Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xiaoyu Du,Tong Gu,Jingyu Xu,Yanqing Qu,Hongge Jia,Shuangping Xu,Mingyu Zhang,Jun Chen
Covalent organic framework (COF) membranes have garnered significant attention as a promising separation technology for dye wastewater treatment, owing to their meticulously ordered pore structure and exceptional chemical stability. The Polyamide COF (Amd-COF) membrane, characterized by amide-linkages, exhibits excellent hydrophilicity and chemical stability, whereas the polyamine COF (Amn-COF) membrane, featuring amine-linkages, demonstrates remarkable flexibility and resistance to chlorine. In this study, we present the synthesis of defect-free Amd/TA-PVA/Amn COF composite membranes with large area and continuous structure through multi-interfacial polymerization. The incorporation of an intermediate layer (TA-PVA) enables stable formation of strong hydrogen bonds between Amd-COF and Amn-COF, thereby enhancing the durability of the composite membranes. Due to the unique structural features and functional groups of the Amd/TA-PVA/Amn COF composite membranes, they exhibit not only high water permeability (119.24 L•m −2 h −1 bar −1 ) but also exceptional rejection efficiency towards Rhodamine B, achieving up to 96.55 % removal. Specifically, the membranes treated with a chlorination intensity of 2000 ppm exhibit stable permeance and dye rejection performance. Moreover, these membranes exhibit exceptional stability in both structure and performance over multiple cycles. This can primarily be attributed to the highest density of amino moieties and phenolic hydroxyl groups on their surface. This work underscores the significant potential of COF membrane incorporating amide and amine functionalities for high-performance separation and anti-chlorine applications.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Pengbo Zhao,Junquan Meng,Rui Zhang,Bing Cao,Pei Li
Pervaporation (PV) desalination membranes have good anti-fouling properties due to its hydrophilic dense surface structure. However, organic fouling is inevitable in long-term operation. Sodium hypochlorite (NaClO) is commonly used for cleaning organic pollutant, but it may damage polymeric membrane. Thus, designing membrane material with good chlorine resistance is crucial for expanding its lifespan. In this study, polyvinyl alcohol (PVA) was selected to prepare PV membrane in concern of its hydrophilicity and good film forming property. Its chlorine resistance was improved by removing the more active 1,2-diols of PVA by reacting with sodium periodate, grafting with poly (styrene-co-maleic anhydride) to decrease its crystallinity, and crosslinking using a fluorocarbon surfactant (FS). The resulting PV membrane exhibited the highest reported chlorine resistance of 768000 ppm·h among PV and RO membranes with a high-water flux of 44.5 ± 1.5 kg/m 2 ·h and salt rejection of 99.93%. A long-term fouling and cleaning cycle experiment was carried out using 10000 ppm humic acid to mimic organic foulants. The flux was recovered 100% after the NaClO cleaning. Hence, the chlorine-resistant PV membrane had the ability for sustainable desalination application.
研究领域:
高分子材料科学
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膜分离技术
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环境工程
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水处理
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化学工程
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Huachuan Sun,Hsiao-Chien Chen,Muhammad Humayun,Yang Qiu,Jun Ju,Yumin Zhang,Mohamed Bououdina,Xinying Xue,Qingju Liu,Yuanjie Pang,Chundong Wang
Immobilizing platinum (Pt) single atoms on appropriate supports with optimized coordination environments and electronic structures is a promising strategy to address the problem of chlorine corrosion during seawater electrolysis. Herein, Pt single atoms on nickel-vanadium layered double hydroxides (Pt-SA/NiV-LDH) matrix are fabricated for chlorine tolerance hydrogen generation. Due to the strong synergetic electronic interaction between atomically dispersed Pt and the ultrathin NiV LDH matrix, the adsorption/dissociation feature of *H 2 O, *OH, and *H are optimized as evidenced theoretically. The as-fabricated Pt-SA/NiV-LDH electrode exhibits an exceptional mass activity (i.e., 30.98 times higher) compared to the commercial Pt/C, along with an ultra-high turnover frequency (TOF) value of 9.90 s −1 in alkaline media. Impressively, only 207 mV overpotential is required to yield a current density of 2000 mA cm ‒2 in an electrolyte solution containing 1 m KOH and 2 M NaCl, indicating its robust resistance to chlorine. Moreover, this kind of material demonstrates remarkably low overpotentials of 130 and 215 mV to attain the industrial-scale current densities of 1000 and 2000 mA cm −2 in alkaline seawater, accompanied by exceptional stability for 500 h working at 500 mA cm −2 . This work provides an insightful reference for the production of sustainable green hydrogen through seawater electrolysis.
研究领域:
材料科学
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催化化学
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能源转换
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2014
·
IF 4.908
Li-Fen Liu,Zhi-Bin Cai,Jiang-Nan Shen,Li-Xiang Wu,Eric M.V. Hoek,Cong-Jie Gao
A novel poly(amide-urethane@imide) reverse osmosis (RO) composite membrane with chlorine-tolerant property was prepared on a polysulfone supporting film through two-step interfacial polymerization. The crosslinking agent – 5-choroformyloxyisophaloyl chloride (CFIC) was first reacted with 4-methyl-phenylenediamine (MMPD) via interfacial polymerization to get the nascent poly(amide-urethane) base membrane (CFIC–MMPD) without curing treatment. Then the resultant base membrane contacted again with the second aqueous solution containing functional secondary amine – N,N′-dimethyl- m -phenylenediamine (DMMPD) to obtain the poly(amide-urethane@imide) TFC RO membrane (MMPD–CFIC@CFIC–DMMPD). X-ray photoelectronic spectroscopy (XPS) was combined with attenuated total reflectance infrared (ATR-IR) to verify that the ultrathin polyimide film (CFIC–DMMPD) has been successfully grafted on the surface of the MMPD–CFIC base membrane. The images of scanning electronic microscopy (SEM) and atomic force microscope (AFM) showed that the poly(amide-urethane@imide) membrane has much smoother, more hydrophilic surface than the poly(amide/imide-urethane) membrane (MMPD/DMMPD–CFIC) prepared by conventional one-step interfacial polymerization of CFIC and composite MMPD/DMMPD. However, the permeation experiment revealed that the poly(amide-urethane@imide) membrane has a slight loss in both salt rejection and water flux than the poly(amide/imide-urethane) membrane and conventional commercialized polyamide membrane (MPD–TMC), but exhibits better chlorine-tolerant property due to the introduction of ultrathin polyimide film (CFIC–DMMPD) on the outmost surface of the TFC RO membrane, and the combination of IR and XPS analyses shows a good agreement with the chlorine exposure results of membranes.
研究领域:
材料科学
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环境工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Zihui Wang,Langming Bai,Jinlong Wang,Heng Liang,Guibai Li
Nanofiltration (NF) based purification technology plays a growing role in water softening, wastewater reuse, and drinking water production , whose core component is the thin-film composite (TFC) polyamide (PA) surface separating layer with high water permeation and significant antifouling and chemical resistance. Strengthening water transport with simultaneously improving chemical tolerance and fouling resistance accords with the demands for sustainable water treatment. In this work, a photo-assisted crosslinked NF membrane with a regulated interlaced stripe surface morphology was fabricated through grafting 2-acrylamido-2-methyl-1-propanesulfonic acid (AMPS) into the PA network during visible light irradiation. Surface structures and chemical features were characterized, and the NF performance, antifouling and chlorine resistance were systematically evaluated. The optimal membrane with AMPS molecules carrying sulfonyl groups crosslinked in the PA network was rendered electronegative charge, uniformly narrowed pore size, improved hydrophilicity, and higher crosslinking degree. The water permeation was augmented to 30.5 L m −2 h −1 ·bar −1 for the optimal membrane, four times more advanced than the pristine membrane with a water permeability of 5.9 L m −2 h −1 ·bar −1 , and the divalent salt retention was improved to 99.7%. In addition, the optimal membrane also exhibited outstanding chlorine tolerance, fouling removal, and antifouling capacity. The flux recovery ratio ( FRR ) of the best membrane outperformed that of the pristine membrane and the flux declined more slowly in the whole fouling cycle testing. This work provides a novel avenue for fabricating high-efficiency TFC membranes with great water permeation and fouling resistance.
研究领域:
环境科学
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材料科学
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水处理技术
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 62
·39127-39137
·
IF 3.108
Hao Wu,Xiao-Lin Chen,Xiang Huang,Hui-Min Ruan,Yan-Li Ji,Li-Fen Liu,Cong-Jie Gao
In this work, a novel semi-aromatic polyamide RO membrane was fabricated by using a new self-made dendritic molecule trimesoylamidoamine (TMAAM) as a key functional amine monomer that combined 1,3-diamino-2-propanol (DAP) to react with trimesoyl chloride (TMC) through interfacial polymerization technology. By adjusting the TMAAM concentration and amine-immersion mode, this new TMAAM-based semi-aromatic polyamide RO membrane exhibits simultaneously improved water permeability, antifouling and chlorine-tolerant properties. The introduced TMAAM units in polyamide chains can enhance the TMAAM-based membrane's water flux due to its dendritic structure as well as rich hydrophilic groups, and the DAP–TMAAM–TMC membrane prepared via the new two-step amine-immersion mode has 1.9 times more water flux without loss of salt rejection than the pristine DAP–TMC membrane and also shows higher water flux than the hand-cast conventional aromatic polyamide MPD–TMC membrane, respectively. At the same time, the regularly distributed hydroxyl groups and aliphatic amide bonds in TMAAM units contribute to the improved hydrophilicity and chlorine-tolerant property of the resultant DAP–TMAAM–TMC membrane, respectively. It is also demonstrated that the new two-step amine-immersion mode leads to a much smoother surface which endows the resultant DAP–TMAAM–TMC membrane with a favorable antifouling ability. This research provides us with a promising functional amine monomer and a new membrane formation method to fabricate a high performance RO membrane.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
Water
·
2024
·Vol. 16
·期 19
·2752
·
IF 3
Weibin Cai,Yuzhe Wang,Yuannan Li,Hong Ye,Fuyuan Xiao,Lei Wang,Hengjun Gai
Nanofiltration (NF) has become a widely used technology in water treatment due to its environmental friendliness, energy efficiency, cost-effectiveness, and operational simplicity. However, polyamide (PA) NF membranes still face challenges, including low permeate flux, limited resistance to organic pollutants, and inadequate resilience to residual chlorine. To address these issues, this study developed a thin-film composite (TFC) NF membrane featuring a separation layer of sandwich structure. Initially, a single separation layer of polyvinyl alcohol (PVA) NF membrane was prepared, followed by the fabrication of a PA layer on its surface, and ultimately, a second PVA layer was constructed on the PA layer. The experimental results show that the PVA/PA/PVA sandwich structure TFC exhibits high permeability to pure water and robust resistance to both pollution and residual chlorine. The PVA-0.20/PA/PVA-0.20 TFC, prepared with a 0.20%w/vPVA solution, achieved a pure water flux of up to 22.05 L m−2h−1bar−1(LMH/bar), which was 2.92 times higher than that of the control TFC membrane. Additionally, it demonstrated a salt rejection rate exceeding 96% for Na2SO4and over 99% for Congo Red (CR) and Victoria Blue B (VB). In comparison with the control TFC membrane, the PVA-0.20/PA/PVA-0.20 membrane exhibited significantly enhanced resistance to pollution. Following immersion in a 1000 ppm NaClO solution for 4 h, the rejection rate of the control TFC membrane decreased markedly and that of the PVA-0.20/PA/PVA-0.20 membrane decreased marginally, indicating excellent resistance to residual chlorine. Due to the robust overall performance of the PVA/PA/PVA membrane, it holds potential advantages for application in treating reclaimed water or slightly polluted water.
研究领域:
水处理
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膜技术
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环境工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Huiqing Wu,Huazhen Sun,Weijie Hong,Long Mao,Yuejun Liu
Tannic acid–FeIII functionalized multiwall carbon nanotubes (TA-MWNTs) were successfully obtained through a simple and rapid procedure by forming a stable TA–FeIII complex coating on the MWNT surface. Hydrophilic TA-MWNTs can disperse well in the aqueous phase and help the formation of a polyamide (PA) thin film nanocomposite (TFN) membrane through interfacial polymerization. TA-MWNT concentration in the aqueous phase was adjusted to achieve the optimal water flux and salt rejection of the TFN membrane. The results reveal that, when 0.03% of TA-MWNTs are added, the optimized water flux of the TFN membrane reaches up to 31.4 L/m2h, 2.36 times of that of the neat PA membrane, along with a well-maintained Na2SO4 rejection. Furthermore, the as-prepared TFN membrane shows improved antifouling ability and good long-term stability. A significantly enhanced chlorine resistant capability of the TFN membrane is also presented, which can be ascribed to the radical capturing capability of phenol groups of TA as well as more oxidation-stable polyester bonds produced by the interaction between the phenol groups of TA and the acyl chloride groups of TMC. Assisted by TA-MWNTs, the TFN membrane is found to have prominent advantages over PA and MWNTs/PA TFN membranes.
研究领域:
材料科学
·
环境工程
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Chunwei Xu,Feifei Shao,Zhan Yi,Hongzhou Dong,Qian Zhang,Jianhua Yu,Jianguang Feng,Xiangfang Wu,Qingqing Zhang,Liyan Yu,Lifeng Dong
Poor chlorine resistance is one of the main challenges of polyamide (PA) reverse osmosis membranes. In this work, PA hybrid membranes modified with oxidized graphitic carbon nitride (CNO), graphitic carbon nitride (g-C 3 N 4 ), or graphene oxide (GO) are prepared by interfacial polymerization. The results show that CNO can be used as antioxidant to improve chlorine resistance of the PA membrane, and PA-CNO hybrid membranes demonstrate better chlorine resistance than PA-GO membranes. For instance, after 40 h active chlorine treatment, salt rejection of PA-CNO decreases by 15%, while the salt rejection of PA-GO, PA-g-C 3 N 4 , and pristine membrane declines by 22%, 30%, and 27%, respectively. X-ray photoelectron spectroscopy is used to analyze antioxidant performance of CNO. The number of C-N bond of PA-CNO membrane and pristine membrane respectively decreases by 1.2% and 7.6% after chlorine treatment, which indicates CNO has ability to capture and react with chlorine free radicals.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Caini Liu,Wenyi Wang,Liuyong Zhu,Fangyan Cui,Chengcheng Xie,Xingyu Chen,Ning Li
A structurally controlled polyethersulfone (PES) membrane, as the substrate of the thin film composite nanofiltration (NF) membranes, was designed and fabricated with aligned carbon nanotubes (ACNTs) by a direct current electric field. The morphology and properties of the NF membranes were simultaneously affected by the PES substrate with especial macrovoids and ACNTs, increasing the permeability from 6.4 to 29.7 L/m 2 h bar. It was confirmed by FT-IR and XPS that the poly(piperazine amide) selective layer of the modified NF membrane has an increased content of –COOH for enhanced hydrophilicity. The zeta potential proves that the surface of the NF membrane modified by electric field has weaker negative charge than that of unmodified membrane in the range of pH = 5–9. Under the combined action of the Donnan effect and size exclusion, the rejection of MgCl 2 increased while maintaining the dianion rejection above 95%. Particularly, the NF membrane modified with ACNTs exhibited better chlorine resistance and antifouling ability, thus improving the stability and perdurability of membranes. Our work utilizes the characteristics of ACNTs to explore its potential in NF membranes.
研究领域:
材料科学
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化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Xu Dong,Xiaojuan Wang,Huacheng Xu,Yijun Huang,Congjie Gao,Xueli Gao
Aiming at enhancing the permeability of reverse osmosis (RO) membranes, polyaniline-co-polypyrrole hollow mesoporous nanospheres (PPHMNs) were synthesized with aniline and pyrrole monomers via a simple and rapid one-step method, and then added to the aqueous phase of interfacial polymerization to fabricate thin-film nanocomposite (TFN) membranes. Hollow cores of the PPHMNs embedded in polyamide layers could reduce the interior transfer resistance of the membrane and shorten the transmission pathway of water molecules. Mesoporous shell of PPHMNs provided more channels for rapid transmission of water molecules. Moreover, amino groups in PPHMNs originated from the monomer of aniline could not only be bonded to polyamide (PA) layer by reacting with acyl chloride groups to prevent the leakage but also improve hydrophilicity of the membrane. Water flux of TFN membrane doped with PPHMNs (TFN-Ps) of 0.005 wt% addition concentration was 34.1 L·m − 2 ·h − 1 which is 76.7% higher than that of thin-film composite (TFC) membrane, and the NaCl rejection all kept over 99.0%. The TFN-Ps also showed excellent long-term stability, chlorine resistance and anti-fouling performance. This work opens an avenue for application of mesoporous hollow nanospheres with amino groups synthesized by simple and time-saving methods in developing TFN membranes with improved water flux.
研究领域:
材料科学
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化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
·
2023
·Vol. 9
·期 18
·
IF 13.6
Yunxiang Bai,Beibei Liu,Jiachen Li,Minghui Li,Zheng Yao,Liangliang Dong,Dewei Rao,Peng Zhang,Xingzhong Cao,Luis Francisco Villalobos,Chunfang Zhang,Quan-Fu An,Menachem Elimelech
The successful implementation of thin-film composite membranes (TFCM) for challenging solute-solute separations in the pharmaceutical industry requires a fine control over the microstructure (size, distribution, and connectivity of the free-volume elements) and thickness of the selective layer. For example, desalinating antibiotic streams requires highly interconnected free-volume elements of the right size to block antibiotics but allow the passage of salt ions and water. Here, we introduce stevioside, a plant-derived contorted glycoside, as a promising aqueous phase monomer for optimizing the microstructure of TFCM made via interfacial polymerization. The low diffusion rate and moderate reactivity of stevioside, together with its nonplanar and distorted conformation, produced thin selective layers with an ideal microporosity for antibiotic desalination. For example, an optimized 18-nm membrane exhibited an unprecedented combination of high water permeance (81.2 liter m−2 hour−1 bar−1), antibiotic desalination efficiency (NaCl/tetracycline separation factor of 11.4), antifouling performance, and chlorine resistance.
研究领域:
材料科学
·
制药工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）