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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

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Front. Environ. Sci. Eng.    2022, Vol. 16 Issue (11) : 138    https://doi.org/10.1007/s11783-022-1572-1
RESEARCH ARTICLE
Separation/degradation behavior and mechanism for cationic/anionic dyes by Ag-functionalized Fe3O4-PDA core-shell adsorbents
Qingqing Li1, Chao Lv1, Xiangwei Xia2, Chao Peng3, Yan Yang4, Feng Guo4, Jianfeng Zhang1,4()
1. College of Mechanics and Materials, Hohai University, Nanjing 210098, China
2. Sinosteel Maanshan General Institute of Mining Research Co., Ltd, Maanshan 243004, China
3. Productivity Centre of Jiangsu Province, Nanjing 210042, China
4. Engineering Research Center on Utilization of Alternative Water Resources, Nanjing 210000, China
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Abstract

● PDA-Fe3O4-Ag was made by hydrothermal and oxidation self-polymerization method.

● PDA-Fe3O4-Ag had great magnetic separation performance.

● PDA-Fe3O4-Ag had good adsorption and degradation performance for ionic dyes.

● PDA-Fe3O4-Ag showed NR and MO degradation potential of 91.2% and 87.5%, respectively.

High-performance adsorbents have been well-studied for the removal of organic dye pollutants to promote environment remediation. In this study, an Ag nanoparticle-functionalized Fe3O4-PDA nanocomposite adsorbent (PDA-Fe3O4-Ag) was synthesized, and the adsorption/separation performance of commonly used cationic and anionic organic dyes by the PDA-Fe3O4-Ag adsorbent were assessed. Overall, PDA-Fe3O4-Ag exhibited a significantly higher adsorption capacity for cationic dyes compared to anionic dyes, the highest of which was more than 110.0 mg/g (methylene blue (MB)), which was much higher than not only the adsorption capacities of the anionic dyes in this study but also other dye adsorption capacities reported in the literature. The dye adsorption kinetics data fitted well to both the pseudo second-order kinetics model and the Langmuir isotherm model, suggesting a monolayer-chemisorption-dominated adsorption mode. Thermodynamics analysis indicated that the adsorption process was both endothermic and spontaneous. Furthermore, the PDA-Fe3O4-Ag adsorbent achieved high photodegradation removal rates of the dyes, especially neutral red (NR) and methyl orange (MO), which were 91.2% and 87.5%, respectively. With the addition of PDA-Fe3O4-Ag, the degradation rate constants of NR and MO increased from 0.08 × 10−2 and 0 min−1 to 2.11 × 10−2 and 1.73 × 10−2 min−1, respectively. The high adsorption and photocatalytic degradation performance of the PDA-Fe3O4-Ag adsorbent make it an excellent candidate for removing cationic and anionic dyes from the industrial effluents.

Keywords PDA      Fe3O4      Magnetic adsorbent      Cationic dyes      Anionic dyes     
Corresponding Author(s): Jianfeng Zhang   
Issue Date: 23 May 2022
 Cite this article:   
Qingqing Li,Chao Lv,Xiangwei Xia, et al. Separation/degradation behavior and mechanism for cationic/anionic dyes by Ag-functionalized Fe3O4-PDA core-shell adsorbents[J]. Front. Environ. Sci. Eng., 2022, 16(11): 138.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-022-1572-1
https://academic.hep.com.cn/fese/EN/Y2022/V16/I11/138
Fig.1  Illustration for the fabrication of PDA-Fe3O4-Ag nanomaterials by hydrothermal method and oxidation self-polymerization (a) the fabrication of Fe3O4 nanoparticles; (b,c) the fabrication of PDA -Fe3O4-Ag.
Fig.2  Microstructural morphology of PDA-Fe3O4-Ag: (a) SEM image; (b) HRTEM images, (c) EDS mapping.
Fig.3  Effect of contact time on adsorption capacity of different dyes by PDA-Fe3O4-Ag. Experimental conditions: Initial dye (MB, JGB, MG, RhB, NR, CR, MO) = 100 mg/L; adsorbents dosage = 0.5 g/L; temperature = 25±1 °C.
Dyes Pseudo-second-order model Experimental qe (mg/g)
k2 (g/mg/min) qe (mg/g) R2
MB 0.000259 117 0.9990 115
JGB 0.000148 106 0.9962 102
MG 0.000172 89.1 0.9962 86.0
RhB 0.000193 76.5 0.9965 74.0
NR 0.000322 39.9 0.9916 38.0
CR 0.000609 29.2 0.9941 29.0
MO 0.000802 19.3 0.9939 19.0
Tab.1  Quasi-secondary kinetic parameters of PDA-Fe3O4-Ag for dyes adsorption at 298 K
Dyes Intra-particle diffusion model
First stage Second stage
ki,1 (mg/g/min0.5) R12 ki,2 (mg/g/min0.5) R22
MB 19.3 0.9899 1.62 0.9334
JGB 12.7 0.9833 2.19 0.9680
MG 7.70 0.9706 1.96 0.9436
RhB 7.35 0.9555 1.50 0.9247
NR 4.62 0.9949 0.889 0.9736
CR 4.24 0.9752 0.491 0.9755
MO 1.72 0.9485 0.418 0.9555
Tab.2  Intra-particle diffusion kinetic of PDA-Fe3O4-Ag for dyes adsorption at 298 K
Dyes T (K) Langmuir constants Freundlich constants
KL (L/mg) qmax (mg/g) R2 1/n KF (L/g) R2
MB 298 0.00298 156 0.9932 0.910 3.94 0.9860
313 0.00392 191 0.9888 1.00 5.00 0.9748
333 0.00691 212 0.9901 0.967 9.82 0.9358
JGB 298 0.0124 128 0.9907 0.755 5.00 0.9961
313 0.00117 109 0.9815 0.997 3.90 0.9381
333 0.00262 159 0.9997 1.08 4.11 0.9715
MG 298 0.00678 79.1 0.9947 0.735 3.94 0.9826
313 0.00923 126 0.9995 0.751 4.72 0.9868
333 0.0123 134 0.9993 0.706 6.58 0.9736
RhB 298 0.00118 75.4 0.9971 0.723 3.30 0.9958
313 0.0195 118 0.9991 0.617 5.82 0.9976
333 0.0110 127 0.9999 0.590 7.34 0.9974
NR 298 0.00788 44.3 0.9558 0.463 4.14 0.9559
313 0.00142 56.8 0.9965 0.525 4.38 0.9966
333 0.0171 88.9 0.9985 0.509 6.33 0.9982
CR 298 0.00201 22.3 0.9519 0.644 1.58 0.9520
313 0.00355 28.3 0.9997 0.390 7.72 0.9974
333 0.00531 41.1 0.9973 0.460 4.74 0.9874
MO 298 0.000860 19.0 0.9873 0.955 0.239 0.9602
313 0.00284 21.3 0.9817 0.718 0.893 0.9149
333 0.0101 37.1 0.9999 0.648 1.53 0.9882
Tab.3  Isothermal parameters of PDA-Fe3O4-Ag for different dyes adsorption
Fig.4  Photocatalytic degradation behavior and kinetics of dyes; (a, b) blank; (c, d) PDA-Fe3O4-Ag. Experimental conditions: Initial dye (MB, JGB, MG, RhB, NR, CR, MO) = 5 mg/L; catalysts dosage = 1.25 g/L; temperature=25±1 °C.
Fig.5  (a) FTIR spectra of MB, PDA-Fe3O4-Ag before and after MB adsorption in aqueous solution; (b) XPS spectra of PDA-Fe3O4-Ag before and after MB adsorption; (c–h) Peak-fitting XPS spectra in the C 1s, N 1s, and O 1s regions of PDA-Fe3O4-Ag and PDA-Fe3O4-Ag-MB: C 1s of (c) PDA-Fe3O4-Ag and (d) PDA-Fe3O4-Ag-MB; N 1s of (e) PDA-Fe3O4-Ag and (f) PDA-Fe3O4-Ag-MB; O 1s of (g) PDA-Fe3O4-Ag and (h) PDA-Fe3O4-Ag-MB.
Fig.6  Schematic treatment mechanism illustration for dyes by PDA-Fe3O4-Ag: (a) Adsorption; (b) Catalytic degradation.
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