Surface Modifications of Superparamagnetic Iron Oxide Nanoparticles with Polyvinyl Alcohol, Chitosan, and Activated Carbon or Graphite as Methylene Blue Adsorbents—Comparative Study
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials
2.2. Characterization
2.3. Determining the Adsorption and Desorption Capacity of Methylene Blue on SPION/PVA/CS/AC and SPION/PVA/CS/GR
2.4. Determining the Adsorption Kinetics, Adsorption Isotherm, and Desorption Kinetics
3. Results and Discussion
3.1. Characterization of SPION/PVA/CS/AC and SPION/PVA/CS/GR
3.1.1. FE-SEM Analysis
3.1.2. XRD Analysis
3.1.3. FTIR Analysis
3.1.4. VSM Analysis
3.1.5. BJH Analysis
3.2. Adsorption
3.3. Desorption
3.4. Comparison
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
Abbreviations
m | Mass of the Nanoparticles (g) |
V | sample volume (mL) |
C0 | initial concentration (mg/mL) |
Ct | concentration at time t (mg/mL) |
Ce | equilibrium aqueous-phase concentration adsorbate (mg/L) |
Q0 | theoretical adsorption capacity (mg/g) |
Qe | amount of MB absorbed per unit mass of nanoparticle at the equilibrium (mg/g) |
Qt | amount of MB absorbed per unit mass of nanoparticle at time t (mg/g) |
Qm | quantity of adsorbate adsorbed in a single monolayer (mg/g) |
α | Theoretical initial adsorption rate |
𝜷 | Theoretical desorption rate |
Mt | Released mass fraction at a time (t) |
M∞ | The Amount of MB at Equilibrium State |
ϴ | fractional surface coverage |
X2 | Chi-square value |
nKP | Korsmeyer-Peppas release exponent factor |
kKP | Korsmeyer-Peppas release rate constant |
kH | Higuchi release rate constant |
KL | constant related to the free adsorption energy and the reciprocal of the concentration at which half saturation of the adsorbent is reached |
k0 | Constant mass fraction at a time (t) release |
k1 | Pseudo-first-order rate constant (s−1) |
k2 | Pseudo-second-order rate constant (s−1) |
ka | Respective rate constant for adsorption |
kd | Respective rate constant for desorption |
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Materials | Peaks (cm−1) | Functional Group | Ref. |
---|---|---|---|
SPION | 3419 | O−H symmetric stretching | [73,74] |
1629 | Carbonyl C=O stretching band | [73,74] | |
587 | Vibration Fe−O | [73,74,75] | |
447 | Vibration Fe−O | [75,76] | |
PVA | 3397 | O−H symmetric stretching | [77,78] |
2944 | CH2 asymmetric stretching | [78,79,80] | |
1736 | C=O stretching band | [79,80,81] | |
1657 | O−H bending mode of OH groups | [80,82,83] | |
1440 | CH2 bending | [78,79,80,82] | |
1330 | CH wagging | [80] | |
1266 | C−O−C stretching | [84] | |
1145 | C−O stretching | [78,80,82,85] | |
1098 | C−O stretching | [78,80,82,85] | |
947 | CH2 rocking | [80] | |
853 | C−C stretching | [80,82] | |
CS | 3425 | O−H symmetric stretching and −NH symmetrical vibration | [78,86] |
2923 | C−H symmetric stretching | [86,87,88] | |
1650 | C=O stretching of amide I | [86,87,88,89] | |
1423 | C−H bending | [88] | |
1382 | CH2 in CH2OH group | [90] | |
1323 | C−N stretching of amide III | [86] | |
1262 | C−H bond in the pyranose ring | [90] | |
1157 | C−O−C asymmetric stretching Saccharide structure of chitosan | [86,88,91] | |
1077 | C−O stretching | [78,88,92] | |
1030 | C−O stretching | [86,88] | |
897 | Saccharide structure of chitosan | [78,91] | |
AC | 3390 | O−H stretching vibration | [93,94] |
2920 | C−H stretching vibration | [94] | |
2855 | C−H stretching vibration | [94] | |
1593 | C=C stretching vibration in aromatic rings | [95] | |
1396 | C−H stretching vibration C−O−H bending vibration | [93] | |
1166 | C−O−H stretching vibration | [95] | |
807 | C−C stretching vibration | [95] | |
GR | 3422 | O−H stretching vibration | [96,97,98] |
2919 | CH2 asymmetric stretching | [96] | |
2856 | CH2 symmetric stretching | [96] | |
1632 | C=C stretching vibration | [96,98] | |
1165 | C−O stretching vibration | [99] | |
1116 | C−O stretching vibration | [99] | |
1065 | C−O stretching of alkoxy group | [96,98] | |
SPION/PVA/CS/AC | 3414 | O−H stretching vibration | This research |
2923 | CH2 asymmetric vibration C−H symmetric stretching | This research | |
1614 | C=O stretching band O−H bending mode of OH groups | This research | |
1384 | C−H stretching vibration C−O−H bending vibration CH2 in CH2OH group | This research | |
1248 | C−O−C stretching C−H bond in the pyranose ring | This research | |
1160 | C−O stretching C−O−C asymmetric stretching Saccharide structure of chitosan C−O−H stretching vibration | This research | |
1064 | C−O stretching | This research | |
569 | Vibration Fe−O | This research | |
SPION/PVA/CS/GR | 3434 | O−H stretching vibration | This research |
2924 | CH2 asymmetric vibration C−H symmetric stretching | This research | |
2860 | CH2 symmetric stretching | This research | |
1629 | C=O stretching band C=C stretching vibration | This research | |
1395 | CH2 in CH2OH group CH wagging | This research | |
1162 | C−O−C asymmetric stretching Saccharide structure of chitosan C−O stretching vibration | This research | |
1115 | C−O stretching vibration | This research | |
1058 | C−O stretching of alkoxy group C−O stretching | This research | |
565 | Vibration Fe−O | This research |
SPION/PVA/CS/AC | SPION/PVA/CS/GR | |
---|---|---|
Surface area (m2/g) | 563.891 | 8.059 |
Pore diameter (Å) | 9.719 | 27.516 |
Pore volume (cm3/g) | 0.251 | 0.017 |
Material | Initial MB Concentration (mg/mL) | Qt (mg/g) | %LC (%) | %EE (%) |
---|---|---|---|---|
SPION/PVA/CS/AC | 0.015 | 7.6 ± 0.2 | 0.76 ± 0.02 | 30.3 ± 0.7 |
0.02 | 14.9 ± 0.1 | 1.5 ± 0.01 | 44.8 ± 0.4 | |
0.025 | 22.4 ± 0.05 | 2.2 ± 0.005 | 53.7 ± 0.1 | |
SPION/PVA/CS/GR | 0.015 | 6.9 ± 0.02 | 0.69 ± 0.002 | 27.7 ± 0.09 |
0.02 | 14.5 ± 0.01 | 1.45 ± 0.001 | 43.4 ± 0.03 | |
0.025 | 22.2 ± 0.004 | 2.22 ± 0.0004 | 53.3 ± 0.009 |
Initial MB Concentration (mg/mL) | ||||
---|---|---|---|---|
0.015 | 0.020 | 0.025 | ||
Pseudo-first order non-linear | Qe mg MB (g particles)−1 | 13.3 | 22.3 | 29.01 |
k1 (g mg−1 day−1) | 1 | 1 | 1 | |
27.2 | 24.1 | 14.5 | ||
Pseudo-second order non-linear | Qe mg MB (g particles)−1 | 13.3 | 22.3 | 29.01 |
k2 (g mg−1 day−1) | 171.8 | 56.2 | 915.9 | |
27.2 | 24.1 | 14.5 | ||
Pseudo-second order linear | Qe mg MB (g particles)−1 | 22.5 | 15.1 | 7.8 |
k2 (g mg−1 day−1) | 0.6 | 0.3 | 0.2 | |
R2 | 0.999 | 0.999 | 0.996 | |
Simplified Elovich | α (mg/(g day)) | 2425.46 | 116,289.7 | 419,458.8 |
β (mg/g) | 2.277 | 1.354 | 0.950 | |
R2 | 0.452 | 0.325 | 0.292 |
Initial MB Concentration (mg/mL) | ||||
---|---|---|---|---|
0.015 | 0.020 | 0.025 | ||
Pseudo-first order non-linear | Qe mg MB (g particles)−1 | 13.3 | 22.3 | 29.01 |
k1 (g mg−1 day−1) | 1 | 1 | 1 | |
28.9 | 25.5 | 14.8 | ||
Pseudo-second order non-linear | Qe mg MB (g particles)−1 | 13.3 | 22.3 | 29.01 |
k2 (g mg−1 day−1) | 171.8 | 56.2 | 915.9 | |
28.9 | 25.5 | 14.8 | ||
Pseudo-second order linear | Qe mg MB (g particles)−1 | 22.3 | 14.6 | 7.1 |
k2 (g mg−1 day−1) | 0.8 | 0.7 | 0.6 | |
R2 | 0.999 | 0.999 | 0.998 | |
Simplified Elovich | α (mg/(g day)) | 140,135.3 | 512,001.3 | 1,076,154.2 |
β (mg/g) | 3.100 | 1.506 | 0.9914 | |
R2 | 0.235 | 0.303 | 0.287 |
Materials | Initial MB Concentration (mg/mL) | kI | I | R2 |
---|---|---|---|---|
SPION/PVA/CS/AC | 0.015 | 0.5 | 5.7 | 0.782 |
0.020 | 0.3 | 13.8 | 0.382 | |
0.025 | 0.2 | 21.8 | 0.253 | |
SPION/PVA/CS/GR | 0.015 | 0.2 | 6.2 | 0.358 |
0.020 | 0.2 | 13.9 | 0.256 | |
0.025 | 0.1 | 21.8 | 0.117 |
Model | Constant | SPION/PVA/CS/AC | SPION/PVA/CS/GR |
---|---|---|---|
Langmuir | kL (L/mg) | −12.06 | −11.98 |
Q0 (mg/g) | 1.06 | 0.68 | |
Average RL | 1.32 ± 0.09 | 1.32 ± 0.09 | |
R2 | 0.94 | 0.96 | |
Freundlich | kF (mg/g) | 9.55 × 10−11 | 1.69 × 10−6 |
(mg/L) | 10.71 | 16.05 | |
R2 | 0.99 | 0.99 |
Materials | Concentration (mg/mL) | % Release Average |
---|---|---|
SPION/PVA/CS/AC | 0.015 | 63.24 ± 8.77 |
0.02 | 27.17 ± 3.53 | |
0.025 | 22.10 ± 2.59 | |
SPION/PVA/CS/GR | 0.015 | 91.29 ± 12.35 |
0.02 | 39.51 ± 4.37 | |
0.025 | 24.42 ± 1.40 |
Korsmeyer–Peppas (KP) | 0th Order | Higuchi | |||||
---|---|---|---|---|---|---|---|
k | n | k | K | KP | 0th order | Higuchi | |
SPION/PVA/CS/AC | |||||||
0.015 | 3.6 | 0.8 | 0.004 | 0.02 | 68.80 | 0.020 | 0.102 |
0.02 | 1.4 | 0.8 | 0.004 | 0.02 | 28.88 | 0.013 | 0.114 |
0.025 | 1.2 | 0.8 | 0.004 | 0.02 | 23.69 | 0.024 | 0.104 |
SPION/PVA/CS/GR | |||||||
0.015 | 6.9 | 0.7 | 0.006 | 0.03 | 101.03 | 0.027 | 0.095 |
0.02 | 1.9 | 0.8 | 0.005 | 0.02 | 43.62 | 0.018 | 0.140 |
0.025 | 1.4 | 0.8 | 0.005 | 0.02 | 26.51 | 0.020 | 0.111 |
Adsorbents | Costs (VND/g) | Adsorption Capacity (mg/g) | %EE (%) | %LC (%) | Adsorption Capacity/Costs (g/VND) |
---|---|---|---|---|---|
SPION/PVA/AC | 681.89 | 21.75 | 57.22 | 2.53 | 31.90 |
SPION/PVA/GR | 1376.63 | 19.87 | 42.30 | 1.99 | 14.43 |
SPION/PVA/CS/AC | 1211.5 | 14.9 | 44.80 | 1.50 | 12.30 |
SPION/PVA/CS/GR | 1761.5 | 14.5 | 43.40 | 1.45 | 8.23 |
SPION/PVA/CS/GO | 22,551.5 | 28.768 | 86.30 | 2.88 | 1.28 |
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Doan, L.; Nguyen, T.M.D.; Le, T.M.; Huynh, K.G.; Quach, T.P.T. Surface Modifications of Superparamagnetic Iron Oxide Nanoparticles with Polyvinyl Alcohol, Chitosan, and Activated Carbon or Graphite as Methylene Blue Adsorbents—Comparative Study. Coatings 2023, 13, 1797. https://doi.org/10.3390/coatings13101797
Doan L, Nguyen TMD, Le TM, Huynh KG, Quach TPT. Surface Modifications of Superparamagnetic Iron Oxide Nanoparticles with Polyvinyl Alcohol, Chitosan, and Activated Carbon or Graphite as Methylene Blue Adsorbents—Comparative Study. Coatings. 2023; 13(10):1797. https://doi.org/10.3390/coatings13101797
Chicago/Turabian StyleDoan, Linh, Tu M. D. Nguyen, Tan M. Le, Khanh G. Huynh, and Tran P. T. Quach. 2023. "Surface Modifications of Superparamagnetic Iron Oxide Nanoparticles with Polyvinyl Alcohol, Chitosan, and Activated Carbon or Graphite as Methylene Blue Adsorbents—Comparative Study" Coatings 13, no. 10: 1797. https://doi.org/10.3390/coatings13101797