kong: Hong Kong University of Science and Technology, 2005
[1] Weiyi Liu, Ting Pan, Hang Liu, Mengyun Jiang, Tingting Zhang. Adsorption behavior of imidacloprid pesticide on polar microplastics under environmental conditions: critical role of photo-aging[J]. Front. Environ. Sci. Eng., 2023, 17(4): 41-.
[2] Mei Shi, Xiao Wang, Mengying Shao, Lun Lu, Habib Ullah, Hao Zheng, Fengmin Li. Resource utilization of typical biomass wastes as biochars in removing plasticizer diethyl phthalate from water: characterization and adsorption mechanisms[J]. Front. Environ. Sci. Eng., 2023, 17(1): 5-.
[3] Jie Wu, Jian Lu, Jun Wu. Effect of gastric fluid on adsorption and desorption of endocrine disrupting chemicals on microplastics[J]. Front. Environ. Sci. Eng., 2022, 16(8): 104-.
[4] Ning Wang, Jiangtao Feng, Wei Yan, Luohong Zhang, Yonghong Liu, Ruihua Mu. Dual-functional sites for synergistic adsorption of Cr(VI) and Sb(V) by polyaniline-TiO2 hydrate: Adsorption behaviors, sites and mechanisms[J]. Front. Environ. Sci. Eng., 2022, 16(8): 105-.
[5] Yanlin Li, Bo Wang, Lei Zhu, Yixing Yuan, Lujun Chen, Jun Ma. Selective targeted adsorption and inactivation of antibiotic-resistant bacteria by Cr-loaded mixed metal oxides[J]. Front. Environ. Sci. Eng., 2022, 16(6): 68-.
[6] Feng Chen, Shihao Guo, Yihao Wang, Lulu Ma, Bing Li, Zhimin Song, Lei Huang, Wen Zhang. Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon adsorbent derived from loofah sponge[J]. Front. Environ. Sci. Eng., 2022, 16(5): 57-.
[7] Mahsa Kheirandish, Chunjiang An, Zhi Chen, Xiaolong Geng, Michel Boufadel. Numerical simulation of benzene transport in shoreline groundwater affected by tides under different conditions[J]. Front. Environ. Sci. Eng., 2022, 16(5): 61-.
[8] Xuemei Hu, Shijie You, Fang Li, Yanbiao Liu. Recent advances in antimony removal using carbon-based nanomaterials: A review[J]. Front. Environ. Sci. Eng., 2022, 16(4): 48-.
[9] Hui Hu, Lei Jiang, Longli Sun, Yanling Gao, Tian Wang, Chenguang Lv. Effective and selective separation of perrhenate from acidic wastewater by super-stable, superhydrophobic, and recyclable biosorbent[J]. Front. Environ. Sci. Eng., 2022, 16(2): 21-.
[10] Jie Wu, Jian Lu, Jun Wu. Adsorption and desorption of steroid hormones on saline soil[J]. Front. Environ. Sci. Eng., 2022, 16(11): 140-.
[11] Mingyi Yang, Lin Shi, Di Zhang, Zhaohui He, Aiping Liang, Xiao Sun. Adsorption of herring sperm DNA onto pine sawdust biochar: Thermodynamics and site energy distribution[J]. Front. Environ. Sci. Eng., 2022, 16(11): 144-.
[12] Yanhui Dai, Jian Zhao, Chunxiao Sun, Diying Li, Xia Liu, Zhenyu Wang, Tongtao Yue, Baoshan Xing. Interaction and combined toxicity of microplastics and per- and polyfluoroalkyl substances in aquatic environment[J]. Front. Environ. Sci. Eng., 2022, 16(10): 136-.
[13] Na Li, Boqiang Gao, Ran Yang, Hu Yang. Simple fabrication of carboxymethyl cellulose and κ-carrageenan composite aerogel with efficient performance in removal of fluoroquinolone antibiotics from water[J]. Front. Environ. Sci. Eng., 2022, 16(10): 133-.
[14] Xianying Ma, Xinhui Zhou, Mengjie Zhao, Wenzhuo Deng, Yanxiao Cao, Junfeng Wu, Jingcheng Zhou. Polypropylene microplastics alter the cadmium adsorption capacity on different soil solid fractions[J]. Front. Environ. Sci. Eng., 2022, 16(1): 3-.
[15] Ziyue Yin, Qing Lin, Shaohui Xu. Using hydrochemical signatures to characterize the long-period evolution of groundwater information in the Dagu River Basin, China[J]. Front. Environ. Sci. Eng., 2021, 15(5): 105-.
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed