J. Mater. Sci. Technol. ›› 2022, Vol. 103: 15-28.DOI: 10.1016/j.jmst.2021.07.012
• Research Article • Previous Articles Next Articles
Qiyun Zhanga, Renquan Wub, Yunhong Zhoub, Qilang Linb,*(
), Changqing Fangc
Received:2021-02-10
Revised:2021-06-12
Accepted:2021-07-05
Published:2022-03-20
Online:2021-09-15
Contact:
Qilang Lin
About author:* College of Materials Science and Engineering, Fuzhou University, Fuzhou 350116, China. E-mail address: linqilang@fzu.edu.cn (Q. Lin).Qiyun Zhang, Renquan Wu, Yunhong Zhou, Qilang Lin, Changqing Fang. A novel surface-oxidized rigid carbon foam with hierarchical macro-nanoporous structure for efficient removal of malachite green and lead ion[J]. J. Mater. Sci. Technol., 2022, 103: 15-28.
Fig. 1. (a) The typical FESEM images of the ORCF, the surfaces (b-d) and fractures (e-h) of pore walls of the ORCF with different magnifications.
Fig. 2. (a) TEM, (b, c) HRTEM images of the ORCF, and (d) its SAED pattern. (e) Schematic illustration of the formation process of the ORCF.
Fig. 3. FESEM images of the surface of the CF-TLC (a, b), the ARCF (c, d) and the ORCF (e, f).
Fig. 4. (a) Digital pictures of the CF-TLC, the ARCF and the ORCF; and (b) their stress-strain compression curves.
| Samples | Bulk density (g cm-3) | Open cell (%) | Porosity (%) | Compressive strength (MPa) |
|---|---|---|---|---|
| ORCF | 0.09 | 98.9 | 95.7 | 0.74 |
| ARCF | 0.10 | 98.6 | 95.4 | 0.93 |
| CF-TLC | 0.11 | 91.8 | 94.2 | 1.72 |
Table 1 Physical characteristics of the ORCF, ARCF and CF-TLC.
| Samples | Bulk density (g cm-3) | Open cell (%) | Porosity (%) | Compressive strength (MPa) |
|---|---|---|---|---|
| ORCF | 0.09 | 98.9 | 95.7 | 0.74 |
| ARCF | 0.10 | 98.6 | 95.4 | 0.93 |
| CF-TLC | 0.11 | 91.8 | 94.2 | 1.72 |
Fig. 5. (a, b) Nitrogen adsorption-desorption isotherms and pore size distributions of the ARCF and the ORCF; (c) FT-IR spectra of the ARCF and the ORCF.
| Sample | SBETa (m2 g-1) | SMicrob (m2 g-1) | SExterc (m2 g-1) | VTotald (cm3 g-1) |
|---|---|---|---|---|
| ORCF | 66.16 | 41.64 | 24.52 | 0.0899 |
| ARCF | 37.43 | 14.72 | 22.71 | 0.0534 |
| CF-TLC | 19.60 | 10.76 | 8.84 | 0.0396 |
Table 2. Textural characteristics of the ORCF, ARCF, and CF-TLC.
| Sample | SBETa (m2 g-1) | SMicrob (m2 g-1) | SExterc (m2 g-1) | VTotald (cm3 g-1) |
|---|---|---|---|---|
| ORCF | 66.16 | 41.64 | 24.52 | 0.0899 |
| ARCF | 37.43 | 14.72 | 22.71 | 0.0534 |
| CF-TLC | 19.60 | 10.76 | 8.84 | 0.0396 |
Fig. 6. XPS survey spectra and high-resolution XPS scan spectra of the ARCF (a, c, and e) and the ORCF (b, d, and f).
| Sample | C 1s | O 1s | Element | ||||||
|---|---|---|---|---|---|---|---|---|---|
| %C-C | %C-O | %C=O | %O-H | %C-O (aromatic) | %C-O (aliphatic) | %C=O | %C | %O | |
| ARCF | 79.55 | 20.45 | - | 23.63 | 45.17 | 31.2 | - | 93.79 | 6.21 |
| ORCF | 64.94 | 32.87 | 2.19 | 14.83 | 25.64 | 50.53 | 9.00 | 82.15 | 17.85 |
Table 3. XPS elemental analysis of the sample obtained.
| Sample | C 1s | O 1s | Element | ||||||
|---|---|---|---|---|---|---|---|---|---|
| %C-C | %C-O | %C=O | %O-H | %C-O (aromatic) | %C-O (aliphatic) | %C=O | %C | %O | |
| ARCF | 79.55 | 20.45 | - | 23.63 | 45.17 | 31.2 | - | 93.79 | 6.21 |
| ORCF | 64.94 | 32.87 | 2.19 | 14.83 | 25.64 | 50.53 | 9.00 | 82.15 | 17.85 |
Fig. 7. Variations of adsorption capacity (a and e) and removal percentage (b and f) as a function of initial concentration for MG (m = 1 g L-1; t = 4 h) and Pb2+ (m = 1 g L-1; t = 3 h) adsorption at different temperatures; Langmuir (c and g) and Freundlich (d and h) isotherms for MG and Pb2+ adsorption onto the ORCF, respectively.
| Adsorbate | T (K) | Langmuir | Freundlich | |||||
|---|---|---|---|---|---|---|---|---|
| Qm (mg g-1) | KL (L mg-1) | RL | R2 | KF (mg g-1)(L/mg)1/n | n | R2 | ||
| MG | 293 | 666.67 | 0.0908 | 0.0136-0.0268 | 0.9997 | 244.73 | 5.2348 | 0.9543 |
| 303 | 675.68 | 0.1240 | 0.0100-0.0198 | 0.9992 | 277.93 | 5.7362 | 0.9678 | |
| 313 | 680.27 | 0.1822 | 0.0068-0.0125 | 0.9985 | 325.08 | 6.7426 | 0.9854 | |
| 323 | 684.93 | 0.2071 | 0.0060-0.0119 | 0.9976 | 348.13 | 7.3513 | 0.9906 | |
| Pb2+ | 293 | 202.43 | 0.1494 | 0.0083-0.0165 | 0.9984 | 41.32 | 2.6078 | 0.8096 |
| 303 | 206.19 | 0.1892 | 0.0066-0.0130 | 0.9989 | 47.67 | 2.7513 | 0.7991 | |
| 313 | 208.77 | 0.2542 | 0.0049-0.0097 | 0.9991 | 55.95 | 2.9705 | 0.7844 | |
| 323 | 210.53 | 0.3412 | 0.0036-0.0073 | 0.9990 | 64.58 | 3.2149 | 0.7695 | |
Table 4. Adsorption isotherm model parameters for MG and Pb2+ adsorption onto the ORCF.
| Adsorbate | T (K) | Langmuir | Freundlich | |||||
|---|---|---|---|---|---|---|---|---|
| Qm (mg g-1) | KL (L mg-1) | RL | R2 | KF (mg g-1)(L/mg)1/n | n | R2 | ||
| MG | 293 | 666.67 | 0.0908 | 0.0136-0.0268 | 0.9997 | 244.73 | 5.2348 | 0.9543 |
| 303 | 675.68 | 0.1240 | 0.0100-0.0198 | 0.9992 | 277.93 | 5.7362 | 0.9678 | |
| 313 | 680.27 | 0.1822 | 0.0068-0.0125 | 0.9985 | 325.08 | 6.7426 | 0.9854 | |
| 323 | 684.93 | 0.2071 | 0.0060-0.0119 | 0.9976 | 348.13 | 7.3513 | 0.9906 | |
| Pb2+ | 293 | 202.43 | 0.1494 | 0.0083-0.0165 | 0.9984 | 41.32 | 2.6078 | 0.8096 |
| 303 | 206.19 | 0.1892 | 0.0066-0.0130 | 0.9989 | 47.67 | 2.7513 | 0.7991 | |
| 313 | 208.77 | 0.2542 | 0.0049-0.0097 | 0.9991 | 55.95 | 2.9705 | 0.7844 | |
| 323 | 210.53 | 0.3412 | 0.0036-0.0073 | 0.9990 | 64.58 | 3.2149 | 0.7695 | |
Fig. 8. Variations of adsorption capacity (a and d) towards MG and Pb2+ as a function of time (m = 1 g L-1; T = 293 K); Pseudo-first-order kinetic (b and e) and Pseudo-second-order (c and f) kinetic models for MG and Pb2+ adsorption onto the ORCF, respectively.
| Absorbate | C0 (mg L-1) | Pseudo-first-order model | Pseudo-second-order model | ||||
|---|---|---|---|---|---|---|---|
| K1 (min-1) | R2 | Qe (mg g-1) | V0 [mg (g min) -1] | R2 | Qe (mg g-1) | ||
| MG | 400 | 0.0191 | 0.9880 | 466.44 | 8.306 | 0.9937 | 467.29 |
| 600 | 0.0199 | 0.9717 | 814.77 | 10.021 | 0.9922 | 689.66 | |
| 800 | 0.0212 | 0.9486 | 1095.83 | 10.886 | 0.9919 | 806.45 | |
| Pb2+ | 80 | 0.0189 | 0.9431 | 40.43 | 4.088 | 0.9954 | 82.91 |
| 160 | 0.0207 | 0.9456 | 105.83 | 5.241 | 0.9904 | 166.94 | |
| 240 | 0.0152 | 0.8542 | 82.86 | 8.051 | 0.9929 | 201.61 | |
Table 5. Adsorption kinetic parameters for MG and Pb2+ adsorption onto the ORCF.
| Absorbate | C0 (mg L-1) | Pseudo-first-order model | Pseudo-second-order model | ||||
|---|---|---|---|---|---|---|---|
| K1 (min-1) | R2 | Qe (mg g-1) | V0 [mg (g min) -1] | R2 | Qe (mg g-1) | ||
| MG | 400 | 0.0191 | 0.9880 | 466.44 | 8.306 | 0.9937 | 467.29 |
| 600 | 0.0199 | 0.9717 | 814.77 | 10.021 | 0.9922 | 689.66 | |
| 800 | 0.0212 | 0.9486 | 1095.83 | 10.886 | 0.9919 | 806.45 | |
| Pb2+ | 80 | 0.0189 | 0.9431 | 40.43 | 4.088 | 0.9954 | 82.91 |
| 160 | 0.0207 | 0.9456 | 105.83 | 5.241 | 0.9904 | 166.94 | |
| 240 | 0.0152 | 0.8542 | 82.86 | 8.051 | 0.9929 | 201.61 | |
Fig. 9. (a, b) Adsorption of MG and Pb2+ as a function of pH, (c, d) the effect of ionic strength on adsorption of MG and Pb2+ (t = 3 h for MG, 1.5 h for Pb2+; C0 = 600 mg L-1 for MG, 160 mg L-1 for Pb2+; T = 293 K); (e, f) Adsorption of MG and Pb2+ as a function of temperature (t = 3 h for MG, 1.5 h for Pb2+; C0 = 600 mg L-1 for MG, 160 mg L-1 for Pb2+; pH = 6 for MG, 5 for Pb2+).
| Absorbate | Temperature (K) | K (L mol-1) | ln KC | ΔG° (kJ mol-1) | ΔH° (kJ mol-1) | ΔS° (J mol-1 K-1) |
|---|---|---|---|---|---|---|
| MG | 293 | 33133.83 | 10.408 | -25.35 | 22.57 | 163.72 |
| 303 | 45248.84 | 10.720 | -27.01 | |||
| 313 | 66486.6 | 11.105 | -28.90 | |||
| 323 | 75572.86 | 11.233 | -30.16 | |||
| Pb2+ | 293 | 30955.68 | 10.340 | -25.19 | 21.77 | 160.69 |
| 303 | 39202.24 | 10.576 | -26.64 | |||
| 313 | 52670.24 | 10.872 | -28.29 | |||
| 323 | 70696.64 | 11.166 | -29.99 |
Table 6. Thermodynamic parameters for MG and Pb2+ adsorption onto the ORCF.
| Absorbate | Temperature (K) | K (L mol-1) | ln KC | ΔG° (kJ mol-1) | ΔH° (kJ mol-1) | ΔS° (J mol-1 K-1) |
|---|---|---|---|---|---|---|
| MG | 293 | 33133.83 | 10.408 | -25.35 | 22.57 | 163.72 |
| 303 | 45248.84 | 10.720 | -27.01 | |||
| 313 | 66486.6 | 11.105 | -28.90 | |||
| 323 | 75572.86 | 11.233 | -30.16 | |||
| Pb2+ | 293 | 30955.68 | 10.340 | -25.19 | 21.77 | 160.69 |
| 303 | 39202.24 | 10.576 | -26.64 | |||
| 313 | 52670.24 | 10.872 | -28.29 | |||
| 323 | 70696.64 | 11.166 | -29.99 |
Fig. 10. (a) The FTIR spectra of the ORCF before and after adsorption; (b) The zeta potentials of the ARCF and the ORCF at different pH values; (c, d) Intra-particle diffusion models for MG and Pb2+ adsorption onto the ORCF, respectively (m = 1 g L-1; T = 293 K).
Fig. 11. Adsorption-desorption cycles for MG (m = 1 g L-1; C0 = 600 mg L-1; t = 3 h; pH = 6; T = 313 K) and Pb2+ (m = 1 g L-1; C0 = 160 mg L-1; t = 1.5 h; pH = 5; T = 313 K) adsorption by the ORCF.
| Adsorbent | Adsorbate | Temperature (°C), pH | Initial concentration (mg L-1) | Equilibrium concentration (mg L-1) | Maximum adsorption capacity (mg g-1) | Partition coefficient (mg g-1 µM-1) | Refs. |
|---|---|---|---|---|---|---|---|
| ORCF | MG | 40, 6 | 600 | 12.32 | 587.68b | 17.407 | This work |
| Pb2+ | 40, 5 | 160 | 2.20 | 157.80b | 14.855 | ||
| APDA-EA | MG | 30, 5.5 | 100 | 48.66 | 89.84a | 0.674 | [ |
| Pb2+ | 50, 5 | 100 | 38.67 | 69b | 0.370 | ||
| Cell-g-HEMA- co-GMA | MG | 25, 7 | 40 | 15.12 | 24.88a | 0.600 | [ |
| Pb2+ | 25, 7 | 200 | 107.41 | 92.59a | 0.179 | ||
| CuFe2O4/DC | MG | 55, 9.5 | 250 | 154.76 | 952.4a | 2.246 | [ |
| Pb2+ | 55, 6.5 | 250 | 157.89 | 921.1a | 1.209 | ||
| FSBP | MG | 20, 5 | 500 | 409.1 | 90.9b | 0.081 | [ |
| Pb2+ | 20, 5 | 500 | 356.3 | 143.7b | 0.084 | ||
| h-GG/SiO2 | MG | 30, 7 | 1000 | 218.75 | 781.25a | 1.303 | [ |
| Pb2+ | 30, 7 | 1400 | 754.85 | 645.15a | 0.177 | ||
| CuS-NRs-AC | MG | 25, 6 | 30 | 9.56 | 145.98a | 5.570 | [ |
| Pb2+ | 25, 6 | 30 | 23.30 | 47.89a | 0.426 | ||
| PDA/CS/Fe3O4 | MG | 30, - | 30 | 18.51 | 57.47a | 1.133 | [ |
| Pb2+ | 30, - | 30 | 20.52 | 47.39a | 0.478 | ||
| Cu-MOFs/Fe3O4 | MG | 45, - | - | - | 113.67b | - | [ |
| Pb2+ | 45, - | - | - | 219b | - | ||
| Activated carbon pellet | MG | 25, - | - | - | 395b | - | [ |
| alginate-acrylamide hydrogel | Pb2+ | 25, 5 | 500 | 60 | 110a | 0.380 | [ |
Table 7. Comparison of different adsorbents for MG and Pb2+ removal.
| Adsorbent | Adsorbate | Temperature (°C), pH | Initial concentration (mg L-1) | Equilibrium concentration (mg L-1) | Maximum adsorption capacity (mg g-1) | Partition coefficient (mg g-1 µM-1) | Refs. |
|---|---|---|---|---|---|---|---|
| ORCF | MG | 40, 6 | 600 | 12.32 | 587.68b | 17.407 | This work |
| Pb2+ | 40, 5 | 160 | 2.20 | 157.80b | 14.855 | ||
| APDA-EA | MG | 30, 5.5 | 100 | 48.66 | 89.84a | 0.674 | [ |
| Pb2+ | 50, 5 | 100 | 38.67 | 69b | 0.370 | ||
| Cell-g-HEMA- co-GMA | MG | 25, 7 | 40 | 15.12 | 24.88a | 0.600 | [ |
| Pb2+ | 25, 7 | 200 | 107.41 | 92.59a | 0.179 | ||
| CuFe2O4/DC | MG | 55, 9.5 | 250 | 154.76 | 952.4a | 2.246 | [ |
| Pb2+ | 55, 6.5 | 250 | 157.89 | 921.1a | 1.209 | ||
| FSBP | MG | 20, 5 | 500 | 409.1 | 90.9b | 0.081 | [ |
| Pb2+ | 20, 5 | 500 | 356.3 | 143.7b | 0.084 | ||
| h-GG/SiO2 | MG | 30, 7 | 1000 | 218.75 | 781.25a | 1.303 | [ |
| Pb2+ | 30, 7 | 1400 | 754.85 | 645.15a | 0.177 | ||
| CuS-NRs-AC | MG | 25, 6 | 30 | 9.56 | 145.98a | 5.570 | [ |
| Pb2+ | 25, 6 | 30 | 23.30 | 47.89a | 0.426 | ||
| PDA/CS/Fe3O4 | MG | 30, - | 30 | 18.51 | 57.47a | 1.133 | [ |
| Pb2+ | 30, - | 30 | 20.52 | 47.39a | 0.478 | ||
| Cu-MOFs/Fe3O4 | MG | 45, - | - | - | 113.67b | - | [ |
| Pb2+ | 45, - | - | - | 219b | - | ||
| Activated carbon pellet | MG | 25, - | - | - | 395b | - | [ |
| alginate-acrylamide hydrogel | Pb2+ | 25, 5 | 500 | 60 | 110a | 0.380 | [ |
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