Synthesis of Zeolites from Greek Fly Ash and Assessment of Their Copper Removal Capacity
Abstract
:1. Introduction
2. Materials and Methods
2.1. Raw Materials and Reagents
2.2. Synthesis of Zeolites
2.3. Kinetic Studies
2.4. Analytical Techniques
3. Results and Discussion
3.1. Raw Material and Zeolite Characterization
3.2. Screening of Na and K Zeolites in Terms of Removal Efficiency
3.3. Kinetic Studies
3.3.1. Effect of Initial Cu(II) Concentration
3.3.2. Effect of Zeolite Dosage
3.3.3. Evaluation of Kinetic Models
3.4. Morphology and Composition Analysis of Zeolites
3.5. Copper Chemical State by XPS Analysis
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Oxide | (wt %) | Oxide | (wt %) |
---|---|---|---|
SiO2 | 40.4 | MnO | 0.08 |
CaO | 16.4 | P2O5 | 0.6 |
Al2O3 | 16.4 | TiO2 | 1.0 |
Fe2O3 | 9.5 | SO3 | 3.4 |
MgO | 3.2 | Cr2O3 | 0.04 |
K2O | 1.8 | a LOI | 3.9 |
Na2O | 3.3 | Total | 100.02 |
Zeolite Code | Particle Size (μm) | Specific Surface Area (m2·g–1) | |
---|---|---|---|
Size | d50 | ||
ZFA1Na | <191 | 11.5 | 15.7 |
ZFA1.5Na | <118 | 17.4 | 14.8 |
ZFA1K | <132 | 11.3 | 21.9 |
ZFA1.5K | <223 | 20.9 | 21.5 |
a NZ | b Experimental | Pseudo-First-Order | Pseudo-Second-Order | Intraparticle Diffusion | ||||||
---|---|---|---|---|---|---|---|---|---|---|
qe,exp | qe,cal | k1 | R2 | qe,cal | k2 | R2 | kp | C | R2 | |
mg·g−1 | mg·g−1 | min−1 | mg·g−1 | g·mg−1·min−1 | mg·g−1·min−0.5 | mg·g−1 | ||||
Z1 | 93.49 | 10.72 | 0.260 | 0.721 | 93.54 | 0.3516 | 1.000 | 92.34 | 0.81 | 0.625 |
196.41 | 158.74 | 0.160 | 0.905 | 201.21 | 0.0034 | 0.997 | 93.30 | 21.12 | 0.936 | |
258.69 | 204.87 | 0.117 | 0.930 | 265.96 | 0.0017 | 0.995 | 136.20 | 21.63 | 0.990 | |
309.70 | 202.44 | 0.075 | 0.878 | 318.47 | 0.0011 | 0.994 | 145.95 | 26.33 | 0.951 | |
Z1.5 | 90.08 | 31.43 | 0.260 | 0.918 | 90.33 | 0.0756 | 0.999 | 3.91 | 75.38 | 0.698 |
176.54 | 95.52 | 0.201 | 0.929 | 177.94 | 0.0122 | 0.999 | 10.14 | 131.5 | 0.975 | |
290.79 | 255.81 | 0.108 | 0.946 | 302.11 | 0.0011 | 0.991 | 23.75 | 132.7 | 0.838 | |
294.01 | 206.82 | 0.089 | 0.847 | 305.81 | 0.0011 | 0.991 | 29.03 | 135.9 | 0.722 |
Materials Used for Copper Removal | Cu(II) Concentration | pH | T | Time | Dosage | Removal Capacity | Removal Degree | Reference |
---|---|---|---|---|---|---|---|---|
mg·L−1 | °C | h | g·L−1 | mg·g−1 | % | |||
Natural zeolite (clinoptilolite) | 20 | 3.5 | 22 | 6 | 37 | 0.54 | 98 | [58] |
Zeolite A | 200 | 3 | 25 | 4 | 5 | 38 | [42] | |
Zeolite X | 200 | 3 | 25 | 4 | 5 | 29 | ||
Zeolite 4A (from coal fly ash) | 100 | 3–4 | 25 | 4 | 1 | 20–70 | 20–80 | [31] |
Pistachio shell biochar | 150 | 7.15 * | 25 | 24 | 10 | 9.5 | 63 | [59] |
ZFA1Na | 200 | 5.5 | 25 | 1 | 0.5 | 310 | 80 | Present study |
Sample No. | |||
---|---|---|---|
a ZFA1Na | ZFA1Na_Cu | ||
Surface analysis (XPS) | |||
Cu2p3/2 | b Eb (eV) | n.a. | 934.3 |
c At (%) | n.a. | 26.8 ± 0.3 | |
Si2p | Eb (eV) | 102.2 | 102.0 |
At (%) | 19.6 ± 0.3 | 20.6 ± 0.3 | |
Al2p | Eb (eV) | 73.9 | 73.7 |
At (%) | 13.8 ± 0.5 | 20.1 ± 0.7 | |
Na1s | Eb (eV) | 1072.2 | 1072.5 |
At (%) | 61.0 ± 0.3 | 19.2 ± 0.3 | |
Cl2p | Eb (eV) | 198.2 | 198.2 |
At (%) | 5.5 ± 0.01 | 13.1 ± 0.3 | |
Cu/Si | n.a. | 1.3 | |
Si/Al | 1.4 | 1.0 | |
Na/Si | 3.1 | 0.9 | |
Cl/Si | 0.3 | 0.6 | |
Bulk analysis (SEM/EDS) | |||
Cu/Si | n.a. | 1.5 | |
Si/Al | 1.8 | 1.3 |
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Vavouraki, A.; Bartzas, G.; Komnitsas, K. Synthesis of Zeolites from Greek Fly Ash and Assessment of Their Copper Removal Capacity. Minerals 2020, 10, 844. https://0-doi-org.brum.beds.ac.uk/10.3390/min10100844
Vavouraki A, Bartzas G, Komnitsas K. Synthesis of Zeolites from Greek Fly Ash and Assessment of Their Copper Removal Capacity. Minerals. 2020; 10(10):844. https://0-doi-org.brum.beds.ac.uk/10.3390/min10100844
Chicago/Turabian StyleVavouraki, Aikaterini, Georgios Bartzas, and Konstantinos Komnitsas. 2020. "Synthesis of Zeolites from Greek Fly Ash and Assessment of Their Copper Removal Capacity" Minerals 10, no. 10: 844. https://0-doi-org.brum.beds.ac.uk/10.3390/min10100844