J. Mater. Sci. Technol. ›› 2019, Vol. 35 ›› Issue (9): 1809-1816.DOI: 10.1016/j.jmst.2019.04.016
• Orginal Article • Next Articles
Jing Wanga, Liang Zhanga, Tianshu Zhanga, Ting Dua, Tao Lib, Tianli Yuea, Zhonghong Lia, Jianlong Wanga*()
Received:
2019-01-25
Revised:
2019-03-18
Accepted:
2019-04-16
Online:
2019-09-20
Published:
2019-07-26
Contact:
Wang Jianlong
About author:
1 These authors contributed equally to this work.
Jing Wang, Liang Zhang, Tianshu Zhang, Ting Du, Tao Li, Tianli Yue, Zhonghong Li, Jianlong Wang. Selective removal of heavy metal ions in aqueous solutions by sulfide-selector intercalated layered double hydroxide adsorbent[J]. J. Mater. Sci. Technol., 2019, 35(9): 1809-1816.
Scheme 1. Synthesis schematic of the flower-like hierarchical NFL-S microstructure and SEM images of the NFL-based composites with the addition of varying amounts of (NH4)2MoS4 (0, 0.05 and 0.1 g).
Fig. 1. (a,b) SEM images of the flower-like NFL-S hierarchical microcomposite at different scales. (c) TEM images of the as-fabricated NFL-S hierarchical microcomposite. (d) HRTEM image of the NiFe-LDH taken from the image location as shown in (c).
Fig. 2. (a) Schematic crystalline structure of NFL-S displaying the host layered construction and abundant interlayer anions. (b) XRD patterns of NFL (black) and NFL-S (red) and, for comparison, the inset schematics of the crystalline structures representing the enlarged interlayer space after intercalation. XPS spectra of (c) NFL-S, (d) Ni 2p, (e) Fe 2p and (f) S 2p.
Single ion | C0 (ppm) | NFL-S | NFL | ||||
---|---|---|---|---|---|---|---|
Ct (ppm) | Removal efficiency (%) | kd (mL/g) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) | ||
Pb2+ | 88.09 | 0.012 | 99.88 | 8.17 × 105 | 0.416 | 95.83 | 2.30 × 104 |
Cu2+ | 95.61 | 0.053 | 99.23 | 1.29 × 105 | 1.042 | 84.85 | 5.60 × 103 |
Zn2+ | 97.62 | 3.590 | 52.76 | 1.12 × 103 | 3.8385 | 49.50 | 980 |
Cd2+ | 89.74 | 6.328 | 34.29 | 522 | 7.12 | 26.06 | 352 |
Mn2+ | 85.032 | 6.057 | 25.16 | 336 | 6.59 | 18.57 | 228 |
Table 1 Adsorption results of NFL-S and NFL at low concentrations ($\widetilde{1}$0 ppm).
Single ion | C0 (ppm) | NFL-S | NFL | ||||
---|---|---|---|---|---|---|---|
Ct (ppm) | Removal efficiency (%) | kd (mL/g) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) | ||
Pb2+ | 88.09 | 0.012 | 99.88 | 8.17 × 105 | 0.416 | 95.83 | 2.30 × 104 |
Cu2+ | 95.61 | 0.053 | 99.23 | 1.29 × 105 | 1.042 | 84.85 | 5.60 × 103 |
Zn2+ | 97.62 | 3.590 | 52.76 | 1.12 × 103 | 3.8385 | 49.50 | 980 |
Cd2+ | 89.74 | 6.328 | 34.29 | 522 | 7.12 | 26.06 | 352 |
Mn2+ | 85.032 | 6.057 | 25.16 | 336 | 6.59 | 18.57 | 228 |
Single ion | C0 (ppm) | NFL-S | NFL | ||||
---|---|---|---|---|---|---|---|
Ct (ppm) | Removal efficiency (%) | kd (mL/g) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) | ||
Pb2+ | 88.09 | 10.23 | 77.86 | 7.61 × 103 | 48.11 | 39.98 | 831 |
Cu2+ | 95.61 | 18.39 | 77.22 | 4.20 × 103 | 52.63 | 42.98 | 816 |
Zn2+ | 97.62 | 53.59 | 44.03 | 821 | 62.37 | 35.25 | 565 |
Cd2+ | 89.74 | 76.33 | 13.41 | 175 | 85.63 | 4.11 | 48 |
Mn2+ | 85.032 | 82.96 | 2.08 | 25 | 83.25 | 1.78 | 21 |
Table 2 Adsorption results of NFL-S and NFL at high concentrations ($\widetilde{1}$00 ppm).
Single ion | C0 (ppm) | NFL-S | NFL | ||||
---|---|---|---|---|---|---|---|
Ct (ppm) | Removal efficiency (%) | kd (mL/g) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) | ||
Pb2+ | 88.09 | 10.23 | 77.86 | 7.61 × 103 | 48.11 | 39.98 | 831 |
Cu2+ | 95.61 | 18.39 | 77.22 | 4.20 × 103 | 52.63 | 42.98 | 816 |
Zn2+ | 97.62 | 53.59 | 44.03 | 821 | 62.37 | 35.25 | 565 |
Cd2+ | 89.74 | 76.33 | 13.41 | 175 | 85.63 | 4.11 | 48 |
Mn2+ | 85.032 | 82.96 | 2.08 | 25 | 83.25 | 1.78 | 21 |
NFL-S | C0 (ppm) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) |
---|---|---|---|---|
Pb2+ | 9.612 | 0.005 | 99.95 | 1.92 × 106 |
Cu2+ | 8.066 | 0.017 | 99.79 | 4.85 × 105 |
Zn2+ | 8.600 | 4.590 | 46.63 | 873 |
Cd2+ | 9.446 | 9.113 | 3.53 | 37 |
Mn2+ | 8.093 | 8.040 | 0.66 | 6 |
Table 3 Adsorption of NFL-S for the five mixed ions.
NFL-S | C0 (ppm) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) |
---|---|---|---|---|
Pb2+ | 9.612 | 0.005 | 99.95 | 1.92 × 106 |
Cu2+ | 8.066 | 0.017 | 99.79 | 4.85 × 105 |
Zn2+ | 8.600 | 4.590 | 46.63 | 873 |
Cd2+ | 9.446 | 9.113 | 3.53 | 37 |
Mn2+ | 8.093 | 8.040 | 0.66 | 6 |
Adsorbent dosage (mg/mL) | Single ion | C0 (ppm) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) |
---|---|---|---|---|---|
1 | Pb2+ | 10.2 | 0.015 | 99.85 | 6.79 × 105 |
Cu2+ | 9.0419 | 0.929 | 89.73 | 8.73 × 103 | |
Zn2+ | 8.455 | 4.620 | 45.36 | 830 | |
2 | Pb2+ | 10.2 | 0.004 | 100.00 | 2.55 × 106 |
Cu2+ | 9.0419 | 0.114 | 98.74 | 7.83 × 104 | |
Zn2+ | 8.455 | 2.623 | 68.98 | 2.22 × 103 |
Table 4 Selective adsorption of NFL-S for separating Pb2+, Cu2+, and Zn2+.
Adsorbent dosage (mg/mL) | Single ion | C0 (ppm) | Ct (ppm) | Removal efficiency (%) | kd (mL/g) |
---|---|---|---|---|---|
1 | Pb2+ | 10.2 | 0.015 | 99.85 | 6.79 × 105 |
Cu2+ | 9.0419 | 0.929 | 89.73 | 8.73 × 103 | |
Zn2+ | 8.455 | 4.620 | 45.36 | 830 | |
2 | Pb2+ | 10.2 | 0.004 | 100.00 | 2.55 × 106 |
Cu2+ | 9.0419 | 0.114 | 98.74 | 7.83 × 104 | |
Zn2+ | 8.455 | 2.623 | 68.98 | 2.22 × 103 |
Fig. 3. Adsorption kinetic curves for Cu2+ and Pb2+: (a) ion concentration change following the contact time, (b) removal efficiency as a function of the contact time, (c) sorption capacity (qt) with contact time, (d) pseudo-second-order kinetic plots for the ion sorption, (e) Langmuir equilibrium isotherm curves of NFL-S for Pb2+ and Cu2+, and (f) Ce/qe plotted against the equilibrium concentration (Ce).
Fig. 4. (a) Reaction scheme of NFL-S and the binding modes of NFL-S with M2+ in the LDH gallery. (b) XRD patterns of NFL-S before and after the adsorption of different heavy metal and mixed ions at concentrations of 10 ppm. The characteristic diffraction peaks from left to right represent the lattice planes of (003), (006), (100), (012), and (110), respectively. (c) O 1 s and S 2p of NFL-S before and after the adsorption of heavy metal ions. 1, 2 and 3 correspond to the binding energies of S 2p for S2-, S-, and S6+.
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