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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Fabrication of superhydrophobic PVDF composite membranes using modified ZIF-8 for efficient and stable membrane distillation: Mitigating fouling and wetting

Peiqing Zhang,Sihang Li,Fan Xiao,Yongfang Xiao,Yi Zhang,Zhongguo Shan,Zhenyu Li,Haihua Wang

Membrane distillation (MD) represents a promising advance in wastewater purification, contributing to the mitigation of water scarcity. Hydrophobic poly(vinylidene fluoride) (PVDF) microporous membrane is susceptible to wetting by low surface tension substances, leading to fouling. To address this, PVDF membrane was superhydrophobically modified using modified ZIF-8 to obtain two composite membranes, AZ/PVDF and Z@C/PVDF. AZ/PVDF and Z@C/PVDF composite membranes were prepared by coating more dispersible APTES-ZIF-8 and ZIF-8@MWCNT, respectively, onto the surface of PVDF membrane. The hydrophobicity of the composite membranes was regulated by silane types, fluorination methods, and fluorination time, resulting in reduced surface roughness and increased surface energy. The contact angles of AZ/PVDF and Z@C/PVDF were 154.2 ± 3.4° and 156.8 ± 4.2°, respectively. Both AZ/PVDF and Z@C/PVDF membranes demonstrated outstanding mechanical, thermal, and chemical stability. AZ/PVDF and Z@C/PVDF membranes outperformed PVDF membrane, extending operation times by 2 h and 3 h, respectively, without obvious NaCl crystals. Furthermore, Z@C/PVDF membrane exhibited superior resistance to wetting by SDS than AZ/PVDF and PVDF membranes, treating pickle brine via the direct contact MD (DCMD) process with a recovery rate of 30.2 % within 10 h. Overall, this research offers a promising approach to fabricating superhydrophobic composite membranes for high-salt brine treatment via DCMD.

研究领域: 化学工程 · 材料科学 · 环境工程 · 纳米技术
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Journal of Hazardous Materials Advances · 2022 · IF 0

Inhibition of membrane biofouling by grafting quorum sensing inhibitors onto ultrafiltration membranes

Rukang Tian,Xiaofang Ma,Yan Wang,Hong Mei,Yunkun Wang

Quorum sensing inhibitors (QSIs) can inhibit biofilm formation by regulating the synthesis of extracellular polymeric substances (EPS), thus alleviating biofouling in the membrane filtration process. In this study, utilizing the adhesion ability of a mussel-inspired biomimetic material, polydopamine (PDA), natural quorum sensing inhibitors, vanillin and furanone, were modified on a commercial polyethersulfone (PES) ultrafiltration (UF) membrane to inhibit the formation of biofilm fouling. We proved that QSIs were successfully grafted onto the membrane surface without blocking the pore structure, and the pure water flux of the membrane was simultaneously improved due to hydrophilicity improvement. The vanillin-modified membrane significantly inhibited the biofilm formation of P. aeruginosa PAO1 (81.7% inhibition rate), while furanone had a certain inhibitory effect on E. coli MG1655 and PAO1. We also tested the modified membrane in the dynamic filtration of simulated wastewater, in which both modified membranes alleviated biofouling.

研究领域: 环境科学 · 微生物学
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Water · 2024 ·Vol. 16 ·期 12 ·1747 · IF 3

Surface Modification of PVDF and PTFE Hollow Fiber Membranes for Enhanced Nitrogen Removal in a Membrane-Aerated Biofilm Reactor

Wenfeng Zai,Yangman Chen,Qingdong Qin,Xiangkun Li,Dezhao Liu

HighlightsPlasma-grafting acrylic acid composite membrane for MABR was prepared.Higher O2transfer rate and better hydrophilicity for modified membranes than pristine.Modified PVDF membrane demonstrated superior nitrogen removal during startup.Activity of denitrifying bacteria was enhanced in the modified PVDF MABR.AbstractMicroporous membranes such as polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF) often exhibit suboptimal hydrophilicity and microbial adhesion, which impede effective nitrogen removal in membrane-aerated biofilm reactors (MABRs), particularly during initial operational phases. To address this issue, the present study introduced acrylic acid (AA) following plasma treatment (P) to enhance membrane performance, thereby engineering a novel composite material optimized for MABR applications. Four MABRs—Reactor with pristine PVDF membrane (R-PVDF), Reactor with composite PVDF membrane (R-PVDF-P-AA), Reactor with pristine PTFE membrane (R-PTFE), and Reactor with composite PTFE membrane (R-PTFE-P-AA)—were evaluated. The modified membranes displayed enhanced roughness and hydrophilicity, which improved biocompatibility and variably increased the oxygen transfer efficiency. Notably, the R-PVDF-P-AA configuration showed a significant enhancement in the removal rates of NH4+-N and total nitrogen (TN), achieving 78.5% and 61.3%, respectively, which was markedly higher than those observed with the original membranes. In contrast, the modified R-PTFE-P-AA exhibited lower removal efficiencies, with NH4+-N and TN reductions of approximately 60.0% and 49.5%. Detailed microbial community analysis revealed that the R-PVDF-P-AA membrane supported robust commensalism between ammonia-oxidizing and denitrifying bacteria, underpinning the improved performance. These findings highlight the critical role of surface chemistry and microbial ecology in optimizing the function of MABRs.

CAS / MDL: 79-10-7 7646-79-9
研究领域: 环境工程 · 微生物学 · 材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Effects on the Performance of Filtration in a Constant-Pressure Stirred Membrane Reactor

Yuanyuan Hui,Xin Feng,Haoliang Wang,Zai-Sha Mao,Chao Yang

Membrane fouling is a troublesome factor in the design and scale-up of stirred membrane reactors. Many efforts have been made to study the fouling mechanism in traditional membrane filtration. However, it is still ambiguous in stirred membrane reactors (SMRs). For this purpose, we investigated the effects of hydrodynamics on membrane filtration performance in SMRs under constant-pressure operation by combining experiment and computational fluid dynamics (CFD) simulation. The results indicate that the strong axial flow is beneficial in maintaining the stability of membrane permeation, while the strong radial flow works oppositely. In addition, the formation of the filtration cake increases the total membrane filtration resistance but keeps smaller particles from blocking the membrane surface channels, which leads to filtration resistance multiplying rapidly. Hence, the formation of the thick cake, strong axial flow, and weak radial flow is conducive to maintaining permeation flux in order to reduce the replacement of the membrane and improve the period of continuous production.

研究领域: 化学工程 · 环境工程 · 生物工程
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Constructing Thin and Cross-Linked Polyimide Membranes by Interfacial Reaction for Efficient CO2 Separation

Xiaochen Xu,Jie Dong,Xian Xiao,Xin Zhao,Qinghua Zhang

At present, the glassy polymeric membrane technology for CO2 separation is still confronted with a predicament that it is still difficult to fabricate membranes with both high CO2 permeance and high gas selectivity. Fortunately, newly developed thin film composite membranes (TFC) (∼100 nm) can facilitate high CO2 permeation by minimizing gas trans-membrane resistance and macrovoid defects. Herein, a novel TFC membrane containing a thin polyimide (PI) selective layer on a PDMS-modified PSf substrate was successfully constructed in situ by an interfacial cross-linking reaction between the amine-end-capped PI oligomer and the trimesoyl chloride (TMC) in a mild solvent system. The thickness of the thin PI selective layer is in the range of 103–485 nm and can be optimized by adjusting the interfacial polymerization parameters such as the TMC concentration. The resultant TFC membrane comprising a polyimide selective layer exhibits an optimum CO2 permeance of 330 GPU with the CO2/N2 and CO2/CH4 ideal selectivities of 30 and 32, respectively. It is an obvious improvement in CO2 separation performance compared with conventional PI flat membrane. In addition, these membranes also show an excellent plasticizing resistance and long-term stability attributed to the cross-linking structure and thin nature. It is expected that this TFC membrane structure combined with its facile fabricating process can facilitate the development of thin glassy polymeric membranes for CO2 separation.

CAS / MDL: 77-58-7 78-10-4
研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2018 · IF 6.578

Controlling structure and properties of polyamide nanofilms by varying amines diffusivity in organic phase

Zhuyuan Wang,Songmiao Liang,Yan Jin,Lianrui Zhao,Lijie Hu

Optimizing thickness and structure of polyamide (PA) selective layer of thin film composite (TFC) membranes is critical to improve the performance of the membranes. Here, we employed controlled interfacial polymerization to fabricate free-standing PA nanofilms on a thermal-reversible agarose hydrogel. Manipulation of the nanofilms structure was approached by tailoring the amine diffusivity in organic phase composed of benzene and n-hexane mixtures. An UV–vis method was firstly developed to in-situ monitor the diffusion process of amines from aqueous phase to organic phase. The structure and properties of the nanofilms were systematically analyzed by SEM, AFM and ATR-IR. Experimental results revealed that the diffusion kinetics of amines in organic phase is strongly depends on the content of benzene in the mixture solvent and therefore give rise to different thickness and structure of the nanofilms. The amines diffusion rate was accelerated at higher benzene content, causing a rougher surface, thicker thickness and smaller Young's modulus of the resultant nanofilms. Remarkably, with good fitting coefficient of R 2 = 0.9936, the thickness of the nanofilms exhibits a linear relationship with their surface roughness .

研究领域: 材料科学 · 化学工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2017 · IF 3.133

Facile fabrication of p-type CuxS transparent conducting thin films by metal sulfide precursor solution approach and their application in quantum dot thin films

Shenjie Li,Tianyong Zha,Qiang Wang,Chengyu Wang,Yujiao Ren,Yanyan Chen,Daocheng Pan

We present a facile route for the fabrication of P-type Cu x S transparent and conducting thin films (TCTFs) using copper (I) oxide and butyl-dithiocarbamic acid as precursors by pulling method on glass. The as-deposited highly conductive crystalline Cu x S films showed high carrier concentration (∼3.11 × 10 22  cm −3 ), low electrical resistivity (∼1.02 × 10 −4  Ω cm) and conclusive p-type conduction. X-ray diffraction studies showed high crystallinity, and the optical transmission spectra in UV–vis–NIR region of such films were recorded, indicating that the transparency was over 75% with a band gap of 1.52 eV. The room-temperature sheet resistance increased from 9.9 to 302.4 Ω sq −1 with increasing baking temperature. The Cu x S/quantum dot bifacial thin films have been fabricated, and the experimental results indicated that luminescent, transparent, and conductive Cu x S/Cu-doped Zn y Cd 1-y S thin films have a very high potential application in thin film solar cells.

研究领域: 材料科学 · 光电材料 · 太阳能电池
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Micromechanism Underlying Wetting Behavior of the Vacuum Membrane Distillation during Desalination

Lei Jiao,Lida Meng,Kangkang Yan,Jing Wang,Ge Li,Zhikan Yao,Zhilin Sun,Lin Zhang

Membrane wetting is a crucial issue in the desalination process by vacuum membrane distillation (VMD). However, the micromechanism of the wetting behavior is far from clear. Here, electrospun nanofiber membranes (ENMs) had been utilized to clarify the pore variations inside the membrane for desalination from NaCl aqueous solution, where the distinct open pore structure of ENMs could address the characterizing limitations for the change occurring in the membrane pores. A wetting formation model had been depicted on the basis of characterized results, illustrating that the basic reason for wetting was the initial NaCl crystallization caused by supersaturation, which was different from the membrane pores blocking or the structure damage caused by scaling. Moreover, membrane regeneration experiments also showed that the wetting caused by the crystallization of NaCl was reversible. By a reasonable regeneration strategy, VMD used for desalination was expected to achieve continuous operation with rejection over 99.9%.

研究领域: 材料科学 · 环境工程
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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Tailored thin film nanocomposite membrane incorporated with Noria for simultaneously overcoming the permeability-selectivity trade-off and the membrane fouling in nanofiltration process

Zhe Yang,Longting Li,Chi Jiang,Na Zhao,Shenghao Zhang,Yaoli Guo,Yi Chen,Shuangmei Xue,Chenhao Ji,Shuzhen Zhao,Ralph Rolly Gonzales,Hideto Matsuyama,Jianzhong Xia,Q. Jason Niu

Membrane fouling as well as the “trade-off effect” between water permeability and selectivity are the grand challenges for nanofiltration (NF) membranes. In this study, a macrocyclic molecule, Noria, was embedded in the polyamide layer to fabricate a thin film nanocomposite (TFN) membrane with high performances of separation and antifouling. Noria was first synthesized and dissolved in a piperazine (PIP) aqueous solution. Then the TFN membrane (i.e., PIP-Noria-TMC membrane, TMC is the abbreviation of 1,3,5-benzenetricarbonyl trichloride) was prepared by interfacial polymerization using PIP-Noria mixture as aqueous phase. The optimal PIP-Noria-TMC membrane reached 147.6 L m -2 h -1 MPa -1 of water permeability, which was almost twice that of the pristine NF membrane (i.e., PIP-TMC membrane). Meanwhile, the PIP-Noria-TMC membrane exhibited comparable Na 2 SO 4 rejection (∼98%) to the PIP-TMC membrane and outstanding mono/divalent salt selectivity. Besides, static adsorption tests using E.coli and bovine serum albumin (BSA) as the model foulants revealed that the surface of PIP-Noria-TMC membranes with high hydrophilicity and electronegative charge could effectively resist foulant attachment, which was also exhibited in the dynamic BSA filtration tests. Therefore, this work provided a practicable pathway to simultaneously overcome the permeability-selectivity trade-off and membrane fouling problems for the NF process.

CAS / MDL: 111-30-8
研究领域: 环境科学 · 材料科学
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CHEMOSPHERE · 2022 · IF 8.943

A novel janus membrane modified by MXene for enhanced anti-fouling and anti-wetting in direct contact membrane distillation

Xiaoju Yan,Chengyu Yang,Cong Ma,Hui Tao,Shirong Cheng,Lin Chen,Guodong Wang,Xinping Lin,Chengzhi Yao

Membrane fouling and wetting limit the applications of membrane distillation (MD) for wastewater treatment , especially when treating the wastewater with a high concentration of low surface tension substances such as oil and surfactants. In this paper, virgin polyvinylidene fluoride (PVDF) membrane was modified by polydimethylsiloxane (PDMS) to enhance anti-wetting ability. Then a thin polydopamine (PDA) layer was coated as a reaction platform for further modification. Polyethyleneimine (PEI) was cross-linked with PDA to form a uniform and stable layer, through hydrogen bonds and electrostatic interaction to immobilize hydrophilic MXene, which formed a Janus MXene-PVDF membrane. The MXene layer was the key for superoleophobicity and high liquid entry pressure (LEP) of membrane, capable of mitigating membrane fouling and wetting when dealing with low surface tension wastewater (LSTW). From the experiments results, pristine PVDF membrane showed severe fouling and wetting with flux decline and salt leakage during treatment of LSTW (surfactants containing water, oil-in-water emulsion and sodium dodecyl sulfate stabilized oil-in-water emulsion). However, under the same conditions, the Janus MXene-PVDF membrane exhibited remarkably stable flux (9.3 kg m −2 h −1 , 9.1 kg m −2 h −1 , 10.2 kg m −2 h −1 ) and salt rejection (almost 99.9%) after 15 h operation. Excellent fouling and wetting resistance of MXene-PVDF membrane was mainly attributed to its superhydrophilic and superoleophobic top surface (in-air water contact angle: 30.2°, under-water oil contact angle: 169.9°) and hydrophobic substrate (in-air water contact angle: 130.8°), together with high LEP value (91.1 Kpa). This study provides a viable route to fabricated a Janus membrane with outstanding fouling and wetting resistance for LSTW, oily wastewater and it has great potential for sewage treatment in the future.

研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Preparation of hydrophobic zeolitic imidazolate framework-71 (ZIF-71)/PVDF hollow fiber composite membrane for membrane distillation through dilute solution coating

Hongbin Li,Hengji Liu,Wenying Shi,Haixia Zhang,Rong Zhou,Xiaohong Qin

Mixed matrix membranes (MMMs) combine the advantages of different materials and hopefully break through the limitation of high mass transfer resistance and low permeability in membrane distillation (MD) process. In this study, hydrophobic zeolitic imidazolate framework-71 (ZIF-71)/polyvinylidene fluoride (PVDF) hollow fiber composite membrane was prepared by the dilute solution coating method. ZIF-71 was incorporated into the PVDF dilute solution and a macroporous hydrophobic ZIF-71/PVDF coating layer was formed on the outer surface of PVDF hollow fiber support membrane through the nonsolvent induced phase separation (NIPS) process. PVDF hollow fiber support membrane was fabricated by the dry-jet wet spinning process. Membrane surface morphologies were observed through Field emission scanning electron microscope (FESEM). The effects of zeolitic imidazolate frameworks (ZIFs) content in PVDF coating layer on membrane surface hydrophobicity and desalination performance were investigated through Dynamic water contact angle (WCA) measurements and the vacuum membrane distillation (VMD) experiment, respectively. The VMD experiment was carried out at feed temperature 50 °C and permeation side vacuum 31.3 kPa using 3.5 wt% NaCl aqueous solution as the feed solution. Compared with the uncoated PVDF hollow fiber membrane, both the surface hydrophobicity and the water permeability of the ZIFs-incorporated PVDF hollow fiber composite membranes are improved. The surface WCA and permeation water flux of ZIFs-PVDF composite membrane increase from 94.5 to 136.5° and 13.5 to 27.1 kg . m −2. h −1 meanwhile the NaCl rejection could maintain at 99.99%. No obvious pore wetting phenomenon was observed for ZIFs-PVDF hollow fiber composite membrane during the continuous VMD experiment for 60 h. The dilute solution coating is a promising method to prepare high-performance hollow fiber composite membrane for the desalination in MD process.

研究领域: 材料科学 · 环境工程
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DESALINATION · 2024 · IF 8.3

Enhancing membrane distillation efficiency in treating high salinity organic wastewater: A pressure-driven membrane electrochemical reactor approach

Xiaolei Chen,Zhongsen Yan,Haiqing Chang,Qiankun Wang,Gongduan Fan,Jinghan Ye,Kaiqin Xu,Heng Liang,Fangshu Qu

Fouling of membranes continues to be a prominent challenge in the membrane distillation (MD) treatment of high salinity organic wastewater (HSOW). Although membrane electrochemical reactor (MER) can effectively inhibit the membrane fouling of MD, the high cost of the proton exchange membrane (PEM) used in MER limits its widespread application. In this study, cost-effective pressure-driven membranes were employed as a substitute for PEM to establish pressure-driven membrane electrochemical reactors for HSOW pre-treatment. By using ultrafiltration membrane (UFM) and reverse osmosis membrane (ROM), UFMER and ROMER were developed, respectively. Due to the superior electrochemical performance of UFM, UFMER saved 43 % of energy compared to PEMER with the highest removal rate of organics (~85 %) in the simulated HSOW treatment. In practical applications, using UFMER significantly reduced the amount and size of complexes in the real nanofiltration concentrate (NC) of landfill leachate. This contributed to the superior specific flux maintenance (97 %) with a salt rejection (>99 %) and the highest recovered specific water flux (99.6 %) in MD cases. UFMER reduced ~27 % of energy compared to PEMER in MER pre-treatment, and saved the most energy (~39.6 %) in MD post-treatment. Hence, this strategy is potential for forthcoming applications, notably in lowering the membrane cost of MER and energy consumption of both MER and MD.

研究领域: 环境科学 · 化学工程
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