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ISSN : 1226-0088(Print)
ISSN : 2288-7253(Online)
Membrane Journal Vol.32 No.4 pp.227-234
DOI : https://doi.org/10.14579/MEMBRANE_JOURNAL.2022.32.4.227

Recent Progress in Zeolite Membrane for Wastewater Treatment: A Review

Joo Yeop Lee*, Rajkumar Patel**†
*Nano Science and Engineering, Underwood International College, Yonsei University, Incheon 21983, South Korea
**Energy and Environmental Science and Engineering, Integrated Science and Engineering Division, Underwood International College, Yonsei University, Incheon 21983, South Korea
†Corresponding author(e-mail: rajkumar@yonsei.ac.kr; http://orcid.org/0000-0002-3820-141X)
August 11, 2022 ; ; August 25, 2022

Abstract


Wastewater is released from leather, textile, paint, wood, or dye processing industries as well as petroleum refining industries. Wastewater from these industries contains water pollutant such as heavy metals and nitrogen compounds and has high chemical oxygen demand (COD). While there various filtering pollutants from wastewater for safe disposal, membrane-based technology is one of the most efficient methods for its high efficiency and low cost. Among various membranes, zeolite membranes gain spotlight for its cost-effectiveness and have undergone a lot of research. This review is focused on recent progress in zeolite membrane for wastewater treatment in following order: i) wastewater treatment, ii) microfiltration membrane, iii) hollow fiber membrane, and iv) ultrafiltration membrane.


ultrafiltration , microfiltration , hollow fiber membrane , wastewater , heavy metal ion

폐수처리를 위한 제올라이트 막의 최근 연구에 대한 총설

이 주 엽*, 라즈쿠마 파텔**†
*연세대학교 언더우드학부 융합과학공학부 나노과학공학
**연세대학교 언더우드학부 융합과학공학부 에너지환경융합전공

초록


폐수는 석유 정제 산업에서만 방출되는 것이 아니고 아니라 가죽, 섬유, 페인트, 목재, 염료 가공 산업에서 또한 방출된다. 이런 산업 폐수는 중금속과 질소화합물 등 수질오염물질을 포함하고 있으며 화학적 산소요구량(COD)이 높다. 안 전한 처리를 위해 폐수에서 각종 오염물질을 걸러내는 방식이 있지만 막 기반 기술은 고효율, 저비용으로 가장 효율적인 방 법 중 하나이다. 다양한 막 중에서, 제올라이트 막은 가성비로 주목을 받고 있으며 많은 연구를 거쳤다. 본 리뷰논문은 i) 폐 수처리, ii) 미세여과막, iii) 중공사막, iv) 초여과막의 순서로 폐수처리를 위한 제올라이트 막의 최근 진척을 중점으로 다루고 있다.


    1. Introduction

    Water pollution is happening all over the world due to inflow of heavy metals and nitrogen compounds and increase in COD[1-9]. These pollutants came mostly from industries that process leather, textile, paint, wood, and dye as well as petroleum refining industries. Therefore, for the sake of both human health and ecological system, this wastewater full of organic and inorganic pollutants need to be treated before discharged into water source. Among the wastewater treatment techniques, treatments that utilize zeolite membranes became hotspot of researching.

    The conventional methods of removing pollutants, especially heavy metals, are normally chemical precipitation, ion-exchange, and electrochemical deposition [10-11]. These methods inevitably generate some problems such as excessive toxic sludge production, lack of quality, and high energy requirements caused by their purification process. However, unlike the conventional methods, membrane separation technology is cost effectiveness and has high separation capability and energy efficiency. Therefore, zeolite membranes play an important role in water purification applications.

    Since zeolite membranes were found to be a great material for the wastewater treatment, there had been a lot of research conducted on improving the membrane performance and durability and broadening the application[ 12-13]. Some trials applied the zeolite membranes into microfiltration or ultrafiltration or made use of hallow fiber support to improve the efficiency of the membranes. This review classifies the recent progress in zeolite membrane for wastewater treatment into four categories; wastewater treatment, microfiltration, hallow fiber, and ultrafiltration which is represented in Fig. 1.

    2. Wastewater Treatment

    High-performance mixed matrix membrane (MMMs) with polysulfone (PSf) matrix and two nanofillers, UiO-66 and Zeolite 4A was fabricated by Anjum et al. [14] (Figs. 2 and 3). MMMs has either UiO-66 or Zeolite 4A as a nanofiller or both and each type of MMMs has different weight percent. Among three types of MMMs, PSf/Zeolite 4A-UiO-66 membrane is unique since it is the first MMM that uses both UiO-66 and Zeolite 4A to get a synergy effect. The effects of nanofillers were examined with the criteria such as water flux, antifouling properties and rejection. Scanning Electron Microscopy (SEM) was used to analyze the effect of nanofiller loadings on possessing wider macrovoids in the membranes. While MMMs with single nanofiller have higher pure water flux but also have tradeoff between permeability and selectivity, MMMs with combined nanofillers (PSf/Zeolite 4A-UiO-66) does not have the tradeoff. Among the combined nanofiller membranes, PSf/Zeolite 4A-UiO-66 (0.5 wt%) have the best antifouling properties. Improve in flux recovery was observed in all MMMs with 0.5 and 1 wt% nanofiller loadings.

    Chang et al. studied about hazardous metal-plating wastewater treatment by using a ceramic membrane consisting of aluminum oxide as support and top layer have a pore size of 0.1 μm[15].

    They put the alumina membrane into a fluidized membrane reactor to improve antifouling property and contaminants removal behaviour. This fluidized membrane reactor fluidizes the granular activated carbon (GAC) particles along the surface of membrane by circulation of wastewater in the reactor. The pH of wastewater determined membrane fouling when there is no media. Neutral pH enabled the deposit of agglomerated particles and colloidal materials on membrane surface, which resulted high fouling rate. However, this fouling layer is not a flaw since it acts as a secondary membrane that enhanced heavy metal ions removal. COD (chemical oxygen demand) removal efficiency was low regardless of the pH. Membrane fouling reduced dramatically with the addition of media, and COD removal efficiency reached 90% with 10% dosage of GAC in the fluidized membrane reactor. Moreover, more than 90% of heavy metals were removed when GAC is used. To evaluate the membrane performance, zeolite particle was researched and it showed that GAC is better for the treatment of wastewater from metal plating in membrane reactor.

    Zeolite-based systems for removing organic contaminants from wastewater to protect aquatic organisms have drawbacks of sinking in water and saturated adsorption site[16]. Nijpanich et al. prepared TiO2/pure silica MFI-type zeolite(PSZ)- hollow glass microspheres (HGMs), a tri-layer floating photocatalyst/adsorbent system, by growth of PSZ crystal to crystallize hydrophobic silicalite-1 on HGMs and then using impregnations to deposit anatase–rutile TiO2 nanoparticles on PSZ-HGM. The hybrid material exhibit excellent photcatalytic against methylene blue (MB) with 98% removal efficiency within 2 h. A mordenite framework inverted (MFI) type zeolite membrane was fabricated by Kumar et al. from cheap tubular ceramic substrate by a hydrothermal process and its performance of removing chromium from synthetic wastewater was evaluated[ 17] (Fig. 4 & 5).

    To prepare uniform MFI zeolite membrane, ceramic substrate was layered with zeolite. As MFI zeolite layer was deposited the porosity decreased from 53% to 51%. Compared to the substrate, the membrane has lower pore size and water permeability, which are 0.272 μm and 4.43 × 10–7 m3/m2s.kPa, respectively. When feed solution with concentration of 1000 ppm was passed through the membrane under 345 kPa pressure, permeate flux was 1.42 × 10–4 m3/m2s with 78% chromium removal.

    3. Microfiltration Membrane

    Jamieson et al. reported on the impact of the four acid components present in the wastewater of the International Space Station (ISS) on Linde Type A (LTA) zeolites to determine whether LTA zeolites are applicable in membrane separations to produce potable water[18].

    The four acid-producing components are chromium (VI) oxide, phosphate of sodium and potassium and sulfuric acid. Composition and morphology of the LTA zeolites were analyzed after exposure to synthetic wastewater. Phosphate solutions degraded the crystal lattice of the zeolite particles completely when its pH is below 5, while the other acid-type solutions need to have pH lower than 1 to degrade completely. It was found out that acidic anions are more important in degradation of LTA zeolites rather than pH. Additionally, they found dihydrogen phosphate anions special since they catalyze aluminum and silicon removal and cause degradation of zeolites in phosphate solutions. Fouling behaviors of the integrated anaerobic fluidized bed membrane bioreactor (AFMBR)-with zeolite column working in RO process and anoxic-aerobic MBR-RO systems for treatment of wastewater was investigated. Li et al. found that removal efficiency of organic content is more than 95%[19]. However, when it comes to total nitrogen (TN) removal, efficiency of the membrane is very less which is 57% for anoxic- aerobic MBR, and just 9% in the AFMBR. Membrane performance of AFMBR is better with lower energy consumption due to liquid-fluidized GAC particles effect on membrane. Over 95% ammonium removed from AFMBR permeate by zeolite column to ensure level of organic and nitrogen percent in RO feed in both process.

    4. Hollow Fiber Membrane

    Hollow fiber membrane made up of Al2O3-NaA zeolite were synthesized by a two-step hydrothermal synthesis to both recycle coal fly ash and remove lead ions in wastewater[20]. Zhu et al. used fly ash and solid waste, as precursor to fabricate NaA zeolite membrane layer with about 6.0 mm thick on the inner wall of Al2O3 hollow fiber support. SEM measurement showed that the pore size of the zeolite membrane was about 0.41 nm in diameter. After 12 hours of filtrating synthetic wastewater under 0.1 MPa of applied pressure, it was found that the Pb(II) removal efficiency reached 99.9% with permeation flux of about 670 L.m-2/h. Lignin is abundant in the wastewater of the papermaking process in hybrid coal fabrication, whose combustion does not corrode the generator and minimum amount of fly ash generation[21]. Metal ions must be removed in the lignin wastewater. Zhuang et al. investigated the performance of alumina hollow fiber membrane deposited with K-Phillipsite (K-PHI) zeolite to remove metal ions by ion exchange. Alumina hollow fiber membrane, the support, prepared by the nonsolvent induced phase separation (NIPS) method. K-PHI seeds was prepared hydrothermal synthesis, seeded them on the support, and deposited them by hydrothermal synthesis. Inductively Coupled Plasma Optical Emission Spectrometer (ICP-OES) was used to measure the change in the concentration of metal ions after ion exchange. It was found that 86 mg/kg of K+ and 54.9 mg/kg of Na+ were extracted. In other words, 71.0% of K+ ions and 27.2% of Na+ ions were removed. K-PHI zeolite membrane can be utilized in removing potassium and sodium ions from the acidic lignin wastewater.

    5. Ultrafiltration Membrane

    New but low-cost ultrafiltration (UF) ceramic membranes were prepared by Aloulou et al. from smectite nanoparticles by sol-gel process its performance against electroplating industry wastewater was evaluated[22]. They fabricated four different membranes, Sm/Z4, Sm/Z5, Sm/Z6, and Sm/Z7 via the Layer-by-Layer technique on tubular microporous supports made up of natural zeolite. The membranes at an optimal temperature of 900°C and pore diameters ranges are over all from 3~21 nm. A cross-flow UF pilot plant was made and trans-membrane pressure range from 3 to 7 bar to evaluate the efficiency of removing heavy metal. Pure water permeabilities are 73 L/h m2 bar for Sm/Z4, and 95 L/h m2 bar for Sm/Z7, which are far less than 1218 L/h m2 bar for the ordinary zeolite support. It was found that Sm/Z6 showed the best performance of 59 L/h m2 permeate flux at a pressure of 3 bar. Ivan et al. fabricated the composite polyaniline-zeolite membrane material for wastewater treatment containing a complex composition of lead, copper and zinc ions as well as phenolic derivatives like phenol, aminophenols or nitrophenols from textile and leather industries[23]. Membrane was synthesized by polymerizing aniline on synthetic zeolite matrices and analyzed by various methods. It was found that both phenol retention and cations retention are enhanced when PANI-Zeolite is used compared to when either polyaniline or zeolite is used alone. Removal of metal ion from industrial wastewater by sorbent assisted UF process was investigated by Katsou et al.[24]. It was found that metals were removed mainly through four processes in this system: i) hydroxide was formed during precipitation ii) adsorption of metals onto zeolite and iii) metal ions are retained by the UF membranes. It was found metal ions can be effectively retained by the UF membranes at pH 9. At pH 6 removal of metal ion takes place. Excellent removal of lead and copper ion is due to the precipitation and complexation with compounds in wastewater. UF membrane prepared from natural aluminosilicate minerals were used to remove nickel ions from solutions and sludge[25]. Natural minerals at pH 6 showed good removal efficiency by sorption process. The film diffusion is dominated at the early stages of the process, but intraparticle diffusion dominated the later stages. Adsorption isotherm at equilibrium of mineral follows Langmuir model but sludge follows Freundlich model.

    6. Conclusions

    Growing global concern due to the presence of heavy metal ion in wastewater is very alarming. Membrane technology is well proven alternative separation process compared to traditional methods. In this area of separation, ceramic membrane is very popular due to their every high thermal stability as well as their inertness to harsh chemical condition unlike organic polymeric membrane. These membranes can be easily prepared from natural mineral or from even industrial waste. Membrane treatment cost can be more economical in case of microfiltration due to less transmembrane pressure then ultrafiltration process. In this review UF, MF and hollow fiber membrane are discussed for wastewater treatment.

    Figures

    MEMBRANE_JOURNAL-32-4-227_F1.gif

    Schematic representation of classification of the review.

    MEMBRANE_JOURNAL-32-4-227_F2.gif

    Cross section SEM images of membranes (a) Neat PSf membrane; (b–d) PSf/Zeolite 4A membranes; (e–g) PSf/UiO-66 membranes; (h–j) PSf/Zeolite 4A-UiO-66 membranes with different nanofiller loadings (0.5 wt%, 1 wt%, 2 wt%, respectively) (Reproduced from Anjum et al.[14]).

    MEMBRANE_JOURNAL-32-4-227_F3.gif

    Flux versus time for mixed-matrix PSf membranes with different nanofiller concentrations during three steps: water flux for 150 min, humic acid solution flux for 150 min, and water flux for 150 min after 30 min washing with distilled water (a) PSf/Zeolite 4A, (b) PSf/UiO-66 and (c) PSf/Zeolite 4A-UiO-66 (Reproduced from Anjum et al.[14]).

    MEMBRANE_JOURNAL-32-4-227_F4.gif

    (a) and (b) FESEM images of the inner and outer surfaces of the substrate; (c) and (d) inner and outer surfaces of the MFI zeolite membrane; (e) MFI zeolite particles; and (f) cross-sectional view of the MFI zeolite membrane (Reproduced from Kumar et al., 17, IWA Publishing).

    MEMBRANE_JOURNAL-32-4-227_F5.gif

    (a) Water flux as a function of time for pressures and (b) water flux as a function of applied pressure for the ceramic substrate and zeolite membrane (Reproduced from Kumar et al., 17, IWA Publishing).

    Tables

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