Adsorption performance and physicochemical mechanism of MnO2-polyethylenimine-tannic acid composites for the removal of Cu(II) and Cr(VI) from aqueous solution

doi:10.1007/s11705-020-1958-1

Frontiers of Chemical Science and Engineering

2021, Vol. 15

Issue (3): 538-551 https://doi.org/10.1007/s11705-020-1958-1

本期目录

Adsorption performance and physicochemical mechanism of MnO₂-polyethylenimine-tannic acid composites for the removal of Cu(II) and Cr(VI) from aqueous solution

Xiaoyan Deng¹, Luxing Wang¹, Qihui Xiu², Ying Wang², Hong Han², Dongmei Dai², Yongji Xu², Hongtao Gao²(

), Xien Liu²

¹. College of Environment and Safety Engineering, State Key Laboratory Base of Eco-Chemical Engineering, Qingdao University of Science & Technology, Qingdao 266042, China
². College of Chemistry and Molecular Engineering, State Key Laboratory Base of Eco-Chemical Engineering, Qingdao University of Science & Technology, Qingdao 266042, China

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Abstract：

In this work, an adsorbent, which we call MnPT, was prepared by combining MnO₂, polyethylenimine and tannic acid, and exhibited efficient performance for Cu(II) and Cr(VI) removal from aqueous solution. The oxygen/nitrogen-containing functional groups on the surface of MnPT might increase the enrichment of metal ions by complexation. The maximum adsorption capacities of MnPT for Cu(II) and Cr(VI) were 121.5 and 790.2 mg·g⁻¹, respectively. The surface complexation formation model was used to elucidate the physicochemical interplay in the process of Cu(II) and Cr(VI) co-adsorption on MnPT. Electrostatic force, solvation action, adsorbate–adsorbate lateral interaction, and complexation were involved in the spontaneous adsorption process. Physical electrostatic action was dominant in the initial stage, whereas chemical action was the driving force leading to adsorption equilibrium. It should be noted that after adsorption on the surface of MnPT, Cr(VI) reacted with some reducing functional groups (hydroxylamine-NH₂) and was converted into Cr(III). The adsorption capacity declined by 12% after recycling five times. Understanding the adsorption mechanism might provide a technical basis for the procedural design of heavy metal adsorbents. This MnPT nanocomposite has been proven to be a low-cost, efficient, and promising adsorbent for removing heavy metal ions from wastewater.

Key words： MnO₂-polyethylenimine-tannic acid composite surface complexation formation model Cu(II) Cr(VI) physicochemical mechanism

收稿日期: 2020-02-15 出版日期: 2021-05-10

Corresponding Author(s): Hongtao Gao

引用本文:

. [J]. Frontiers of Chemical Science and Engineering, 2021, 15(3): 538-551.
Xiaoyan Deng, Luxing Wang, Qihui Xiu, Ying Wang, Hong Han, Dongmei Dai, Yongji Xu, Hongtao Gao, Xien Liu. Adsorption performance and physicochemical mechanism of MnO₂-polyethylenimine-tannic acid composites for the removal of Cu(II) and Cr(VI) from aqueous solution. Front. Chem. Sci. Eng., 2021, 15(3): 538-551.

链接本文:

https://academic.hep.com.cn/fcse/CN/10.1007/s11705-020-1958-1
https://academic.hep.com.cn/fcse/CN/Y2021/V15/I3/538

Fig.1

Fig.2

Fig.3

Fig.4

Fig.5

Fig.6

Tab.1

Tab.2

Cu_T/(mg·L^-¹)	Complex	$p K Cu, i s$	$Δ G (ads) i 0$ /(kJ·mol^-¹)	$Δ G (lat) i 0$ /(kJ·mol^-¹)	$Δ G (coul) i 0$ /(kJ·mol^-¹)	$Δ G (solve) i 0$ /(kJ·mol^-¹)	$Δ G (chem) i 0$ /(kJ·mol^-¹)
150	SOCu⁺	−8.20	−46.76	9.26	2.72	8.83	−67.57
125	SOCu⁺	−8.36	−47.73	7.84	2.72	8.83	−67.12
100	SOCu⁺	−8.58	−48.96	6.49	2.72	8.83	−67.00
75	SOCu⁺	−8.86	−50.58	5.04	2.72	8.83	−67.18
50	SOCu⁺	−9.22	−52.59	3.38	2.72	8.83	−67.52
150	SOCu(OH)	−10.97	−62.61	9.34	1.36	8.83	−35.37
125	SOCu(OH)	−11.14	−63.58	7.91	1.36	8.83	−35.47
100	SOCu(OH)	−11.36	−64.83	6.54	1.36	8.83	−36.02
75	SOCu(OH)	−11.65	−66.47	5.09	1.36	8.83	−36.12
50	SOCu(OH)	−12.00	−68.49	3.40	1.36	8.83	−35.10
150	SOCu(OH)₂⁺	−15.60	−88.99	0	0	0	−55.99

Tab.3

$Cr T$ /(mg·L^-¹)	Complex	$p K Cr, i s$	$Δ G (ads) i 0$ /(kJ·mol^-¹)	$Δ G (lat) i 0$ /(kJ·mol^-¹)	$Δ G (coul) i 0$ /(kJ·mol^-¹)	$Δ G (solve) i 0$ /(kJ·mol^-¹)	$Δ G (chem) i 0$ /(kJ·mol^-¹)
150	SHCrO₄	-6.31	-35.99	14.67	-1.36	0.21	-49.50
125	SHCrO₄	-6.47	-36.89	13.19	-1.36	0.21	-48.93
100	SHCrO₄	-6.68	-38.14	11.84	-1.36	0.21	-48.82
75	SHCrO₄	-7.01	-39.97	10.41	-1.36	0.21	-49.23
50	SHCrO₄	-7.47	-42.63	7.82	-1.36	0.21	-49.30
150	SCrO₄⁻	-8.23	-46.98	14.28	-2.72	0.88	-59.43
125	SCrO₄⁻	-8.39	-47.88	12.85	-2.72	0.88	-58.89
100	SCrO₄⁻	-8.60	-49.08	11.53	-2.72	0.88	-58.77
75	SCrO₄⁻	-8.91	-50.86	10.14	-2.72	0.88	-59.16
50	SCrO₄⁻	-9.37	-53.46	7.61	-2.72	0.88	-59.24

Tab.4

Fig.7

Fig.8

Tab.5

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