Electro-conductive crosslinked polyaniline/carbon nanotube nanofiltration membrane for electro-enhanced removal of bisphenol A

doi:10.1007/s11783-023-1659-3

Front. Environ. Sci. Eng.

2023, Vol. 17

Issue (5) : 59 https://doi.org/10.1007/s11783-023-1659-3

RESEARCH ARTICLE

Electro-conductive crosslinked polyaniline/carbon nanotube nanofiltration membrane for electro-enhanced removal of bisphenol A

Haiguang Zhang, Lei Du, Jiajian Xing, Gaoliang Wei, Xie Quan(

)

Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China

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Abstract

● A crosslinked polyaniline/carbon nanotube NF membrane was fabricated.

● Electro-assistance enhanced the removal rate of the NF membrane for bisphenol A.

● Intermittent voltage-assistance can achieve nearly 100% removal of bisphenol A.

● Membrane adsorption–electro-oxidation process is feasible for micropollutant removal.

Nanofiltration (NF) has attracted increasing attention for wastewater treatment and potable water purification. However, the high-efficiency removal of micropollutants by NF membranes is a critical challenge. Owing to the adsorption and subsequent diffusion, some weakly charged or uncharged micropollutants, such as bisphenol A (BPA), can pass through NF membranes, resulting in low removal rates. Herein, an effective strategy is proposed to enhance the BPA removal efficiency of a crosslinked polyaniline/carbon nanotube NF membrane by coupling the membrane with electro-assistance. The membrane exhibited a 31.9% removal rate for 5 mg/L BPA with a permeance of 6.8 L/(m²·h·bar), while the removal rate was significantly improved to 98.1% after applying a voltage of 2.0 V to the membrane. Furthermore, when BPA coexisted with humic acid, the membrane maintained 94% removal of total organic carbon and nearly 100% removal of BPA at 2.0 V over the entire filtration period. Compared to continuous voltage applied to the membrane, an intermittent voltage (2.0 V for 0.5 h with an interval of 3.5 h) could achieve comparable BPA removal efficiency, because of the combined effect of membrane adsorption and subsequent electrochemical oxidation. Density functional theory calculations and BPA oxidation process analyses suggested that BPA was adsorbed by two main interactions: π–π and hydrogen-bond interactions. The adsorbed BPA was further electro-degraded into small organic acids or mineralized to CO₂ and H₂O. This work demonstrates that NF membranes coupled with electro-assistance are feasible for improving the removal of weakly charged or uncharged micropollutants.

Keywords Nanofiltration Membrane Electro-assistance Adsorption Bisphenol A

Corresponding Author(s): Xie Quan

Issue Date: 15 December 2022

Cite this article:

Haiguang Zhang,Lei Du,Jiajian Xing, et al. Electro-conductive crosslinked polyaniline/carbon nanotube nanofiltration membrane for electro-enhanced removal of bisphenol A[J]. Front. Environ. Sci. Eng., 2023, 17(5): 59.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-023-1659-3
https://academic.hep.com.cn/fese/EN/Y2023/V17/I5/59

Fig.1 (a) Low-resolution SEM images of the surface of CPANi/CNT membrane. (b) High-resolution SEM images of the membrane in (a). (c) Photograph of a CPANi/CNT membrane. (d, e) SEM images of the cross-section of CPANi/CNT membrane. (f) TEM images of the CPANi/CNT composite. (g)–(j) show EDS mapping images of the cross-section of CPANi/CNT membrane in (d).

Fig.2 (a) FTIR spectra, (b) XPS spectra and (c) four-probe I–V curves of CNT and CPANi/CNT membranes. The CPANi/CNT membrane was prepared with ANi concentration of 0.2 mol/L. The inset in Fig. 2(c) shows that the CPANi/CNT membrane serves as a connecting conductor in the electric circuit. (d) CV scans (50 cycles) of CNT and CPANi/CNT membranes (the electrolyte was 10 mmol/L Na₂SO₄ solution, scanning rate was 50 mV/s and scanning range was between 0 and 1.6 V vs. SCE).

Fig.3 SEM images of CPANi/CNT membranes prepared with the same CNT loadings but different ANi concentrations of (a) 0.05 mol/L, (b) 0.10 mol/L, (c) 0.20 mol/L and (d) 0.30 mol/L. (e) Electro-conductivity levels of the composite membranes with different ANi concentrations. (f, g) Water permeances and BPA rejection rates of the composite membranes after pre-filtering 5 mg/L BPA feed solution containing 10 mmol/L Na₂SO₄ under 2.0 bar for 2 h. (h) Time variations of BPA rejection rates of the membrane prepared with 0.20 mol/L ANi concentration under 2.0 bar for different feed concentrations of BPA.

Fig.4 (a) BPA removal rates of CPANi/CNT membrane under different voltages (feed: 5 mg/L BPA solution containing 10 mmol/L Na₂SO₄, operation pressure: 2.0 bar). (b) CV curves of the membrane in the absence and presence of BPA (the electrolyte was 10 mmol/L Na₂SO₄ solution and the scanning rate was 50 mV/s). (c) Permeance and BPA removal rate of the membrane at 2.0 V during operation for 10 h. (d) Variation of BPA removal rate of the membrane with and without applied voltages.

Fig.5 Permeation ﬂuxes and BPA removal rates of the membrane at 2.0 V under (a) different transmembrane pressures (5 mg/L BPA solution containing 10 mmol/L Na₂SO₄) and (b) different feed concentrations of BPA (C_0,BPA, operation pressure: 2.0 bar).

Fig.6 (a) TOC removal rates and (b) normalized fluxes of the CPANi/CNT membrane at 0 and 2.0 V as a function of operation time (feed: 100 μg/L BPA solution containing 10 mg/L HA and 10 mmol/L Na₂SO₄, operation pressure: 2.0 bar). (c) Time variation of BPA removal rates at 0 and 2.0 V. (d) Removal rate of BPA by intermittently applying a voltage of 2.0 V. The voltage is applied for 0.5 h and the time interval is 3.5 h; feed: 100 μg/L BPA solution containing 10 mg/L HA and 10 mmol/L Na₂SO₄; operation pressure: 2.0 bar. (e) Stable adsorption configurations of BPA on PANi (i: π–π interactions and ii: hydrogen-bond interactions) and graphitic carbon (iii: π–π interactions and iv: hydrogen-bond interactions). The electron densities are displayed transparently. (f) Schematic diagram of the adsorption–electro-oxidation mechanism for BPA removal.

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