Phosphogypsum-Modified Vinasse Shell Biochar as a Novel Low-Cost Material for High-Efficiency Fluoride Removal
Abstract
:1. Introduction
2. Results and Discussion
2.1. Characterization Analysis
2.1.1. SEM-EDS
2.1.2. XRD
2.1.3. FTIR
2.1.4. BET
2.1.5. Zeta Potential
2.1.6. XPS
2.2. Batch Adsorption
2.2.1. Effect of Pyrolysis Temperature
2.2.2. Effect of Dosage
2.2.3. Effect of pH
2.2.4. Effect of Co-Existing Anions
2.3. Adsorption Kinetics Analysis
2.4. Adsorption Isotherm Study
2.5. Adsorption Thermodynamic Study
2.6. Mechanism of F− Adsorption
- (1)
- Ion exchange. The analysis of FTIR and XPS revealed that the surface of MVS600 was rich in hydroxyl groups, and the content of the hydroxyl group became less after adsorption. This indicated that when fluoride approached MVS600, the hydroxyl groups on the surface were replaced by fluorine ions, as shown in Equation (1);
- (2)
- Chemical precipitation. Both XRD analysis and XPS analysis confirmed the production of CaF2. F− and Ca2+ on the MVS600 surface had a very tight attraction for each other and easily formed CaF2 precipitates, as shown in Equation (2);
- (3)
- Electrostatic attraction. It could be seen from the zeta potential analysis under low pH conditions that the C–O groups on the surface of MVS600 were protonated to C–OH+ and carried a large number of positive charges. Negatively charged fluorine ions were removed by electrostatic interaction with them, as shown in Equation (3). The formation of weakly ionized HF under strongly acidic conditions and deprotonation of surface functional groups under alkaline conditions reduced the degree of F adsorption. Under near-neutral conditions, F− adsorption could be described using other equations;
- (4)
- Hydrogen bonding. Due to the high electronegativity of O and F, the shared electron pair of –OH groups on the surface of MVS600 was biased toward O, so H easily interacted with F and formed an –OH⋯F hydrogen bond, as shown in Equation (4). This might be responsible for the change in O–H binding energy before and after adsorption in the XPS spectra.
3. Experimental Section
3.1. Reagents
3.2. Preparation of Materials
3.3. Physicochemical Characterization
3.4. Adsorptive Experiments
3.4.1. Adsorption Kinetics Modeling
3.4.2. Adsorption Isotherm Modeling
3.4.3. Adsorption Thermodynamics
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Samples | BET Surface Area (m2/g) | Total Pore Volume (cm3/g) | Average Pore Diameter (nm) |
---|---|---|---|
VS600 | 64.5 | 0.1487 | 9.22 |
MVS600 | 71.3 | 0.1492 | 8.37 |
C0 (mg/L) | Pseudo-First Order Model | ||||
---|---|---|---|---|---|
qe,exp (mg/g) | qe,cal (mg/g) | k1 (1/min) | R2 | SD | |
100 | 100.5 | 46.99 | 0.02154 | 0.9391 | 0.264 |
60 | 63.0 | 37.41 | 0.02222 | 0.9583 | 0.223 |
20 | 22.5 | 12.38 | 0.02347 | 0.9606 | 0.229 |
Pseudo-Second Order Model | |||||
qe,exp (mg/g) | qe,cal (mg/g) | k2 (g/mg·min) | R2 | SD | |
100 | 100.5 | 101.3 | 0.001929 | 0.9989 | 0.0192 |
60 | 63.0 | 63.86 | 0.002108 | 0.9967 | 0.0526 |
20 | 22.5 | 22.84 | 0.006834 | 0.9977 | 0.122 |
Intraparticle Diffusion Model | |||||
qe,exp (mg/g) | C (mg/g) | k3 (mg/g·min1/2) | R2 | SD | |
100 | 100.5 | 42.84 | 5.17 | 0.8510 | 9.01 |
60 | 63.0 | 21.28 | 3.635 | 0.8882 | 5.37 |
20 | 22.5 | 8.53 | 1.237 | 0.8643 | 2.04 |
Elovich Model | |||||
qe,exp (mg/g) | α (mg/(g·min)) | β (g/mg) | R2 | SD | |
100 | 100.5 | 150.9 | 0.07321 | 0.9862 | 2.74 |
60 | 63.0 | 44.76 | 0.1058 | 0.9963 | 0.973 |
20 | 22.5 | 21.96 | 0.3082 | 0.9867 | 0.638 |
Isotherm Models | Parameters | Values (25 °C) | Values (35 °C) | Values (45 °C) |
---|---|---|---|---|
Langmuir | KL/(L/mg) | 0.01887 | 0.02678 | 0.04010 |
qm/(mg/g) | 253.8 | 228.8 | 209.2 | |
R2 | 0.9654 | 0.9419 | 0.9136 | |
SD | 2.14 | 2.64 | 4.47 | |
Freundich | KF ((mg/g) × (L/mg)1/n) | 6.482 | 8.276 | 11.79 |
1/n | 0.7829 | 0.7493 | 0.6844 | |
R2 | 0.9988 | 0.9940 | 0.9980 | |
SD | 1.26 | 3.14 | 2.11 | |
Temkin | AT/(L/mg) | 39.91 | 40.15 | 38.66 |
BT | 0.3091 | 0.3792 | 0.5371 | |
R2 | 0.9598 | 0.9677 | 0.9366 | |
SD | 6.14 | 5.73 | 8.55 | |
Sips | qm | 290.9 | 321.9 | 353.5 |
Ks | 0.015 | 0.014 | 0.016 | |
ms | 0.9823 | 0.9002 | 0.8836 | |
R2 | 0.9963 | 0.9937 | 0.9925 | |
SD | 1.83 | 2.59 | 3.12 |
Material | Qmax (mg/g) | Conditions | Reference |
---|---|---|---|
Zirconium impregnated carbon | 40.02 | W = 10 g/L, 4.0, 25 °C | [71] |
SWCNTs | 63.2 | W = 0.6 g/L, pH = 6.0, T = 30 °C | [72] |
GAC-Fe3O4 | 2.74 | W = 1 g/L, pH = 3.0, T = 25 °C | [73] |
Mytilus coruscus shells | 82.93 | W = 3.33 g/L, pH = 7.0, T = 25 °C | [74] |
Y-Zr-Al composite | 31.0 | W = 1 g/L, pH = 7.0, T = 25 °C | [75] |
Al2O3 microfiber clusters | 14.96 | W = not mentioned, pH = 5.0, T = 40 °C | [76] |
AC-Si-Mg-La | 54.83 | W = 0.2 g/L, pH = 5.0, T = 25 °C | [17] |
La/Fe/Al loaded rice straw biochar | 111.11 | W = 1 g/L, pH = 7.0, T = 25 °C | [77] |
DTAB/H2O2–clay | 53.66 | W = 2 g/L, pH = 2.0, T = 25 °C | [78] |
HAO@GO | 129.23 | W = 0.05 g/L, pH = 7.0, T = 25 °C | [79] |
rGO-Ce/Ag | 434.78 | W = not mentioned, pH = 7.0, T = 25 °C | [80] |
Ca modified Mg-Zr MMOs | 370.37 | W = 0.5 g/L, pH = 7.0, T = 25 °C | [81] |
MVS600 | 290.9 | W = 0.667 g/L, pH = 7.0, T = 25 °C | Present study |
T (°C) | Kd | ΔG0 (kJ/mol) | ΔH0 (kJ/mol) | ΔS0 (J/(mol∙K)) |
---|---|---|---|---|
25 | 6.482 | −4.633 | 23.53 | 94.29 |
35 | 8.276 | −5.414 | 23.53 | 94.29 |
45 | 11.79 | −6.526 | 23.53 | 94.29 |
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Liu, Z.; Zhang, J.; Mou, R. Phosphogypsum-Modified Vinasse Shell Biochar as a Novel Low-Cost Material for High-Efficiency Fluoride Removal. Molecules 2023, 28, 7617. https://doi.org/10.3390/molecules28227617
Liu Z, Zhang J, Mou R. Phosphogypsum-Modified Vinasse Shell Biochar as a Novel Low-Cost Material for High-Efficiency Fluoride Removal. Molecules. 2023; 28(22):7617. https://doi.org/10.3390/molecules28227617
Chicago/Turabian StyleLiu, Zheng, Jingmei Zhang, and Rongmei Mou. 2023. "Phosphogypsum-Modified Vinasse Shell Biochar as a Novel Low-Cost Material for High-Efficiency Fluoride Removal" Molecules 28, no. 22: 7617. https://doi.org/10.3390/molecules28227617