In Situ Modification of Activated Carbons by Oleic Acid under Microwave Heating to Improve Adsorptive Removal of Naphthalene in Aqueous Solutions
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials
2.2. Preparation of Starch-Based Carbon (SC), Starch-Based Activated Carbon (SAC), Pulverized Coal (PC), and Pulverized Coal-Based Activated Carbon (PCAC)
2.3. One-Pot Preparation of Activated Carbons (ACs) by Simultaneous Oleic Acid (OA) Modification and KOH Activation
2.4. Modification of Materials with OA in n-Hexane
2.5. Characterization
2.6. Adsorption Experimental Studies
2.6.1. Batch Adsorption
2.6.2. Column Adsorption
2.7. Data Analysis
3. Results
3.1. Characterization of Materials
3.2. Batch Adsorption
3.2.1. Adsorption Kinetics
3.2.2. Adsorption Isotherms
3.2.3. Adsorption Mechanism
3.2.4. Regeneration of In Situ Modified Activated Carbons (IMACs)
3.3. Column Adsorption
3.3.1. Effect of Column Height
3.3.2. Effect of Flow Rate
3.3.3. Effect of Initial NAP Concentration
3.3.4. Breakthrough Analysis
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
Nomenclature
Abbreviations | |
AC | activated carbon |
ABET | BET specific surface area |
AMicro | micropore specific surface area |
AE | external specific surface area |
APS | average pore size |
BTF | banana trunk fibers |
BET | Brunauer-Emmett-Teller |
BJH | Barrett-Joyner-Halenda |
EDAX | Energy Dispersive X-ray Analysis |
FT-IR | Fourier Transmission InfraRed spectroscopy |
IMACs | in situ modified ACs |
NAP | naphthalene |
OA | Oleic acid |
OBTF | OA modified BTF |
OMC | ordered mesoporous carbon |
O-PCAC1 | in situ modified PCAC |
O-PCAC2 | conventional- modified PCAC with OA |
O-SAC1 | in situ modified SAC |
O-SAC2 | conventional- modified SAC with OA |
PC | pulverized coal |
PCAC | pulverized coal-based ACs |
PFO | pseudo-first-order |
PSO | pseudo-second-order |
RL | reflection loss |
RMSE | Root mean square error |
SAC | Starch-based AC |
SC | starch-based carbon |
SEM | Scanning Electron Microscopy |
VMeso | mesopore volume |
VMicro | micropore volume |
VTotol | total pore volume |
XPS | X-ray photoelectron spectroscopy |
Symbols | |
Ac | the area under the breakthrough curve |
C | a constant related to the boundary layer thickness |
C0 | initial/inlet NAP concentration |
Ce | equilibrium NAP concentration |
Ct | the outlet NAP concentration |
C0-Ct | the adsorbed NAP concentration |
H | column height |
K1 | pseudo-first-order rate constant |
K2 | pseudo-second-order rate constant |
kAB | the kinetic constant |
Kbf | liquid-film diffusion constant |
KF | a constant related to the bonding energy |
KL | a constant related to the free energy |
KP | the intraparticle diffusion constant |
KPi | the calculated diffusion rate parameter at different stages |
kTh | the Thomas rate constant |
m | the mass of adsorbents used |
N0 | the saturation concentration |
Q | the flow rate |
Q0 | low rate |
q0 | the adsorption capacity |
qe | the equilibrium adsorption capacity |
qEq | the amount of NAP adsorbed per unit dry weight |
qm | the maximal adsorption capacity |
qtotal | the maximum column capacity |
R2 | correlation coefficients |
T | the temperature of adsorption system |
te | the exhaustion time |
tb | breakthrough time |
ttotal | the total flow time |
V | the volume of the NAP solution |
W | the total amount of IMACs in the column |
α | initial sorption constant |
β | initial desorption constant |
v | the feed flow rate |
U0 | the superficial velocity |
z | the bed depth of the fixed bed column |
1/n | a constant related to adsorption intensity |
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Samples | ABET m2/g | AMicro m2/g | AE m2/g | VTotol cm3/g | VMicro cm3/g | VMeso cm3/g | APS nm | Ref. |
---|---|---|---|---|---|---|---|---|
SC | 8.90 | – | 8.53 | 0.006 | – | – | 2.62 | [19] |
SAC | 616.80 | 522.65 | 94.18 | 0.327 | 0.255 | – | 2.12 | [19] |
O-SAC1 | 912.89 | 481.16 | 431.73 | 0.588 | 0.232 | 0.356 | 2.58 | This study |
O-SAC2 | 284.25 | – | 284.25 | 0.298 | 0.280 | 0.018 | 4.80 | This study |
PC | 4.19 | 1.46 | 2.73 | 0.014 | 0.001 | 0.013 | 12.97 | This study |
PCAC | 401.70 | 337.30 | 64.40 | 0.210 | 0.160 | – | 2.34 | [19] |
O-PCAC1 | 725.00 | 435.34 | 289.66 | 0.484 | 0.214 | 0.270 | 2.67 | This study |
O-PCAC2 | 30.58 | 25.03 | 5.55 | 0.020 | 0.007 | 0.013 | 2.67 | This study |
Component Assignment Binding Energy (eV) | Peak I | Peak II | Peak III | Peak IV | |
---|---|---|---|---|---|
C=O | C–O | R–O*–C=O | O*=C–OH | ||
531.2 | 532.4 | 533.3 | 534.3 | ||
Concentration (%) | SC | 14.7 | 26.7 | 30.4 | 28.2 |
SAC | 21.0 | 22.7 | 26.0 | 30.4 | |
O-SAC1 | 29.6 | 30.0 | 28.0 | 12.3 | |
O-SAC2 | 31.1 | 29.7 | 29.1 | 10.0 | |
PC | 9.3 | 43.3 | 18.3 | 29.0 | |
PCAC | 21.4 | 52.4 | 17.5 | 8.7 | |
O-PCAC1 | 27.5 | 25.5 | 26.1 | 20.9 | |
O-PCAC2 | 18.4 | 29.7 | 15.5 | 36.5 |
Samples | N% | C% | H% | S% | O,diff% | N/C | H/C | O/C | [O+N]/C |
---|---|---|---|---|---|---|---|---|---|
SC | 0.02 | 62.98 | 6.78 | 0.40 | 29.82 | 0.000 | 0.108 | 0.474 | 0.480 |
SAC | 0.07 | 67.84 | 4.68 | 0.26 | 27.15 | 0.010 | 0.069 | 0.400 | 0.405 |
O-SAC1 | 0.53 | 57.78 | 1.85 | 0.73 | 39.11 | 0.009 | 0.032 | 0.677 | 0.686 |
O-SAC2 | 0.09 | 56.85 | 1.40 | 0.32 | 41.34 | 0.002 | 0.025 | 0.727 | 0.729 |
PC | 0.65 | 68.33 | 0.48 | 0.34 | 30.20 | 0.010 | 0.007 | 0.442 | 0.451 |
PCAC | 0.21 | 67.10 | 3.81 | 0.23 | 28.65 | 0.003 | 0.057 | 0.427 | 0.433 |
O-PCAC1 | 0.60 | 76.81 | 1.74 | 0.65 | 20.21 | 0.008 | 0.023 | 0.263 | 0.271 |
O-PCAC2 | 0.57 | 57.61 | 1.03 | 1.22 | 39.59 | 0.010 | 0.018 | 0.687 | 0.697 |
Models | Parameter | O-SAC1 | O-PCAC1 |
---|---|---|---|
C0 (mg/L) | 30 | 30 | |
qexp (mg/g) | 180.8 | 187.8 | |
PFO | qe, cal (mg/g) | 70.93 | 62.87 |
K1 (1/min) | 0.0756 | 0.1156 | |
R2 | 0.8688 | 0.8911 | |
RMSE | 11.9 | 13.0 | |
PSO | qe, cal (mg/g) | 181.82 | 188.68 |
K2 (g/mg min) | 0.0047 | 0.0091 | |
R2 | 0.9988 | 0.9999 | |
RMSE | 3.6 | 3.9 | |
Elovich | qe, cal (mg/g) | 184.46 | 196.94 |
(1/β)ln(αβ) (mg/g) | 124.18 | 137.44 | |
1/β | 13.7570 | 13.5780 | |
R2 | 0.9870 | 0.9508 | |
RMSE | 16.1 | 15.4 |
Adsorbents | C0 (mg/L) | T (K) | qe (mg/g) | Ref. |
---|---|---|---|---|
Modified walnut shells | 25 | 298 | 7.20 | [15] |
Modified coal-based AC | 30 | 298 | 131.20 | [21] |
Modified zeolite | 1 | 303 | 0.30 | [31] |
ZnS-NPs-AC | 50 | 298 | 142.70 | [35] |
Modified hazelnut shell | 25 | 298 | 17.30 | [36] |
SC | 30 | 303 | 52.9 | [19] |
SAC | 30 | 303 | 158.9 | [19] |
PC | 30 | 303 | 75.26 | This study |
PCAC | 30 | 303 | 160.7 | [19] |
O-SAC1 | 30 | 303 | 180. 8 | This study |
O-PCAC1 | 30 | 303 | 187.8 | This study |
O-SAC2 * | 30 | 303 | 116.2 | This study |
O-PCAC2 * | 30 | 303 | 120.5 | This study |
Models | Parameters | O-SAC1 | O-PCAC1 |
---|---|---|---|
Langmuir | qmax (mg/g) | 270.27 | 333.33 |
KL (L/mg) | 0.5873 | 0.6122 | |
R2 | 0.9889 | 0.9820 | |
RMSE | 9.7 | 9.6 | |
Freundlich | KF (L/mg) | 103.52 | 123.48 |
1/n | 0.3433 | 0.4156 | |
R2 | 0.9934 | 0.9926 | |
RMSE | 2.9 | 2.1 |
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Wu, Z.; Liu, P.; Wu, Z.; Cravotto, G. In Situ Modification of Activated Carbons by Oleic Acid under Microwave Heating to Improve Adsorptive Removal of Naphthalene in Aqueous Solutions. Processes 2021, 9, 391. https://doi.org/10.3390/pr9020391
Wu Z, Liu P, Wu Z, Cravotto G. In Situ Modification of Activated Carbons by Oleic Acid under Microwave Heating to Improve Adsorptive Removal of Naphthalene in Aqueous Solutions. Processes. 2021; 9(2):391. https://doi.org/10.3390/pr9020391
Chicago/Turabian StyleWu, Zhansheng, Pengyun Liu, Zhilin Wu, and Giancarlo Cravotto. 2021. "In Situ Modification of Activated Carbons by Oleic Acid under Microwave Heating to Improve Adsorptive Removal of Naphthalene in Aqueous Solutions" Processes 9, no. 2: 391. https://doi.org/10.3390/pr9020391