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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2020, Vol. 14 Issue (3) : 52    https://doi.org/10.1007/s11783-020-1229-x
RESEARCH ARTICLE
Crosslinking acrylamide with EDTA-intercalated layered double hydroxide for enhanced recovery of Cr(VI) and Congo red: Adsorptive and mechanistic study
Jing Li, Haiqin Yu, Xue Zhang, Rixin Zhu, Liangguo Yan()
School of Water Conservancy and Environment, University of Jinan, Jinan 250022, China
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Abstract

• Functional groups of AM and EDTA in composite increased removal of Cr(VI) and CR.

• Removal process reached equilibrium within 30 min and was minimally affected by pH.

• Elimination of Cr(VI) was promoted by coexisting CR.

• Adsorption process of CR was less influenced by the presence of Cr(VI).

• Mechanisms were electrostatic attraction, surface complexation and anion exchange.

We prepared ethylenediaminetetraacetic acid (EDTA)-intercalated MgAl-layered double hydroxide (LDH-EDTA), then grafted acrylamide (AM) to the LDH-EDTA by a cross-linking method to yield a LDH-EDTA-AM composite; we then evaluated its adsorptive ability for Congo red (CR) and hexavalent chromium (Cr(VI)) in single and binary adsorption systems. The adsorption process on LDH-EDTA-AM for CR and Cr(VI) achieved equilibrium quickly, and the removal efficiencies were minimally affected by initial pH. The maximum uptake quantities of CR and Cr(VI) on LDH-EDTA-AM were 632.9 and 48.47 mg/g, respectively. In mixed systems, chromate removal was stimulated by the presence of CR, while the adsorption efficiency of CR was almost not influenced by coexisting Cr(VI). The mechanisms involved electrostatic attraction, surface complexation, and anion exchange for the adsorption of both hazardous pollutants. In the Cr(VI) adsorption process, reduction also took place. The removal efficiencies in real contaminated water were all higher than those in the laboratory solutions.

Keywords Chromate      Dye adsorption      Simultaneous removal      Cross-linking method      Amino functionalization     
Corresponding Author(s): Liangguo Yan   
Issue Date: 11 March 2020
 Cite this article:   
Jing Li,Haiqin Yu,Xue Zhang, et al. Crosslinking acrylamide with EDTA-intercalated layered double hydroxide for enhanced recovery of Cr(VI) and Congo red: Adsorptive and mechanistic study[J]. Front. Environ. Sci. Eng., 2020, 14(3): 52.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-020-1229-x
https://academic.hep.com.cn/fese/EN/Y2020/V14/I3/52
Fig.1  XRD patterns (A) and FTIR spectra (B) of LDH-EDTA (a), LDH-EDTA-AM (b), and AM (c).
Fig.2  XPS spectrum (A), high-resolution XPS spectra of C 1s (B), N 1s (C), and O 1s (D) of LDH-EDTA-AM.
Fig.3  TEM (A), high resolution TEM (B), SEM (C), and EDS element composition (D) of LDH-EDTA-AM.
Fig.4  Adsorption quantity of CR and Cr(VI) as a function of reaction time (A) (concentration: Cr(VI): 50 mg/L, CR: 100 mg/L, dosage: 0.03 g, pH: initial value, reaction time: 5–360 min), linear fit of IPD model (B), and adsorption isotherms of Cr(VI) (C) and CR (D) (dosage: 0.03 g, pH: initial value, reaction time: 30 min, concentration of Cr(VI): 20–200 mg/L, concentration of CR: 10–800 mg/L) in single and Cr-CR binary systems.
Model Parameter Unit Cr(VI) CR
q(e,exp) mg/g 28.71 66.67
Pseudo-first-order kinetic equation q(e,cal) mg/g 2.325 3.053
k1 1/min 0.0095 0.0094
R2 0.7083 0.7068
Pseudo-second-order kinetic equation q(e,cal) mg/g 28.81 66.93
k2 g/(mg·min) 0.0185 0.0143
R2 0.9996 0.9999
Intra-particle diffusion kd1 mg/(g·min1/2) 2.476 0.8437
C1 17.19 58.83
R2 0.9797 0.9108
kd2 mg/(g·min1/2) 0.0329 0.0018
C2 31.10 66.64
R2 0.9232 0.9582
Tab.1  Calculated parameters of the kinetic models for the adsorption of Cr(VI) and CR by LDH-EDTA-AM
Pollutant Langmuir isotherm model Freundlich isotherm model
qm
(mg/g)
b
(L/mg)
R2 kf
((mg/g)/(mg/L)n)
n R2
Cr(VI) 48.47 0.9251 0.9995 23.11 5.551 0.7569
Cr(VI) + 10 mg/L CR 53.82 0.6678 0.9985 24.43 5.269 0.8260
Cr(VI) + 20 mg/L CR 58.93 0.5582 0.9976 25.43 4.981 0.8687
CR 632.9 0.06715 0.9562 39.43 1.397 0.9755
CR+ 10 mg/L Cr(VI) 635.6 0.05362 0.9174 34.55 1.300 0.9398
CR+ 20 mg/L Cr(VI) 637.9 0.06603 0.9476 39.84 1.373 0.9752
Tab.2  Calculated parameters of the isotherm models for the adsorption of Cr(VI) and CR by LDH-EDTA-AM
Fig.5  Zeta potentials (A), XRD patterns (B), and FTIR spectra (C) of LDH-EDTA-AM before and after adsorption of Cr(VI) and CR.
Fig.6  XPS survey (A), Cr 2p (B), S 2p (C), C 1s (D), N 1s (E), and O 1s (F) spectra of LDH-EDTA-AM before and after adsorption in Cr(VI)-CR binary systems.
Fig.7  Regeneration cycles of LDH-EDTA-AM for CR (A) and Cr(VI) (B) (concentration: Cr(VI): 50 mg/L, CR: 100 mg/L, dosage: 0.03 g, reaction time: 30 min, pH: initial value) in Cr(VI)-CR binary systems, and effects of adsorbent dosage (C) (concentration: Cr(VI): 50 mg/L, CR: 100 mg/L, reaction time: 30 min, pH: initial value, dosage: 0.005–0.15 g) and initial solution pH (D) (concentration: Cr(VI): 50 mg/L, CR: 100 mg/L, dosage: 0.03 g, reaction time: 30 min, pH: 2.0–12.0) on adsorption by LDH-EDTA-AM.
Adsorbent Adsorption capacity (mg/g) pH Reference
Cr(VI) CR
LDH-EDTA-AM 48.47 632.9 2.0–10.0 this work
MgAlZr-LDH 24.32 4.0 Das et al. (2004)
LDH/ESM 27.9 5.1 Guo et al. (2011)
CaAl-LDH 42.92 3.0 Zhang et al. (2012)
Fe3O4/MgAl-LDH 289 2.0–6.0 Shan et al. (2014)
ZnAl-CLDH 21.3 3.0 Yan et al. (2015)
Fe3O4@ZnAl-CLDH 19.6 3.0 Yan et al. (2015)
Calcined MgAl-CO3-LDH 143.2 2.0 Li et al. (2016a)
Mg/Al-LDH nanoflakes 585 4.0 Li et al. (2016b)
NiFe-LDH 26.78 2.0 Lu et al. (2016)
Tab.3  Comparison of adsorption capacities of LDH-based adsorbents for Cr(VI) and CR
Fig.8  Adsorption efficiency of LDH-EDTA-AM for CR and Cr(VI) in different wastewater samples (concentration: Cr(VI): 50 mg/L, CR: 100 mg/L, reaction time: 30 min, dosage: 0.03 g, pH: initial value).
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