Recently Developed Adsorbing Materials for Fluoride Removal from Water and Fluoride Analytical Determination Techniques: A Review
Abstract
:1. Introduction
2. Fluoride Removal from Drinking Water by Adsorption
2.1. Carbon-Based Adsorbents
2.1.1. Activated Carbon
Activated Carbon Fibers Modified with Zirconium (Zr-ACF)
Activated Carbon of Avocado Seeds (ACAS)
Activated Carbon Derived from CaCl2-Modified Crocus Sativus Leaves (AC-CMCSL)
La/Mg/Si-Activated Carbon
2.1.2. Graphene Oxide
Graphene Oxide/Alumina Nano-Composite
Graphene Oxide–Aluminum Oxyhydroxide Interaction (GO–Al–O(OH))
Graphene Oxide/Eggshell (GO/ES) Adsorbent
Graphene Oxide Anchored Sand (ZIGCS) Functionalized by Zr(IV)
2.1.3. Carbon Nanotubes (CNTs)
Hydroxyapatite/Multi-Walled Carbon Nanotubes (HA-MWCNTs)
2.2. Other Adsorbents
2.2.1. SRH Adsorbent
2.2.2. Fe@BDC and Fe@ABDC Fe-Based MOF Composites
2.2.3. Modified Kaolin–Bentonite Composites (KBNPs)
2.2.4. Ce\Zn Ceramic Oxides
2.2.5. Porous MgO Nanostructures
2.2.6. Lanthanum Modified Mesoporous Alumina (La/MA)
2.2.7. Iron Oxide Nanoparticles Modified with Ionic Liquid (IL-Iron Oxide)
2.2.8. γ-Al2O3/γ-Fe2O3 Composite
2.2.9. Zirconium-Based Metal Organic Framework (MOF-801) Adsorbent
2.2.10. Biosynthetic Crystals by Microbially Induced Calcium Carbonate Precipitation (BC-ICP)
2.2.11. Lanthanum Ferrite Nanoparticles (LaFeO3 NPs)
Adsorbent | pH | Adsorbent Dosage (g L−1) | Time (min) | Adsorption Capacity (mg g−1) | Regeneration (Cycles) | ΔG° (kJ mol−1) (at 303 K) | ΔH° (kJ mol−1) | Ref. |
---|---|---|---|---|---|---|---|---|
Activated Carbon Based Adsorbents | ||||||||
Zr-ACF | 7.0 | 2.0 | 30 | 28.50 | - | <0 | >0 | [50] |
ACAS | 6.0 | 19.0 | 60 | 1.20 | - | - | - | [54] |
AC-CMCSL | 4.5 | 15.0 | 70 | 2.01 | - | −0.20576 | +22.6 | [55] |
La/Mg/Si-AC | 8.0 | 0.2 | 150 | 220.5 | 5 | −1.41 × 104 (at 308 K) | +7.5 × 103 | [56] |
Graphene Oxide Based Adsorbents | ||||||||
GO/Al2O3 | 6.0 | 8.0 | 90 | 6.30 | 4 | −2.32 | +24.6 | [62] |
GO–Al–O(OH) | 7.0 | 2.0 | 60 | 51.42 | - | −5.84 | +21.4 | [63] |
GO/ES | - | 0.05 | 120 | 56.0 | - | 0.1865 (at 298 K) | −12.7 | [64] |
ZIGCS | 4.0 | 2.0 | 60 | 175.0 | 5 | −0.045 (at 308 K) | +30.6 | [65] |
Carbon Nanotubes Based Adsorbents | ||||||||
HA-MWCNTs | 7.0 | 2.0 | 120 | 39.22 | - | −1.964 | +6.4 | [67] |
Other Adsorbents | ||||||||
SRH | 8.0 | 4.0 | 60 | 6.0 | 4 | +2.6 | +2.6 | [68] |
Fe@BDC & Fe@ABDC MOF | 6.6 | 0.1 | 60 | 4.90 & 4.92 | 6 | +0.6 & +1.2 | +0.6 & +1.2 | [69] |
KBNPs | 6.5 | 6.0 | 120 | 1.72 | - | - | - | [70] |
Ce\Mn ceramic oxide | 7.0 | - | 15 | 257.8 | - | - | - | [71] |
MgO | 6.7 | 0.2 | 60 | 29,131 | 5 | −47.6 | −47.6 | [72] |
La/MA | 6.0 | 2.0 | 60 | 26.45 | 5 | + 3.9 | +3.9 | [73] |
IL-iron oxide | 8.0 | 0.06 | 30 | 67.9 | 3 | +6.6 | +6.6 | [74] |
γ-Al2O3/γ-Fe2O3 | 7.0 | 1.0 | 15 | 105.04 | 5 | +14.4 | +14.4 | [75] |
MOF-801 | - | 1.0 | 120 | 17.33 | 4 | - | - | [76] |
BC-ICP | 7.0 | 1.0 | - | 5.10 | - | +2.3 | +2.3 | [77] |
LaFeO3 NPs | 5.0 | 0.9 | 60 | 2.58 | - | −0.51 | −0.51 | [78] |
3. Analytical Methods for Fluoride Determination in Drinking Water
3.1. Electrochemical Methods
3.2. Chromatographic Methods
3.3. Spectroscopic Methods
3.4. Microfluidic Methods
3.5. Sensors
4. Conclusions
- The modification of activated carbon with metal oxides and hydroxides was found to effectively remove fluoride from water, providing adsorption capacities of up to 25 mg g−1 for the case of Zr-ACF and 220.5 mg g−1 for La/Mg/Si-AC.
- Similarly, graphene oxide modification enhanced significantly the adsorbing efficiency, exhibiting ever higher adsorption capacities than those achieved with modified activated carbon which, in the case of ZIGCS, reached 175 mg g−1.
- The use of MgO nanostructures exhibited a maximum Langmuir adsorption capacity of 29,131 mg g−1, which is the highest for any adsorbent reported till now for the development of fluoride adsorbents.
- Regeneration experiments can be performed, provided that all the materials can be recycled from three to six cycles.
- Al materials reported are effective in the pH range relevant to drinking water treatment (i.e., 6–8).
- Ion-selective electrodes, spectrometry, ionic chromatography, etc., are considered as well-established and are widely used.
- The development of new methodologies that can selectively, accurately, and rapidly detect fluoride is of paramount importance and, thus, is still in the forefront of research.
- Currently, a plethora of promising sensing systems that take advantage of the technological progress of our times (e.g., the development of smartphone-based sensors) are gaining more and more popularity.
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Fluoride Concentration (mg L−1) | Effects | International Standards Organization | Permissible Limit (mg L−1) |
---|---|---|---|
<0.5 | Prevention of teeth cavities | World Health Organization (WHO) | 0.6–1.5 |
0.5–1.5 | Helps in bones and teeth development | Bureau of Indian Standards (BIS) | 0.6–1.5 |
1.5–4 | Dental problems in children | US Public Health Standards | 0.8 |
>4 | Dental and skeleton fluorosis | Indian Council of Medical Research (ICMR) | 1.0 |
>10 | Crippling skeletal fluorosis, possibly cancer | Directive 98/83/EC | 1.5 |
Reagent | Method | Application | Linear Range | LOD | Ref. |
---|---|---|---|---|---|
7-O-tert-butyldiphenylsilyl-4-methylcoumarin | Fluorescence | Surface and ground water | 0.2–10 mg L−1 | 0.2 mg L−1 | [2] |
Hydroxyl-decorated coumarin connected with the bulky tert-butyldiphenyloxysilyl group | Fluorescence | Drinking water | 0–9.15 mg L−1 | 0.043 mg L−1 | [120] |
2-hydroxy-1-naphthalene formaldehyde | Fluorescence | Drinking water | 0–50 equiv | 1.4 × 10−8 M | [121] |
Silyl capped hydroxylpyrenealdehyde | Colorimetric and Fluorescence | Drinking water and toothpaste | 0–50 μM and 50–250 μM | 2.7 μg L−1 | [50] |
Iron (III) thiocyanate | Colorimetric | Drinking water | - | - | [122] |
Naphthalene−benzothiazole as the fluorophore and tert-butyldimethylsilyl as the reactive groups (Sensor 1) Naphthalene−benzothiazole as the fluorophore and tert-butyldiphenylsilyl as the reactive groups (Sensor 2) | Fluorescence | Drinking water | 0–6 μM (Sensor 1) 0–40 μM (Sensor 2) | 73 nM (Sensor 1) 138 nM (Sensor 2) | [123] |
Nitrogen-doped GO | Fluorescence | Water | - | 1 × 10−12 M | [124] |
Zirconium-SPADNS | Colorimetric | Ground water | 0.2–2 mg L−1 | 0.2 mg L−1 | [35] |
Near-cubic ceria@ zirconia nanocages) and a xylenol | Colorimetric | Field water | 0.1–5 mg L−1 | 0.06 mg L−1 | [125] |
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Tolkou, A.K.; Manousi, N.; Zachariadis, G.A.; Katsoyiannis, I.A.; Deliyanni, E.A. Recently Developed Adsorbing Materials for Fluoride Removal from Water and Fluoride Analytical Determination Techniques: A Review. Sustainability 2021, 13, 7061. https://doi.org/10.3390/su13137061
Tolkou AK, Manousi N, Zachariadis GA, Katsoyiannis IA, Deliyanni EA. Recently Developed Adsorbing Materials for Fluoride Removal from Water and Fluoride Analytical Determination Techniques: A Review. Sustainability. 2021; 13(13):7061. https://doi.org/10.3390/su13137061
Chicago/Turabian StyleTolkou, Athanasia K., Natalia Manousi, George A. Zachariadis, Ioannis A. Katsoyiannis, and Eleni A. Deliyanni. 2021. "Recently Developed Adsorbing Materials for Fluoride Removal from Water and Fluoride Analytical Determination Techniques: A Review" Sustainability 13, no. 13: 7061. https://doi.org/10.3390/su13137061