Enhanced adsorptive removal of Cr(VI) in aqueous solution by polyethyleneimine modified palygorskite

doi:10.1016/j.cjche.2020.03.019

Abstract

Abstract: Polyethyleneimine (PEI) modified palygorskite (Pal) was used for the adsorption of Cr(VI) in aqueous solution. The absorbent was characterized by Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TGA). Characterized results confirmed that the Pal has been successfully modified by PEI. The modification of PEI increased the Cr(VI) adsorption performance of the Pal by the adsorption combined reduction mechanism, and amino groups of the adsorbent play the main role in the enhanced Cr(VI) adsorption. The maximum adsorption capacity was 51.10 mg·g^-1 at pH 4.0 and 25 ℃. The adsorption kinetics of Cr(VI) on the adsorbent conforms to the Langmuir isotherm model. The maximum adsorption occurs at pH 3, and then the adsorption capacity of PEI-Pal was decreased with the increase of pH values. The adsorption kinetics of Cr(VI) on PEI-Pal was modeled with pseudo-second-order model. The addition of Cl^-, SO₄^2- and PO₄^3- reduced the Cr(VI) adsorption by competition with Cr(VI) for the active sites of PEI-Pal. The Cr(VI) saturated PEI-Pal can be regenerated in alkaline solution, and the adsorption capacity can still be maintained at 30.44 mg·g^-1 after 4 cycles. The results demonstrate that PEI-Pal can be used as a potential adsorbent of Cr(VI) in aqueous solutions.

Key words: Palygorskite, Polyethyleneimine, Adsorption, Cr(VI)

摘要： Polyethyleneimine (PEI) modified palygorskite (Pal) was used for the adsorption of Cr(VI) in aqueous solution. The absorbent was characterized by Fourier transform infrared spectroscopy (FT-IR) and thermogravimetric analysis (TGA). Characterized results confirmed that the Pal has been successfully modified by PEI. The modification of PEI increased the Cr(VI) adsorption performance of the Pal by the adsorption combined reduction mechanism, and amino groups of the adsorbent play the main role in the enhanced Cr(VI) adsorption. The maximum adsorption capacity was 51.10 mg·g^-1 at pH 4.0 and 25 ℃. The adsorption kinetics of Cr(VI) on the adsorbent conforms to the Langmuir isotherm model. The maximum adsorption occurs at pH 3, and then the adsorption capacity of PEI-Pal was decreased with the increase of pH values. The adsorption kinetics of Cr(VI) on PEI-Pal was modeled with pseudo-second-order model. The addition of Cl^-, SO₄^2- and PO₄^3- reduced the Cr(VI) adsorption by competition with Cr(VI) for the active sites of PEI-Pal. The Cr(VI) saturated PEI-Pal can be regenerated in alkaline solution, and the adsorption capacity can still be maintained at 30.44 mg·g^-1 after 4 cycles. The results demonstrate that PEI-Pal can be used as a potential adsorbent of Cr(VI) in aqueous solutions.

关键词: Palygorskite, Polyethyleneimine, Adsorption, Cr(VI)

Jiahong Wang, Tongtong Sun, Atif Saleem, Yao Chen. Enhanced adsorptive removal of Cr(VI) in aqueous solution by polyethyleneimine modified palygorskite[J]. Chinese Journal of Chemical Engineering, 2020, 28(10): 2650-2657.

Jiahong Wang, Tongtong Sun, Atif Saleem, Yao Chen. Enhanced adsorptive removal of Cr(VI) in aqueous solution by polyethyleneimine modified palygorskite[J]. 中国化学工程学报, 2020, 28(10): 2650-2657.

References

[1] R. Yu, Y. Shi, D. Yang, Y. Liu, J. Qu, Z. Yu, Graphene oxide/chitosan aerogel microspheres with honeycomb-cobweb and radially oriented microchannel structures for broad-spectrum and rapid adsorption of water contaminants, ACS Appl. Mater. Interfaces 9(2017) 21809-21819.
[2] V. Gopalakannan, N. Viswanathan, Development of nano-hydroxyapatite embedded gelatin biocomposite for effective Cr(VI) removal, Ind. Eng. Chem. Res. 54(2015) 12561-12569.
[3] J. Wu, H. Zhang, P. He, Q. Yao, L. Shao, Cr(VI) removal from aqueous solution by dried activated sludge biomass, J. Hazard. Mater. 176(2010) 697-703.
[4] D. Park, Y. Yun, D. Lee, J. Park, Optimum condition for the removal of Cr(VI) or total Cr using dried leaves of Pinus densiflora, Desalination. 271(2011) (2011) 309-314.
[5] F. Fu, W. Han, Z. Cheng, T. Bing, Removal of hexavalent chromium from wastewater by acid-washed zero-valent aluminum, Desalin. Water Treat. 57(2016) 5592-5600.
[6] H. Altundogan, Cr(VI) removal from aqueous solution by iron (III) hydroxide-loaded sugar beet pulp, Process Biochem. 40(2004) 1443-1452.
[7] M. Yue, M. Zhang, B. Liu, X. Xu, X. Li, Q. Yue, Characteristics of amine surfactant modified peanut shell and its sorption property for Cr(VI), Chin. J. Chem. Eng. 21(2013) 1260-1268.
[8] M. Singh, Heavy metal pollution in freshly deposited sediments of the Yamuna River (the Ganges River tributary):A case study from Delhi and Agra urban centres, India, Environ. Geol. 40(2001) 664-671.
[9] C. Namasivayam, M. Sureshkumar, Removal of chromium(VI) from water and wastewater using surfactant modified coconut coir pith as a biosorbent, Bioresour. Technol. 99(2008) 2218-2225.
[10] B. Xie, S. Chao, X. Zhe, X. Li, X. Zhang, J. Chen, B. Pan, One-step removal of Cr(VI) at alkaline pH by UV/sulfiteprocess:Reduction to Cr(III) and in situ Cr(III) precipitation, Chem. Eng. J. 308(2017) 791-797.
[11] Y. Yao, Q. Wei, M. Sun, Y. Chen, X. Ren, Environmentally friendly chromium electrodeposition:Effect of pre-electrolysis on a Cr(III) bath in an anion-exchange membrane reactor, RSC Adv. 3(2013) 13131-13136.
[12] S. Das, P. Chakraborty, R. Ghosh, S. Paul, S. Mondal, A. Panja, A. Nandi, Folic acidpolyaniline hybrid hydrogel for adsorption/reduction of chromium(VI) and selective adsorption of anionic dye from water, ACS Sustainable Chem. Eng. 5(2017) 9325-9337.
[13] L. Melita, M. Popescu, Removal of Cr (VI) from industrial water effluents and surface waters using activated composite membranes, J. Membr. Sci. 312(2008) 157-162.
[14] A. Yavuz, E. Dincturk-Atalay, A. Uygun, F. Gode, E. Aslan, A comparison study of adsorption of Cr(VI) from aqueous solutions onto alkyl-substituted polyaniline/chitosan composites, Desalination. 279(2011) 325-331.
[15] L. Yan, J. Wang, H. Yu, Q. Wei, B. Du, X. Shan, Adsorption of benzoic acid by CTAB exchanged montmorillonite, Appl. Clay Sci. 37(2007) 226-230.
[16] Y. Xie, D. Shao, X. Lu, T. Hayat, N. Alharbi, C. Chen, G. Song, D. Chen, Y. Sun, Spectroscopic investigation of enhanced adsorption of U(VI) and Eu(III) on magnetic attapulgite in binary system, Ind. Eng. Chem. Res. 57(2018) 7533-7543.
[17] K. Bhattacharyya, S. Gupta, Adsorption of chromium(VI) from water by clays, Ind. Eng. Chem. Res. 45(2006) 7232-7240.
[18] Y. Ling, J. Zhang, Chelate regulatory ζ-potentials of montmorillonite and its adsorption capacity for Cr(III), Chem. J. Chin. Univ. 30(2009) 2478-2483.
[19] Y. Wang, Y. Feng, X. Zhang, X. Zhang, J. Jiang, J. Yao, Alginate-based attapulgite foams as efficient and recyclable adsorbents for the removal of heavy metals, J. Colloid Interf. Sci. 514(2017) 190-198.
[20] F. Ying, D. Chen, A novel catalyst of Fe-octacarboxylic acid phthalocyanine supported by attapulgite for degradation of Rhodamine B, Mater. Res. Bull. 45(2010) 1728-1731.
[21] J. Huang, X. Wang, Q. Jin, Y. Li, Y. Wang, Removal of phenol from aqueous solution by adsorption onto OTMAC-modified attapulgite, J. Environ. Manag. 84(2007) 229-236.
[22] L. Peng, L. Jiang, L. Zhu, A. Wang, Attapulgite/poly(acrylic acid) nanocomposite (ATP/PAA) hydrogels with multifunctionalized attapulgite (org-ATP) nanorods as unique cross-linker:Preparation optimization and selective adsorption of Pb(II) ion, ACS Sustainable Chem. Eng. 2(2014) 269-271.
[23] B. Yuan, X. Yin, X. Liu, X. Li, L. Sun, Enhanced hydrothermal stability and catalytic performance of hkust-1 by incorporating carboxyl-functionalized attapulgite, ACS Appl. Mater. Interfaces 8(2016) (2016) 16457-16464.
[24] X. Li, Y. Jiang, X. Liu, L. Shi, D. Zhang, L. Sun, Direct synthesis of zeolites from a natural clay, attapulgite, ACS Sustainable Chem. Eng. 5(2017) 6124-6130.
[25] H. Chen, Y. Zhao, A. Wang, Removal of cu(II) from aqueous solution by adsorption onto acid-activated palygorskite, J. Hazard. Mater. 149(2007) 346-354.
[26] J. Zhang, Q. Wang, A. Wang, Synthesis and characterization of chitosan-g-poly (acrylic acid)/attapulgite superabsorbent composites, Carbohydr. Polym. 68(2007) 367-374.
[27] L. Chen, H. Liang, Y. Lu, C. Cui, S. Yu, Synthesis of an attapulgite clay@carbon nanocomposite adsorbent by a hydrothermal carbonization process and their application in the removal of toxic metal ions from water, Langmiur. 27(2011) 8998-9004.
[28] B. Li, W. Li, Q. Zhang, W. Weng, H. Wan, Attapulgite as natural catalyst for glucose isomerization to fructose in water, Catal. Commun. 99(2017) 20-24.
[29] K. Doke, E. Khan, Equilibrium, kinetic and diffusion mechanism of Cr(VI) adsorption onto activated carbon derived from wood apple shell, Arab. J. Chem. 10(2017) S252-S260.
[30] Y. Chen, H. Xu, S. Wang, L. Kang, Removal of Cr(VI) from water using polypyrrole/attapulgite core-shell nanocomposites:Equilibrium, thermodynamics and kinetics, RSC Adv. 4(2014) 17805-17811.
[31] H. Lu, H. Lu, Y. Chen, ZVI/PANI/ATP composite by static polymerization as adsorbent for removal of Cr(VI), RSC Adv. 4(2014) 5873-5879.
[32] Z. Yang, B. Wang, L. Chai, Removal of Cr(III) and Cr(VI) from aqueous solution by adsorption on sugarcane pulp residue, J. Cent. S. Univ. Technol. 16(2009) 101-107.
[33] X. Zhang, L. Lv, Y. Qin, M. Xu, X. Jia, Z. Chen, Removal of aqueous Cr(VI) by a magnetic biochar derived from Melia azedarach wood, Bioresour. Technol. 256(2018) 1-10.
[34] W. Zhu, Q. Dang, C. Liu, D. Yu, G. Chang, X. Pu, Q. Wang, Cr(VI) and Pb(II) capture on pH-responsive polyethyleneimine and chloroacetic acid functionalized chitosan microspheres, Carbohydr. Polym. 219(2019) 353-367.
[35] X. Feng, C. Liang, J. Yu, X. Jiang, Facile fabrication of graphene oxidepolyethylenimine composite and its application for the Cr(VI) removal, Sep. Sci. Technol. 53(2018) 2376-2387.
[36] B. Qiu, J. Guo, X. Zhang, D. Sun, H. GU, Q. Wang, H. Wang, X. Wang, X. Zhang, B. Weeks, Z. Guo, S. Wei, Polyethylenimine facilitated ethyl cellulose for hexavalent chromium removal with a wide pH range, ACS Appl. Mater. Interfaces 6(2014) 19816-19824.
[37] S. Deng, Y. Ting, Polyethylenimine-modified fungal biomass as a high-capacity biosorbent for Cr(VI) anions:Sorption capacity and uptake mechanisms, Environ. Sci. Technol. 39(2005) 8490-8496.
[38] Y. Xing, X. Chen, D. Wang, Electrically regenerated ion exchange for removal and recovery of Cr(VI) from wastewater, Environ. Sci. Technol. 41(2007) 1439-1443.
[39] Y. Ho, Removal of copper ions from aqueous solution by tree fern, Water Res. 37(2013) 2323-2330.
[40] C. Li, T. Zhou, H. Jin, Y. Lian, W. Han, Effective adsorption/reduction of Cr(VI) oxyanion by halloysite@polyaniline hybrid nanotubes, ACS Appl. Mater. Interfaces 9(2017) 6030-6043.
[41] D. Zhao, H. Zhu, C. Wu, S. Feng, A. Alsaedi, T. Hayat, Facile synthesis of magnetic Fe₃O₄/graphene composites for enhanced U(VI) sorption, Appl. Surf. Sci. 444(2018) 691-698.