Kinetic Modelling of the Removal of Multiple Heavy Metallic Ions from Mine Waste by Natural Zeolite Sorption
Abstract
:1. Introduction
2. Materials and Methods
2.1. Zeolite Sample Material
2.2. Kinetic Experimental Procedure
- single-component system—10 meq/L per metal,(lead [P], copper [C], iron [F], nickel [N], zinc [Z]);
- dual-component system [D]—5.0 meq/L per metal(lead-copper [D-PC], lead-iron [D-PF], lead-nickel [D-PN], lead-zinc [D-PZ],copper-iron [D-CF], copper-nickel [D-CN], iron-zinc [D-FZ], nickel-zinc [D-NZ]);
- triple-component system [T]—3.3 meq/L per metal (lead-copper-iron), and;
- multi-component system [M]—2.0 meq/L per metal (all five metals).
2.3. Analytical Procedure
2.4. Sorption Kinetics Principles and Model Selection
- Reaction-Type ModelChemisorption—chemical reaction at the sites of the functional ionic groups within the zeolite and focuses on the process as a whole.
- Diffusion-Type Model
- Film Diffusion—diffusion of counterions in the adherent layer surrounding the zeolite (between the external solution and crystal surface).
- Intra-Particle Diffusion—diffusion of counterions in the solute within the zeolite pores and/or along the pore walls.
- Mass Action—sorption or desorption between the active sites and the sorbate material.
2.4.1. Reaction-Type Models
Pseudo-First-Order Rate Equation
Pseudo-Second-Order Rate Equation
Elovich’s Equation
2.4.2. Diffusion-Type Models
3. Results and Discussion
3.1. Acidity Levels
3.2. Heavy Metallic Ion Levels
3.3. Sorption Kinetics
4. Conclusions
Acknowledgments
Author Contributions
Conflicts of Interest
References
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1 | 2 | 3 | 4 | 5 | 6 | 7 |
---|---|---|---|---|---|---|
Analyte | Sample ID | %RSD | Concentration (mg/L) | meq/g | %R | |
Triplicate Mean (Calib) | DIL | |||||
Pb | [P]-S4 | 0.24 | 75.93 | 1214.81 | 0.1919 | 76.8 |
220.353 | [P]1803 | 0.59 | 35.20 | 281.63 | ||
Cu | [C]-S2 | 0.40 | 105.37 | 421.49 | 0.0533 | 21.4 |
327.393 | [C]1802 | 0.16 | 82.84 | 331.37 | ||
Fe | [F]-S1 | 0.53 | 105.83 | 211.65 | 0.0757 | 30.3 |
238.204 | [F]1801 | 0.55 | 73.73 | 147.46 | ||
Ni | [N]-S2 | 0.32 | 87.30 | 349.19 | 0.0268 | 10.7 |
231.604 | [N]1802 | 0.36 | 77.92 | 311.69 | ||
Zn | [Z]-S2 | 1.10 | 104.67 | 418.68 | 0.0494 | 19.8 |
206.200 | [Z]1802 | 0.74 | 83.94 | 335.77 |
1 | 2 | 3 | 4 | 5 | 6 | 7 | 1 | 2 | 3 | 4 | 5 | 6 | 7 |
---|---|---|---|---|---|---|---|---|---|---|---|---|---|
Analyte | Sample ID | %RSD | Concentration (mg/L) | meq/g | %R | Analyte | Sample ID | %RSD | Concentration (mg/L) | meq/g | %R | ||
Triplicate Mean (Calib) | DIL | Triplicate Mean (Calib) | DIL | ||||||||||
Pb | [D-PC]-S3 | 0.13 | 75.47 | 603.79 | 0.1102 | 88.3 | Cu | [D-CF]-S1 | 0.90 | 95.76 | 191.51 | 0.0283 | 22.7 |
220.353 | [D-PC]1802 | 0.59 | 17.68 | 70.73 | 327.393 | [D-CF]1801 | 0.58 | 74.06 | 148.13 | ||||
Cu | [D-PC]-S3 | 0.11 | 24.18 | 193.44 | 0.0153 | 12.2 | Fe | [D-CF]-S1 | 2.75 | 50.61 | 101.21 | 0.0534 | 42.8 |
327.393 | [D-PC]1802 | 0.61 | 42.44 | 169.77 | 238.204 | [D-CF]1801 | 0.70 | 28.95 | 57.90 | ||||
Pb | [D-PF]-S3 | 0.42 | 75.98 | 607.82 | 0.0992 | 79.5 | Cu | [D-CN]-S1 | 0.50 | 94.92 | 189.85 | 0.0361 | 28.9 |
220.353 | [D-PF]1802 | 0.54 | 31.19 | 124.77 | 327.393 | [D-CN]1801 | 0.40 | 67.46 | 134.92 | ||||
Fe | [D-PF]-S3 | 0.31 | 13.01 | 104.11 | 0.0471 | 37.7 | Ni | [D-CN]-S1 | 0.23 | 80.53 | 161.06 | 0.0125 | 10.0 |
238.204 | [D-PF]1802 | 0.45 | 16.21 | 64.82 | 231.604 | [D-CN]1801 | 0.48 | 72.48 | 144.96 | ||||
Pb | [D-PN]-S3 | 0.82 | 77.16 | 617.29 | 0.1112 | 89.1 | Fe | [D-FZ]-S1 | 2.31 | 51.15 | 102.30 | 0.0546 | 43.7 |
220.353 | [D-PN]1802 | 0.68 | 16.81 | 67.22 | 238.204 | [D-FZ]1801 | 0.20 | 28.78 | 57.56 | ||||
Ni | [D-PN]-S3 | 0.86 | 21.05 | 168.37 | 0.0092 | 7.40 | Zn | [D-FZ]-S1 | 2.69 | 90.55 | 181.09 | 0.0236 | 18.9 |
231.604 | [D-PN]1802 | 0.12 | 38.99 | 155.94 | 206.200 | [D-FZ]1801 | 0.22 | 73.43 | 146.85 | ||||
Pb | [D-PZ]-S3 | 1.01 | 76.78 | 614.22 | 0.1105 | 88.5 | Ni | [D-NZ]-S1 | 1.22 | 80.15 | 160.31 | 0.0067 | 5.4 |
220.353 | [D-PZ]1802 | 0.50 | 17.68 | 70.72 | 231.604 | [D-NZ]1801 | 3.49 | 75.85 | 151.71 | ||||
Zn | [D-PZ]-S3 | 0.92 | 23.46 | 187.65 | 0.0138 | 11.0 | Zn | [D-NZ]-S1 | 1.30 | 89.51 | 179.02 | 0.0244 | 19.6 |
206.200 | [D-PZ]1802 | 0.83 | 41.75 | 166.98 | 206.200 | [D-NZ]1801 | 3.84 | 71.99 | 143.99 |
1 | 2 | 3 | 4 | 5 | 6 | 7 |
---|---|---|---|---|---|---|
Analyte | Sample ID | %RSD | Concentration (mg/L) | meq/g | %R | |
Triplicate Mean (Calib) | DIL | |||||
Pb | [T]-S2 | 1.27 | 100.05 | 400.21 | 0.0750 | 90.2 |
220.353 | [T]1801 | 0.21 | 19.66 | 39.32 | ||
Cu | [T]-S2 | 1.16 | 33.76 | 135.03 | 0.0158 | 19.0 |
327.393 | [T]1801 | 1.58 | 54.70 | 109.40 | ||
Fe | [T]-S2 | 0.59 | 17.23 | 68.92 | 0.0412 | 49.5 |
238.204 | [T]1801 | 1.81 | 17.40 | 34.80 | ||
Pb | [M]-S1 | 0.53 | 117.76 | 235.52 | 0.0469 | 94.0 |
220.353 | [M]1800 | 0.67 | 14.20 | 14.20 | ||
Cu | [M]-S1 | 1.96 | 37.58 | 75.16 | 0.0109 | 21.9 |
327.393 | [M]1800 | 0.99 | 58.74 | 58.74 | ||
Fe | [M]-S1 | 2.26 | 20.52 | 41.03 | 0.0281 | 56.2 |
238.204 | [M]1800 | 1.24 | 17.97 | 17.97 | ||
Ni | [M]-S1 | 0.56 | 32.87 | 65.75 | 0.0045 | 9.10 |
231.604 | [M]1800 | 1.48 | 59.76 | 59.76 | ||
Zn | [M]-S1 | 2.23 | 35.99 | 71.98 | 0.0082 | 16.5 |
206.200 | [M]1800 | 1.63 | 60.12 | 60.12 |
SYSTEM | CC | Equilibrium Sorption | Sorption Rate Constant | Initial Sorption Rate | ||
---|---|---|---|---|---|---|
(meq/g) | (g/meq·min) | (meq/g·min) | ||||
[P] | 4.098 | 217.01 | 0.9926 | 0.244 | 0.077 | 0.0046 |
[C] | 15.750 | 836.09 | 0.9291 | 0.063 | 0.297 | 0.0012 |
[F] | 11.872 | 419.08 | 0.9708 | 0.084 | 0.336 | 0.0024 |
[N] | 34.919 | 739.14 | 0.9806 | 0.029 | 1.650 | 0.0014 |
[Z] | 15.237 | 1106,10 | 0.9147 | 0.066 | 0.210 | 0.0009 |
[D-PC]-Pb | 7.474 | 299.43 | 0.9941 | 0.134 | 0.187 | 0.0033 |
[D-PC]-Cu | 55.217 | 2840,90 | 0.9282 | 0.018 | 1.073 | 0.0004 |
[D-PC] | 6.596 | 269.78 | 0.9906 | 0.152 | 0.161 | 0.0037 |
[D-PF]-Pb | 7.692 | 448.41 | 0.9904 | 0.130 | 0.132 | 0.0022 |
[D-PF]-Fe | 18.375 | 727.45 | 0.9703 | 0.054 | 0.464 | 0.0014 |
[D-PF] | 5.489 | 275.71 | 0.9837 | 0.182 | 0.109 | 0.0036 |
[D-PN]-Pb | 7.465 | 284.48 | 0.9957 | 0.134 | 0.196 | 0.0035 |
[D-PN]-Ni | 109.750 | 3126,00 | 0.5378 | 0.009 | 3.853 | 0.0003 |
[D-PN] | 6.976 | 254.36 | 0.9914 | 0.143 | 0.191 | 0.0039 |
[D-PZ]-Pb | 7.436 | 293.22 | 0.9973 | 0.134 | 0.189 | 0.0034 |
[D-PZ]-Zn | 40.653 | 5898,50 | 0.4358 | 0.025 | 0.280 | 0.0002 |
[D-PZ] | 6.534 | 280.74 | 0.9946 | 0.153 | 0.152 | 0.0036 |
[D-CF]-Cu | 21.169 | 2683,00 | 0.9629 | 0.047 | 0.167 | 0.0004 |
[D-CF]-Fe | 16.655 | 581.48 | 0.9750 | 0.060 | 0.477 | 0.0017 |
[D-CF] | 10.297 | 488.73 | 0.9703 | 0.097 | 0.217 | 0.0020 |
[D-CN]-Cu | 21.936 | 1271,30 | 0.9453 | 0.046 | 0.379 | 0.0008 |
[D-CN]-Ni | 72.008 | 1686,80 | 0.9498 | 0.014 | 3.074 | 0.0006 |
[D-CN] | 17.329 | 747.04 | 0.9471 | 0.058 | 0.402 | 0.0013 |
[D-FZ]-Fe | 16.438 | 502.40 | 0.9778 | 0.061 | 0.538 | 0.0020 |
[D-FZ]-Zn | 28.869 | 3101,00 | 0.6387 | 0.035 | 0.269 | 0.0003 |
[D-FZ] | 11.140 | 451.04 | 0.9554 | 0.090 | 0.275 | 0.0022 |
[D-NZ]-Ni | 133.600 | 999.38 | 0.9731 | 0.007 | 17.860 | 0.0010 |
[D-NZ]-Zn | 19.459 | 3808,80 | 0.3642 | 0.051 | 0.099 | 0.0003 |
[D-NZ] | 24.852 | 1452,00 | 0.9113 | 0.040 | 0.425 | 0.0007 |
[T]-Pb | 11.194 | 394.10 | 0.9980 | 0.089 | 0.318 | 0.0025 |
[T]-Cu | 48.524 | 3252,90 | 0.9141 | 0.021 | 0.724 | 0.0003 |
[T]-Fe | 21.496 | 721.14 | 0.9807 | 0.047 | 0.641 | 0.0014 |
[T] | 6.438 | 237.29 | 0.9918 | 0.155 | 0.175 | 0.0042 |
[M]-Pb | 18.593 | 465.67 | 0.9990 | 0.054 | 0.742 | 0.0021 |
[M]-Cu | 58.274 | 6429,20 | 0.8600 | 0.017 | 0.528 | 0.0002 |
[M]-Fe | 31.695 | 989.38 | 0.9830 | 0.032 | 1.015 | 0.0010 |
[M]-Ni | 190.820 | 5086,10 | 0.9747 | 0.005 | 7.159 | 0.0002 |
[M]-Zn | −51.894 | 2,5482,00 | 0.1723 | -0.019 | 0.106 | 0.0000 |
[M] | 8.630 | 303.14 | 0.9931 | 0.116 | 0.246 | 0.0033 |
SYSTEM | Diffusion Rate Constant A | CCA | SYSTEM | Diffusion Rate Constant B | Boundary Constant B | CCB |
---|---|---|---|---|---|---|
(meq/g·min1/2) | (meq/g·min1/2) | (meq/g) | ||||
[P] | 0.015 | 0.9818 | [P] | 0.016 | −0.004 | 0.9828 |
[C] | 0.004 | 0.9882 | [C] | 0.004 | −0.000 | 0.9883 |
[F] | 0.006 | 0.9548 | [F] | 0.005 | 0.006 | 0.9747 |
[N] | 0.002 | 0.6930 | [N] | 0.002 | 0.007 | 0.9629 |
[Z] | 0.004 | 0.9729 | [Z] | 0.004 | −0.003 | 0.9846 |
[D-PC]-Pb | 0.009 | 0.9597 | [D-PC]-Pb | 0.009 | 0.004 | 0.9627 |
[D-PC]-Cu | 0.001 | 0.9658 | [D-PC]-Cu | 0.001 | 0.000 | 0.9669 |
[D-PC] | 0.010 | 0.9662 | [D-PC] | 0.010 | 0.004 | 0.9690 |
[D-PF]-Pb | 0.008 | 0.9790 | [D-PF]-Pb | 0.008 | −0.004 | 0.9827 |
[D-PF]-Fe | 0.004 | 0.9860 | [D-PF]-Fe | 0.003 | 0.003 | 0.9951 |
[D-PF] | 0.012 | 0.9873 | [D-PF] | 0.012 | −0.001 | 0.9876 |
[D-PN]-Pb | 0.009 | 0.9569 | [D-PN]-Pb | 0.009 | 0.005 | 0.9622 |
[D-PN]-Ni | 0.001 | 0.4479 | [D-PN]-Ni | 0.001 | 0.002 | 0.5521 |
[D-PN] | 0.010 | 0.9527 | [D-PN] | 0.009 | 0.007 | 0.9616 |
[D-PZ]-Pb | 0.009 | 0.9542 | [D-PZ]-Pb | 0.009 | 0.004 | 0.9576 |
[D-PZ]-Zn | 0.001 | 0.9088 | [D-PZ]-Zn | 0.001 | −0.002 | 0.9378 |
[D-PZ] | 0.010 | 0.9639 | [D-PZ] | 0.010 | 0.003 | 0.9649 |
[D-CF]-Cu | 0.002 | 0.9523 | [D-CF]-Cu | 0.002 | −0.004 | 0.9933 |
[D-CF]-Fe | 0.004 | 0.9666 | [D-CF]-Fe | 0.004 | 0.005 | 0.9902 |
[D-CF] | 0.006 | 0.9923 | [D-CF] | 0.006 | 0.001 | 0.9925 |
[D-CN]-Cu | 0.003 | 0.9888 | [D-CN]-Cu | 0.003 | −0.001 | 0.9915 |
[D-CN]-Ni | 0.001 | 0.6540 | [D-CN]-Ni | 0.001 | 0.003 | 0.9089 |
[D-CN] | 0.004 | 0.9795 | [D-CN] | 0.004 | 0.002 | 0.9843 |
[D-FZ]-Fe | 0.005 | 0.9332 | [D-FZ]-Fe | 0.004 | 0.007 | 0.9906 |
[D-FZ]-Zn | 0.002 | 0.9303 | [D-FZ]-Zn | 0.002 | −0.002 | 0.9494 |
[D-FZ] | 0.006 | 0.9777 | [D-FZ] | 0.006 | 0.005 | 0.9907 |
[D-NZ]-Ni | 0.001 | −0.2510 | [D-NZ]-Ni | 0.000 | 0.003 | 0.6264 |
[D-NZ]-Zn | 0.002 | 0.9348 | [D-NZ]-Zn | 0.002 | −0.004 | 0.9801 |
[D-NZ] | 0.002 | 0.9605 | [D-NZ] | 0.002 | −0.000 | 0.9605 |
[T]-Pb | 0.006 | 0.9434 | [T]-Pb | 0.006 | 0.005 | 0.9536 |
[T]-Cu | 0.001 | 0.9747 | [T]-Cu | 0.001 | −0.001 | 0.9826 |
[T]-Fe | 0.003 | 0.9622 | [T]-Fe | 0.003 | 0.004 | 0.9900 |
[T] | 0.011 | 0.9668 | [T] | 0.010 | 0.008 | 0.9761 |
[M]-Pb | 0.004 | 0.8584 | [M]-Pb | 0.004 | 0.007 | 0.9130 |
[M]-Cu | 0.001 | 0.9473 | [M]-Cu | 0.001 | −0.001 | 0.9851 |
[M]-Fe | 0.002 | 0.9465 | [M]-Fe | 0.002 | 0.003 | 0.9886 |
[M]-Ni | 0.000 | 0.8566 | [M]-Ni | 0.000 | 0.001 | 0.9251 |
[M]-Zn | 0.001 | 0.8479 | [M]-Zn | 0.001 | −0.002 | 0.9720 |
[M] | 0.008 | 0.9585 | [M] | 0.008 | 0.007 | 0.9713 |
SYSTEM | (meq/g) | % Achieved of at 3 h | OBSERVATION | |||||
---|---|---|---|---|---|---|---|---|
SINGLE HMI | [P] | 0.1919 | 0.2440 | 78.7 | Highest Single Uptake of 76.8% for [P] | |||
[C] | 0.0533 | 0.0635 | 84.0 | |||||
[F] | 0.0757 | 0.0842 | 89.8 | |||||
[N] | 0.0268 | 0.0286 | 93.5 | Lowest Single Uptake of 10.7% for [N] | ||||
[Z] | 0.0494 | 0.0656 | 75.3 | |||||
DUAL [D] | [PC] | 0.1255 | 0.1516 | 82.7 | ||||
[PF] | 0.1462 | 0.1822 | 80.3 | Highest [D] Uptake of 58.5% for [PF] | ||||
[PN] | 0.1204 | 0.1433 | 84.0 | |||||
[PZ] | 0.1243 | 0.1530 | 81.2 | |||||
[CF] | 0.0817 | 0.0971 | 84.1 | |||||
[CN] | 0.0486 | 0.0577 | 84.1 | |||||
[FZ] | 0.0782 | 0.0898 | 87.1 | |||||
[NZ] | 0.0311 | 0.0402 | 77.3 | Lowest [D] Uptake of 12.4% for [NZ] | ||||
TRIPLE [T] | 0.1320 | 0.1553 | 85.0 | [D-PC] | Increased | 5.2% | 2.5% | |
[D-PF] | Decreased | 9.8% | 14.7% | |||||
[D-CF] | Increased | 61.5% | 59.9% | |||||
MULTI [M] | 0.0986 | 0.1159 | 85.1 | [D-PC] | Decreased | 21.4% | 23.6% | |
[D-PF] | Decreased | 32.6% | 36.4% | |||||
[D-CF] | Increased | 20.7% | 19.3% | |||||
[T] | Decreased | 25.3% | 25.4% | |||||
Sorbent Material | HMI | Sorption Trends | Reference | |
---|---|---|---|---|
American 85–95% Clinoptilolite | (meq/g) | This Study | ||
Pb2+ | 0.1919 | 0.2440 | ||
Fe3+ | 0.0757 | 0.0842 | ||
Cu2+ | 0.0533 | 0.0635 | ||
Zn2+ | 0.0494 | 0.0656 | ||
Ni2+ | 0.0268 | 0.0286 | ||
Pb2+ >> Fe3+Cu2+ > Zn2+ > Ni2+ | ||||
Brazilian Zeolite (Scolecite) | Cu2+ | 130 μeq/g | Bosso and Enzweiler (2002) [47] | |
Zn2+ | 64 μeq/g | |||
Pb2+ | 56 μeq/g | |||
Ni2+ | 31 μeq/g | |||
Co2+ | 7.8 μeq/g | |||
Cd2+ | 3.2 μeq/g | |||
Cu2+ >> Zn2+ > Pb2+ > Ni2+ > Co2+ > Cd2+ | ||||
Turkish 70% Clinoptilolite | Co2+ | 77.96% (0.448 meq/g) | Erdem et al. (2004) [2] Wang and Peng (2010) [18] | |
Cu2+ | 66.10% (0.282 meq/g) | |||
Zn2+ | 45.96% (0.268 meq/g) | |||
Mn2+ | 19.84% (0.153 meq/g) | |||
Co2+ > Cu2+ > Zn2+ > Mn2+ | ||||
Ukrainian 75% Clinoptilolite | Pb2+ | 27.7 mg/g | Sprynskyy et al. (2006) [4] | |
Cu2+ | 25.76 mg/g | |||
Ni2+ | 13.03 mg/g | |||
Cd2+ | 4.22 mg/g | |||
Pb2+ > Cu2+ > Cd2 > Ni2+ | ||||
Sardinian 40–70% Clinoptilolite | Pb2+ | 0.34 meq/g | Cincotti et al. (2006) [48] | |
Cu2+ | 0.27–1.2 meq/g | |||
Zn2+ | 0.1 meq/g | |||
Cd2+ | 0.05-0.19 meq/g | |||
Pb2+ > Cu2+ > Cd2+ ≅ Zn2+ | ||||
Turkish Zeolite(Clinoptilolite and Heulandite) | Single- | Multi- | Oter and Akcay (2007) [27] Wang and Peng (2010) [18] | |
Pb2+ | 0.730 meq/g | 0.299 meq/g | ||
Zn2+ | 0.251 meq/g | 0.108 meq/g | ||
Cu2+ | 0.227 meq/g | 0.022 meq/g | ||
Ni2+ | 0.173 meq/g | 0.017 meq/g | ||
Pb2+ > Zn2+ > Cu2+ > Ni2+ | ||||
Turkish Clinoptilolite | Fe3+ | 6.41 mg/g | Motsi et al. (2009) [38] | |
Zn2+ | 1.60 mg/g | |||
Cu2+ | 0.44 mg/g | |||
Mn2+ | 0.37 mg/g | |||
Fe3+ > Zn2+ > Cu2+ > Mn2+ | ||||
Brine Sediments | Zn2+ | 4.85 mg/g | Fu and Wang (2011) [19] | |
Cu2+ | 2.58 mg/g | |||
Sawdust Materials | Zn2+ | 4.69 mg/g | ||
Cu2+ | 2.31 mg/g | |||
Dried Marine Green Macroalga Algal Biomass | Cu2+ | 1.46 mmol/g | ||
Zn2+ | 1.97 mmol/g | |||
Rhizopus Oryzae Fungi Biomass | Cu2+ | 19.4 mg/g (Natural) | ||
43.7 mg/g (NaOH-treated) |
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Ciosek, A.L.; Luk, G.K. Kinetic Modelling of the Removal of Multiple Heavy Metallic Ions from Mine Waste by Natural Zeolite Sorption. Water 2017, 9, 482. https://doi.org/10.3390/w9070482
Ciosek AL, Luk GK. Kinetic Modelling of the Removal of Multiple Heavy Metallic Ions from Mine Waste by Natural Zeolite Sorption. Water. 2017; 9(7):482. https://doi.org/10.3390/w9070482
Chicago/Turabian StyleCiosek, Amanda L., and Grace K. Luk. 2017. "Kinetic Modelling of the Removal of Multiple Heavy Metallic Ions from Mine Waste by Natural Zeolite Sorption" Water 9, no. 7: 482. https://doi.org/10.3390/w9070482