Multi-functional polyethersulfone nanofibrous membranes with ultra-high adsorption capacity and ultra-fast removal rates for dyes and bacteria

doi:10.1016/j.jmst.2020.10.065

Abstract

Abstract:

The adsorption technology has been widely applied in water remediation for contamination removal of dyes and bacteria, by virtue of the advantages of adsorption technology including high efficiency, energy conservation and ease of operation. Simultaneous removal of dyes and bacteria has been realized by some reported materials, but to achieve satisfactory adsorption amounts and rates remain an unmet goal for decades. Herein, a poly(methacrylatoethyl trimethyl ammonium chloride-co-methyl methacrylate) copolymer was synthesized, and then blended with polyethersulfone for the fabrication of nanofibrous membranes via electrospinning for the use of fast and massive removal of dyes and bacteria. Owing to the introduction of abundant quaternary ammonium groups, the maximum adsorption amount for methyl orange was up to 909.8 mg g-1. In addition, the modified nanofibrous membranes showed good recyclability, broad applications in severe environments, selective adsorption ability, and excellent dynamic removal performance. Especially, thanks to the abundant functional groups, the membranes showed fast adsorption ability for bacteria through electrostatic interaction. It should be noted that the clearance ratio for Staphylococcus aureus or Escherichia coli by 6 min of static adsorption could reach 93 % or 90 % for each. Additionally, dynamic removal ratio via filtration with the nanofibrous membranes could reach 99.7 % for Staphylococcus aureus or 98.7 % for Escherichia coli in 90 s. Therefore, the proposed approach towards the quaternary ammonium modified polyethersulfone nanofibrous membranes creates a new route for ultra-high adsorption capacity and ultra-fast removal rates for dyes and bacteria in water remediation.

Key words: Electrospinning, Dye, Bacteria, Water remediation, Nanofibrous membrane

Jianxu Bao, Hang Li, Yuanting Xu, Shengqiu Chen, Zhoujun Wang, Chunji Jiang, Huilin Li, Zhiwei Wei, Shudong Sun, Weifeng Zhao, Changsheng Zhao. Multi-functional polyethersulfone nanofibrous membranes with ultra-high adsorption capacity and ultra-fast removal rates for dyes and bacteria[J]. J. Mater. Sci. Technol., 2021, 78: 131-143.

Figures/Tables 12

Fig. 1. FTIR (A) and XPS (B) of PESM and PQAM; SEM images of PESM (C) and PQAM (D); Nanofibrous diameter distributions of PESM (E) and PQAM (F).

Fig. 2. (A) Adsorption performance of PQAM at different initial MO concentrations; (B) Linear fitting of the pseudo-second-order adsorption model at different initial MO concentrations; The corresponding linear plot for Langmuir model (C) and Freundlich model (D) for MO adsorption process.

Table 1 Pseudo-first-order and pseudo-second-order kinetic model parameters.

C₀(μmol/L)	q_e[exp] (mg/g)	Pseudo-first-order model		Pseudo-second-order model
C₀(μmol/L)	q_e[exp] (mg/g)	q_e[calcu](mg g^-1)	R₁²	q_e[calcu](mg g^-1)	R₂²
1400	845.9	255.6	0.7316	854.7	0.9998
1200	769.6	233.2	0.7916	787.4	0.9999
1000	724.4	215.6	0.8334	719.4	0.9998
800	677.7	154.7	0.5676	680.2	0.9999

Table 2 Langmuir and Freundlich isotherm model parameters.

T (K)	Langmuir isotherm model			Freundlich isotherm model
T (K)	K_L(L mg^-1)	q_max(mg g^-1)	R_L²	n	K_F((mg g^-1)(L mg^-1)^1/ⁿ)	R_F²
298.15	0.1759	826.4	0.9931	5.55	307.12	0.8218
308.15	0.1375	847.5	0.9904	4.71	265.47	0.8478
318.15	0.1267	877.2	0.9883	4.49	260.55	0.8794

Fig. 3. (A) Performance of PQAM during 5 cycles for the desorption/resorption of MO; (B) Static adsorption amounts of PQAM in different pH of MO solutions; and the static adsorption amounts of PQAM for five different dyes (C) and two different toxic heavy metal ions (D).

Fig. 4. (A) Images of selective adsorption of PQAM for MO from MB/MO mixed solution and the chemical structures of MB and MO; (B) UV-vis spectra of MB/MO mixed solution before and after adsorption.

Fig. 5. (A) Dynamic removal performance of PQAM for MO via filtration; (B) UV-vis spectra of MO solution before and after filtration; (C) Dynamic removal performance for 5 filtration-regeneration cycles and (D) selective filtration-separation of PQAM for MO from MB/MO mixed solution.

Fig. 6. (A) Fluorescent images of S. aureus and E. coli after 3 h incubation with PESM and PQAM; (B) The relative proportions of live/dead S. aureus and E. coli on the surface of the prepared membranes; SEM images of S. aureus (C) and E. coli (D) after 3 h incubation with PESM and PQAM.

Fig. 7. Agar plate photographs of S. aureus (A) and E. coli (B) in adsorption experiment; Pseudo-second-order model of S. aureus (C) and E. coli (D) adsorption; (E) Schematic diagram of the adsorption process for bacteria.

Fig. 8. (A) Agar plate photographs of S. aureus and E. coli before and after 3 cycles adsorption-desorption; (B) Clearance ratios for S. aureus and E. coli in 3 cycles; (C) Schematic diagram of the killing, desorbing and recycle process; SEM images of PQAM after adsorption and after desorption for S. aureus (D) and E. coli (E).

Fig. 9. Agar plate photographs of PESM (A) and PQAM (B) for S. aureus and E. coli before and after filtration; (C) Clearance ratios of dynamic removal for bacteria via filtration; SEM images of PESM and PQAM after filtration for S. aureus (D) and E. coli (E).

Table 3 Comparisons of equilibrium time and adsorption capacities toward dyes, as well as antibacterial effects through various electrospun nanofibrous membranes.

Adsorbents	Dyes		Bacteria			Refs
Adsorbents	t_e (min)	q_max (mg g^-1)	t_e (min)	Adsorption ratio (%)	Killing ratio (%)	Refs
Chitosan/MgO composite	30	90 (MO)	1440	-	93(E. coli)	[42]
Polyaniline/Guar gum/acrylic acid hydrogel	240	-	-	-	Efficient for E. coli and S. aureus	[44]
Polyurethane/ graphene oxide NFM	60	109 (MB)	-	-	Efficient for E. coli and S. aureus	[45]
Polyacrylonitrile/ polyetherimide/Fe NFM	180	77.5 (CR)	480	-	90(E. coli) 99(S. aureus)	[29]
Quaternary ammonium modified cellulose mats	180	694 (CR)	240	-	99.9(E. coli) 99(S. aureus)	[43]
Graphene oxide foams	640	446 (RB)	300	-	Efficient for S. aureus	[46]
CuO-ZnO composite nanofibers	1440	126 (CR)	720	-	Efficient for E. coli and S. aureus	[30]
In-situ crosslinked quaternary ammonium NFM	360	208 (CR)	720	-	99(E. coli) 99(S. aureus)	[31]
Quaternary ammonium modified polyethersulfone NFM	50	909 (MO)	20	99(E. coli and S. aureus)	96(E. coli) 88(S. aureus)	This work

References 46

[1]	R.P. Schwarzenbach, T. Egli, T.B. Hofstetter, U. von Gunten, B. Wehrli, Annu. Rev. Env. Resour. 35(2010) 109-136. DOI URL
[2]	A. Birhanlı, M.J.D. Ozmen, Drug Chem. Toxicol. 28(2005) 51-65.
[3]	K.S. Kim, Lancet Infect. Dis. 10(2010) 32-42. DOI URL
[4]	H.F. Wertheim, H.N. Nguyen, W. Taylor, T.T. Lien, H.T. Ngo, T.Q. Nguyen, B.N. Nguyen, H.H. Nguyen, H.M. Nguyen, C.T. Nguyen, T.T. Dao, T.V. Nguyen, A. Fox, J. Farrar, C. Schultsz, H.D. Nguyen, K.V. Nguyen, P. Horby, PLoS One 4(2009) e5973. DOI URL
[5]	Y. Xu, D. Yuan, J. Bao, Y. Xie, M. He, Z. Shi, S. Chen, C. He, W. Zhao, C. Zhao, J. Mater. Chem. A 6(2018) 13359-13372. DOI URL
[6]	Y. Xu, J. Bao, X. Zhang, W. Li, Y. Xie, S. Sun, W. Zhao, C. Zhao, J. Colloid Interface Sci. 533(2019) 526-538. DOI URL
[7]	Y. Xing, J. Cheng, J. Wu, M. Zhang, X.A. Li, W. Pan, J. Mater. Sci. Technol. 45(2020) 84-91. DOI URL
[8]	S. Zhao, Z. Wang, J. Membr. Sci. 524(2017) 214-224. DOI URL
[9]	J. Lin, W. Ye, H. Zeng, H. Yang, J. Shen, S. Darvishmanesh, P. Luis, A. Sotto, B. Van der Bruggen, J.Membr. Sci. 477(2015) 183-193.
[10]	J.B. Tarkwa, N. Oturan, E. Acayanka, S. Laminsi, M.A. Oturan, Environ. Chem. Lett. 17(2018) 473-479. DOI URL
[11]	K. Rajeshwar, M.E. Osugi, W. Chanmanee, C.R. Chenthamarakshan, M.V.B. Zanoni, P. Kajitvichyanukul, R. Krishnan-Ayer, J. Photochem. Photobiol. C 9(2008) 171-192. DOI URL
[12]	Z. Jia, L.B.T. La, W.C. Zhang, S.X. Liang, B. Jiang, S.K. Xie, D. Habibi, L.C. Zhang, J. Mater. Sci. Technol. 33(2017) 856-863. DOI URL
[13]	Y. Xu, W. Lin, H. Wang, J. Guo, D. Yuan, J. Bao, S. Sun, W. Zhao, C. Zhao, Compos. Sci. Technol. 199(2020), 108353.
[14]	E. Brillas, C.A. Martínez-Huitle, Appl. Catal.B 166-167(2015) 603-643. DOI URL
[15]	M. Sala, M.C. Gutiérrez-Bouzán, Int. J. Photoenergy 2012 (2012) 1-12.
[16]	W.W. Wilson, M.M. Wade, S.C. Holman, F.R.J.J. Champlin, J. Microbiol. Methods 43(2001) 153-164. DOI URL
[17]	J. Malakootikhah, A.H. Rezayan, B. Negahdari, S. Nasseri, H. Rastegar, Carbohydr. Polym. 170(2017) 190-197. DOI PMID
[18]	M.J. Sharrer, S.T. Summerfelt, G.L. Bullock, L.E. Gleason, J. Taeuber, Aquacult. Eng. 33(2005) 135-149. DOI URL
[19]	X. Wang, X. Hu, H. Wang, C. Hu, Water Res. 46(2012) 1225-1232. DOI URL
[20]	M. Florjanic, J. Kristl, Drug Dev. Ind. Pharm. 32(2006) 1113-1121. PMID
[21]	M.T. Yagub, T.K. Sen, S. Afroze, H.M. Ang, Adv. Colloid Interface Sci. 209(2014) 172-184. DOI URL
[22]	Y. Liao, C.H. Loh, M. Tian, R. Wang, A.G. Fane, Prog. Polym. Sci. 77(2018) 69-94. DOI URL
[23]	J. Xue, T. Wu, Y. Dai, Y. Xia, Chem. Rev. 119(2019) 5298-5415. DOI URL
[24]	M. Zhang, W. Ma, J. Cui, S. Wu, J. Han, Y. Zou, C. Huang, J. Hazard. Mater. 383(2020), 121152.
[25]	J. Cui, F. Li, Y. Wang, Q. Zhang, W. Ma, C. Huang, Sep. Purif. Technol. 250(2020), 117116.
[26]	J. Shen, Z. Li, Y.N. Wu, B. Zhang, F. Li, Chem. Eng. J. 264(2015) 48-55. DOI URL
[27]	W. Ma, Y. Li, S. Gao, J. Cui, Q. Qu, Y. Wang, C. Huang, G. Fu, ACS Appl. Mater. Interfaces 12(2020) 23644-23654. DOI URL
[28]	B. Shen, D. Zhang, Y. Wei, Z. Zhao, X. Ma, X. Zhao, S. Wang, W. Yang, Polymers (Basel) 11(2019) 1511.
[29]	R.K. Sadasivam, S. Mohiyuddin, G. Packirisamy, ACS Omega 2(2017) 6556-6569. DOI PMID
[30]	D. Malwal, P. Gopinath, J. Hazard. Mater. 321(2017) 611-621. DOI URL
[31]	C. Lv, S. Chen, Y. Xie, Z. Wei, L. Chen, J. Bao, C. He, W. Zhao, S. Sun, C. Zhao, J. Colloid Interface Sci. 556(2019) 492-502. DOI URL
[32]	H. Deng, Y. Xu, Q. Chen, X. Wei, B. Zhu, J. Membr. Sci. 366(2011) 363-372. DOI URL
[33]	L. Zhang, M. Tang, J. Zhang, P. Zhang, J. Zhang, L. Deng, C. Lin, A. Dong, J. Appl. Polym. Sci. 134(2017) 44632.
[34]	B. Cramariuc, R. Cramariuc, R. Scarlet, L.R. Manea, I.G. Lupu, O. Cramariuc, J. Electrostatics 71(2013) 189-198. DOI URL
[35]	F.C. Wu, R.L. Tseng, S.C. Huang, R.S. Juang, Chem. Eng. J. 151(2009) 1-9. DOI URL
[36]	H. Moussout, H. Ahlafi, M. Aazza, H. Maghat, Int. J. Modern Sci. 4(2018) 244-254.
[37]	É.C. Lima, M.A. Adebayo, F.M. Machado, Kinetic and Equilibrium Models of Adsorption, Carbon Nanomaterials As Adsorbents for Environmental and Biological Applications,Springer, 2015, pp. 33-69.
[38]	T. Xu, H. Li, C. He, H. Xu, X. Song, H. Ji, C. Zhao, J. Environ. Chem. Eng. 7(2019), 103393.
[39]	X. Song, T. Xu, L. Yang, Y. Li, Y. Yang, L. Jin, J. Zhang, R. Zhong, S. Sun, W.J.B. Zhao, Biomacromolecules 21(2020) 1762-1775. DOI PMID
[40]	B. Satilmis, T. Uyar, Appl. Surf. Sci. 453(2018) 220-229. DOI URL
[41]	E.F.C. Chaúque, L.N. Dlamini, A.A. Adelodun, C.J. Greyling, J.C. Ngila, Phys. Chem. Earth 100(2017) 201-211. DOI URL
[42]	Y. Haldorai, J.J. Shim, Appl. Surf. Sci. 292(2014) 447-453. DOI URL
[43]	Y. Hu, F. Liu, Y. Sun, X. Xu, X. Chen, B. Pan, D. Sun, J. Qian, Chem. Eng. J. 371(2019) 730-737. DOI URL
[44]	R. Sharma, B.S. Kaith, S. Kalia, D. Pathania, A. Kumar, N. Sharma, R.M. Street, C. Schauer, J. Environ. Manage 162(2015) 37-45. DOI URL
[45]	S.P. Sundaran, C.R. Reshmi, P. Sagitha, O. Manaf, A. Sujith, J. Environ. Manag. 240(2019) 494-503. DOI URL
[46]	S. Jayanthi, N. KrishnaRao Eswar, S.A. Singh, K. Chatterjee, G. Madras, A.K. Sood, RSC Adv. 6(2016) 1231-1242.