Fast Removal of Aqueous Mn(Ⅱ) Using Partially Reduced Graphene Oxide-Fe3O4†

doi:10.7503/cjcu20160664

Abstract

Abstract:

Partially reduced graphene oxide-Fe₃O₄ composite(PRGO-Fe₃O₄) was prepared by one step co-precipitation onto graphene oxide(GO) synthesized by modified Hummers method. The as obtained composite was characterized by XRD, FESEM, EDX, HRTEM, SAED, XPS and FTIR. The impact of pH, contact time, dosage, foreign substances, reduction of GO and cycle times on the adsorption performance of the composite towards Mn(Ⅱ) were investigated and the dsorption isotherm, thermodynamics and kinetics were analyzed. The results indicate that Fe₃O₄ distribute evenly and uniformly in the as-obtained composite, with a fine particle size of 15—20 nm, resulting in a low remanence and coercivity. The composite shows efficient adsorption property and good recycability towards aqueous Mn(Ⅱ) owing to the thin GO sheets in its structure caused by the anchoring effect of Fe₃O₄. Adsorption equilibrium was reached within 3 min with the adsorption percent and capacity of 99.35% and 404.49 mg/g, respectively, under the conditions of pH=7, dosage 500 mg/L, and initial concentration of Mn(Ⅱ) of 201.32 mg/L, with the subsequent magnetic separation taking only 10 s. After five consecutive cycles, the adsorption capacity of the composite remians 78% that of the first cycle. Analyses on the mechanism and thermodynamics show that the adsorption is an endothermic, sponta-neous and monolayer chemical adsorption step.

Key words: Partially reduced graphene oxide-Fe3O4(PRGO-Fe3O4), Fast removal of Mn(Ⅱ), Adsorption property

CLC Number:

O647.32

TrendMD:

BULIN Chaoke, GUO Ting, ZHANG Bangwen, DAI Zhian, YU Huitao, XING Ruiguang, ZI Luxiong. Fast Removal of Aqueous Mn(Ⅱ) Using Partially Reduced Graphene Oxide-Fe₃O₄^†[J]. Chem. J. Chinese Universities, 2017, 38(2): 217.

Figures/Tables 15

Fig.1 XRD pattern of PRGO-Fe3O4

Fig.2 FESEM images of GO(A) and PRGO-Fe3O4(B) and EDX pattern PRGO-Fe3O4(C)

Fig.3 HRTEM images of GO(A) and PRGO-Fe3O4(B, C) and SAED pattern of PRGO-Fe3O4(D)

Fig.4 FTIR spectra of GO(a), PRGO-Fe3O4(b) and Fe3O4(c)

Fig.5 Survey XPS spectra of GO(a), PRGO-Fe3O4(b) and PRGO-Fe3O4-Mn(c)(A), C1s XPS spectra of GO(B) and PRGO-Fe3O4(C) and O1s XPS spectra of PRGO-Fe3O4(a) and PRGO-Fe3O4-Mn(b)(D)

Fig.6 Magnetization curve of PRGO-Fe3O4Inset at the upper left corner shows the magnification of hysteresis loop; inset at the lower right corner shows the magnetic separation of PRGO-Fe3O4 from water under an external magnetic field.

Fig.7 Dependence of zeta potential of PRGO- Fe3O4 hydrogel on pH

Fig.8 Effect of pH on Mn(Ⅱ) adsorptionInset shows the evolution of Mn(Ⅱ) species with pH.

Fig.9 Effect of contact time on Mn(Ⅱ) adsorption

Fig.10 Effect of adsorbent dosage on Mn(Ⅱ) adsorption

Fig.11 Effect of humic acid concentration on Mn(Ⅱ) adsorption

Fig.12 Comparison on the adsorption property of GO and PRGO-Fe3O4 towards Mn(Ⅱ)

Fig.13 Cycling adsorption capacity of PRGO-Fe3O4 towards Mn(Ⅱ)

Table 1 Parameters of the adsorption models

Model	Parameter	R²	Model	Parameter	R²
Langmuir	Q_max=943.3962 mg/g	0.9439	Pseudo first order	k₁=1.8585 min^-1	0.9647
	K_L=0.2494 L/mg			Q_e=98.0600 mg/g
Freundlich	n=2.6687	0.9908	Pseudo second order	k₂=0.2034 g·mg^-1·min^-1	0.9999
	K_L=541.6608			Q_e=404.8583 mg/g
Temkin	A_T=5.4466 J/mol	0.9962	Intra-particle diffusion	K_pi=13.4465 mg·g^-1·min^-0.5	0.9925
	B_T=1.8775 L/g			c=98.0611 mg/g
D-R	Q_max=1757.5042 mg/g	0.8855	Liquid film diffusion		0.9648
	E=39.3643 kJ/mol

Table 2 Thermodynamic data of liquid film diffusion at different temperature according to Van’t Hoff formula

Temperature/K	ΔG/(kJ/mol)	ΔH/(kJ/mol)	ΔS/(J·K^-1·mo^-1)
293	-10.32	16.70	93.24
298	-10.79
303	-11.26
313	-11.72

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Fast Removal of Aqueous Mn(Ⅱ) Using Partially Reduced Graphene Oxide-Fe₃O₄^†

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