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Frontiers of Chemical Science and Engineering

ISSN 2095-0179

ISSN 2095-0187(Online)

CN 11-5981/TQ

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Front. Chem. Sci. Eng.    2021, Vol. 15 Issue (5) : 1185-1196    https://doi.org/10.1007/s11705-020-2032-8
RESEARCH ARTICLE
Efficient removal of Cr(VI) and Pb(II) from aqueous solution by magnetic nitrogen-doped carbon
Wanyue Liu1, Xiaoqin Liu1, Jinming Chang1,2, Feng Jiang1, Shishi Pang1, Hejun Gao1,2(), Yunwen Liao1(), Sheng Yu1
1. College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637000, China
2. Institute of Applied Chemistry, China West Normal University, Nanchong 637000, China
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Abstract

The magnetic nitrogen-doped carbon (MNC) was prepared from polypyrrole by a simple high temperature calcination process in this paper. The structure and properties of MNC were analyzed by scanning electron microscope, Fourier transform infrared spectroscopy, X-ray diffraction, Brunner-Emmet-Teller, vibrating sample magnetometer, and X-ray photoelectron spectroscopy. The capacity of MNC to adsorb Cr(VI) and Pb(II) was evaluated. The effects of the initial pH, dosage, concentration and temperature on the adsorption capacity of MNC were measured. MNC had a large specific surface area and a special porous structure. Its nitrogen and carbon sources were rich, and the ratio of carbon to nitrogen was fixed. The maximum Cr(VI)-adsorption capacity and maximum Pb(II) adsorption capacity of MNC could reach 456.63 and 507.13 mg∙g−1 at 318 K, respectively. The pseudo-second-order model was used to describe the adsorption kinetics of MNC, and the Freundlich model was employed to discuss its isotherms. The adsorption process was affected by the electrostatic force, the reducing reaction, pores and chelation. The results of this study suggest that MNC is a material with superior performance, and is very easily regenerated, reused, and separated in the adsorption process.
Keywords magnetic      nitrogen-doped carbon      adsorption      Cr(VI)      Pb(II)     
Corresponding Author(s): Hejun Gao,Yunwen Liao   
Just Accepted Date: 03 March 2021   Online First Date: 12 April 2021    Issue Date: 30 August 2021
 Cite this article:   
Wanyue Liu,Xiaoqin Liu,Jinming Chang, et al. Efficient removal of Cr(VI) and Pb(II) from aqueous solution by magnetic nitrogen-doped carbon[J]. Front. Chem. Sci. Eng., 2021, 15(5): 1185-1196.
 URL:  
https://academic.hep.com.cn/fcse/EN/10.1007/s11705-020-2032-8
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I5/1185
Fig.1  Preparation process of MNC.
Fig.2  Micromorphology of (a and b) MNC, and mapping of MNC: (c) all elements; (d) N; (e) Fe; (f) Co.
Fig.3  FTIR spectra of MNC and NC.
Fig.4  XRD patterns of MNC and NC.
Fig.5  (a) BET analysis of MNC and NC; (b) BJH pore size distributions of MNC and NC.
Fig.6  XPS spectra of (a) MNC, (b) N 1s, (c) Co 2p and (d) Fe 2p.
Fig.7  Effect of pH on (a) Cr(VI) and (b) Pb(II) adsorption by MNC and NC (dosage= 2 mg, adsorption equilibrium time= 2 h, the initial CCr(VI) = 20 mg?L−1, CPb(II) = 20 mg?L−1).
Fig.8  Effect of the adsorption equilibrium time on the adsorption capacity: (a and b) MNC; (c and d) NC.
Kinetic models C0/(mg·L−1, Cr(VI)) C0/(mg·L−1, Pb(II))
20 40 60 20 60 100
?qe,exp/(mg·g−1) 185.71 333.83 363.33 130.85 284.23 390.75
Pseudo-first-order
?qe,cal/(mg·g−1) 34.57 103.39 116.95 26.89 61.64 179.11
?k1/(g·mg−1·min−1) 4.24 × 10−2 2.13 × 10−2 2.49 × 10−2 9.93 × 10−3 1.70 × 10−2 1.64 × 10−2
?R2 0.7811 0.8663 0.7420 0.8414 0.4714 0.9287
Pseudo-second-order
?qe,cal/(mg·g−1) 186.92 337.84 367.65 130.89 287.36 398.41
?k2/(g·mg−1·min−1) 3.47 × 10−3 7.98 × 10−4 7.56 × 10−4 4.52 × 10−3 1.08 × 10−3 3.51 × 10−4
?R2 0.9999 0.9999 0.9999 0.9999 0.9998 0.9993
Elovich
?α1/(mg·g−1·min−2) 384.65 176.29 233.38 1.76 × 104 2040.33 906.15
?b1/(g·mg−1·min−1) 3.19 × 10−2 1.39 × 10−2 1.34 × 10−2 9.29 × 10−2 3.14 × 10−2 2.19 × 10−2
?R12 0.9888 0.9469 0.8299 0.9481 0.8942 0.9468
?α2/(mg·g−1·min−1) 7.05 × 10170 6.05 × 1019 1.26 × 1022 7.74 × 1034 5.70 × 10111 1.31 × 10103
?b2/(g·mg−1·min−1) 2.15 1.48 × 10−2 0.15 0.65 0.92 0.62
?R22 0.9566 0.9168 0.9322 0.8416 0.9304 0.9043
Liquid-film
?kf /min 0.0189 0.0206 0.0162 0.0154 0.0185 0.0213
?R2 0.8072 0.9272 0.8739 0.9541 0.8816 0.9775
Tab.1  Kinetic parameters for adsorption of Cr(VI) and Pb(II) onto MNC
Intra-particle C0/(mg·L−1, Cr(VI)) C0/(mg·L−1, Pb(II))
20 40 60 20 60 100
1st stage
?Ki1/(mg·g−1·min−1/2) 22.65 53.54 68.33 6.38 19.62 18.24
?C1 71.23 43.17 31.92 80.31 132.01 165.66
?R12 0.9443 0.9693 0.9767 0.9572 0.9847 0.9502
2nd stage
?Ki2/(mg·g−1·min−1/2) 7.98 × 10−2 1.09 1.23 0.41 0.17 0.19
?C2 184.62 314.54 341.80 124.75 282.45 388.77
?R22 0.9393 0.7817 0.9031 0.7402 0.9711 0.8711
Tab.2  Particle diffusion parameters of MNC in Cr(VI) and Pb(II) solutions
Fig.9  Langmuir and Freundlich adsorption isotherm models of (a) Cr(VI) and (b) Pb(II).
Isothermal models Cr(VI) Pb(II)
298 K 308 K 318 K 298 K 308 K 318 K
Langmuir
?qm/(mg·g−1) 339.65 378.44 442.40 377.02 451.58 535.02
?KL/(L·mg−1) 0.62 0.57 0.32 0.11 0.12 0.07
?R2 0.8853 0.9099 0.7846 0.6138 0.7800 0.4732
Freundlich
?KF/(mg·g−1·mg−n·Ln) 157.74 162.71 173.17 114.65 138.93 192.05
?1/n 0.20 0.23 0.25 0.24 0.24 0.19
?R2 0.9345 0.9579 0.9822 0.9477 0.9759 0.9316
Tab.3  Langmuir and Freundlich adsorption isotherm parameters of MNC
Adsorbates Adsorbents ?qe/(mg·g−1) Ref.
Cr(VI) Fe3O4@Arg-PPy 322.58 [32]
PPy/Fe3O4 nanocomposite 208.77 [33]
Poly(N,N-dimethylaminoethyl methacrylate) 165.00 [34]
A-RS/PVA 140.39 [35]
MNC 456.63 This work
PVA/Chi 266.12 [36]
Pb(II) P(AA-co-MA-co-AAc) cryogel 172.49 [37]
MNPs@SiO2-TSD-TEOS? 417.00 [38]
MNC 507.13 This work
Tab.4  Adsorption capacities of different sorbents for Cr(VI) and Pb(II)
Fig.10  XPS spectra: (a) Cr 2p and (b) N 1s after Cr(VI) adsorption; (c) Pb 4f and (d) O 1s after adsorption of Pb(II); (e) O 1s of MNC.
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