CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Mingliang Zhang,Qian Ye,Qianqian Yi,Hanbin Wu,Chao Liu,Bingjie Zhang,Xinyi Li,Bin Yan
Extensive studies have been conducted on advanced oxidation processes (AOPs) for the removal of antibiotics in water environments. However, the separation and recovery of powdered catalysts from water at the end of the reaction remains a great challenge, which hinders the large-scale application of powder photocatalysts. Inspired by the high sustainability, energy efficiency, and cleanliness of photocatalytic technique in antibiotic degradation, we have developed a stable and efficient ultra-thin porous g-C 3 N 4 /β-phase polyvinylidene fluoride (CA-CNS/β-PVDF) membrane for antibiotics removal. Under the optimal reaction conditions, the tetracycline (TC) removal rate of the membrane reached 93.12 % within 2 h due to the synergistic effect of the embedded ultra-thin porous g-C 3 N 4 and β-phase polyvinylidene fluoride (PVDF). The CA-CNS/β-PVDF membrane still maintained excellent photocatalytic performance after five cycles, showing good stability and reusability. The electron paramagnetic resonance (EPR) and free radical quenching analyses suggest that the TC degradation efficiency is enhanced by the synergistic effect of free radical-non-free radical mixed pathways (•O 2 , •OH, h + , 1 O 2 ) and 1 O 2 plays an important role in the degradation process. The excellent photocatalytic antibiotics degradation performances of CA-CNS/β-PVDF membrane were still obtained in actual water samples under natural sunlight, suggesting its great application potentials. The photocatalytic mechanism, possible degradation intermediates, and degradation pathways are elucidated based on the theoretical calculations and experiments. The toxicity analysis by QSAR shows that the CA-CNS/β-PVDF membrane successfully reduces the biological toxicity of three antibiotics (TC, OTC, CIP) during the photocatalysis. In all, our work provides a universal immobilization technique of powdered photocatalysts to improve their wastewater purification efficiencies.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Fei Bi,Zhemei Zheng,Rongrong Li,Ruiying Du,Li Zhao,Shanshan Xiao,Liyan Wang,Xiangting Dong
Photocatalytic composite membranes (BPMs) are preferred materials for wastewater treatment due to their high photocatalytic activity and ease of recovery. However, conventional blending modification methods for preparing BPMs often lead to drawbacks such as uneven distribution of photocatalysts, low loading efficiency, facile detachment of photocatalysts, poor reusability, and a limited specific surface area of the membranes. These issues significantly diminish their photocatalytic activity and restrict their practical applications. To address these challenges, this thesis introduces a novel preparation method for PVP-modified PVDF/BiOBr photocatalytic membranes, using a combination of electrospinning and solvothermal techniques. This approach enhances the stability of BiOBr microspheres on the PVDF nanofiber membranes, effectively tackling the issue of loading powder photocatalysts. These membranes, composed of PVDF nanofibers and uniformly sized BiOBr microspheres, exhibit a significant specific surface area of 15.69 m 2 /g. The modified PVDF/BiOBr photocatalytic membranes demonstrate remarkable degradation efficiencies: 100 % degradation of Rhodamine B (RhB) in 25 min, 93.8 % degradation of tetracycline (TC) in 30 min, and 74.6 % degradation of hexavalent chromium ions (Cr 6+ ) in 60 min. Moreover, after five cyclic experiments, the photocatalytic degradation rate of sample M 3 remains above 99 % with a minimal loss rate of only 0.5 %. The method developed for preparing PVDF/BiOBr photocatalytic membranes represents a universally applicable and straightforward strategy for fabricating advanced membrane materials. This preparation technique not only provides innovative design ideas and fabrication methods for new photocatalytic materials but also extends to other functional materials. The PVDF/BiOBr photocatalytic membrane materials hold great promise in offering technical and theoretical support for photocatalytic wastewater treatment.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2025
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IF 6.3
Yanhua Cui,Yixuan Hong,Weilong Shi,Zengkai Wang
Background Photocatalytic membrane technology has attracted widespread concern in the field of water purification due to its high-efficiency and eco-friendly. However, the active sites of photocatalyst are easily embedding in the polymer membrane, consequently reducing degradation efficiency of photocatalytic membrane. Methods In this study, two-dimensional/two-dimensional regenerated silk fibroin-carbonized carbon modified graphite carbon nitride/bismuth vanadate heterojunction (2D/2D C-g-C 3 N 4 /BiVO 4 ) with excellent photocatalytic performance was synthesized by electrostatic self-assembly method. Then C-g-C 3 N 4 /BiVO 4 heterojunction was selected as catalytic structural units, three-dimensional (3D) interfacial networked poly(vinylidene fluoride) membrane-supported C-g-C 3 N 4 /BiVO 4 heterojunction (C-g-C 3 N 4 /BiVO 4 /PVDF) was fabricated by electrospinning technique. The combination of C-g-C 3 N 4 /BiVO 4 heterojunction and interfacial networked PVDF membrane synergistically enhanced their permeability, antifouling and antibacterial performance. Significant findings The optimized C-g-C 3 N 4 /BiVO 4 /PVDF photocatalytic membrane had higher degradation TC efficiency (83.33 %) than other membrane samples, and the efficiency of bacterial inactivation of C-g-C 3 N 4 /BiVO 4 /PVDF could reach 99.00 %. The C-g-C 3 N 4 /BiVO 4 /PVDF exhibited tremendous enhancement in the permeability (13,488.2 L m −2 h −1 ) and flux recovery efficiency (94.44 %). The free radical trapping tests and ESR spectra indicated that superoxide radical (·O 2 ⁻ ) was the dominant active species. In addition, the as-prepared C-g-C 3 N 4 /BiVO 4 /PVDF could easily recover and reuse, and photocatalytic activity basically remain unchanged, highlighting the potential application of membrane photocatalyst for the practical wastewater treatment.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Hao Yang,Baikang Zhu,Lijing Zhu,Zhixiang Zeng,Gang Wang,Zhu Xiong
A photocatalytic membrane with significant degradation and antifouling performance has become an important part in wastewater treatment. However, the low catalyst loading on the polymer membrane limits its performance improvement. Herein, we fabricated poly(vinylidene fluoride) (PVDF) and poly(acrylic acid) (PAA) blend membranes with a rough surface via a vapor-induced phase separation (VIPS) process. Then Fe3+ was cross-linked with the carboxyl groups on the membrane surface and further in situ mineralized into β-FeOOH nanorods. The resultant membranes exhibit not only hydrophilicity and underwater superoleophobicity but also favorable separation efficiency and high water flux in oil-in-water emulsions separation. Under visible light irradiation, the membrane can degrade methylene blue (MB) to 95.2% in 180 min. More importantly, the membrane has a significant photocatalytic self-cleaning ability for crude oil with a flux recovery ratio (FRR) as high as 94.1%. This work brings a new strategy to fabricate the rough and porous surface for high loading of the hydrophilic photo-Fenton catalyst, improving the oil/water emulsion separation and antifouling performance of the membranes.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMOSPHERE
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2019
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IF 5.108
Yahui Shi,Jinhui Huang,Guangming Zeng,Wenjian Cheng,Jianglin Hu,Lixiu Shi,Kaixin Yi
Photocatalytic membranes (PMs), coupling of membrane filtration and photocatalysis , have exhibited the potential for application in the wastewater treatment . In this study, we firstly adopted the supramolecular aggregates of melamine (M), cyanuric acid (C), and urea (U) in specific dimethyl sulfoxide (DMSO) as precursors to prepare carbon nitride MCU-C 3 N 4 with high photocatalytic performance, and a kind of novel-designed photocatalytic membrane was prepared via filtrating the mixture of graphene oxide (GO) nanosheets and MCU-C 3 N 4 on PVDF membrane supports, and then crosslinked using glutaraldehyde (GA) to construct a steady coating on the GO/MCU-C 3 N 4 /PVDF membrane. GO/MCU-C 3 N 4 /PVDF composite membrane exhibited higher permeation flux than that of GO/PVDF membrane and exhibited excellent separation performance for oil-in-water emulsion. A visible light-driven self-cleaning four-stage filtration by a self-built dead-end filtration system was carried out to evaluate membrane antifouling property, and GO/MCU-C 3 N 4 /PVDF membrane (M2) possessed higher flux recovery ratio (FRR) (∼92.36%) and lower irreversible fouling resistance (R ir ) ratio (∼8%) under 30min visible-light irradiation, maintaining relatively higher FRR (>72%) during 4 cycling of four-stage filtrating experiments. GO/MCU-C 3 N 4 /PVDF PMs are equipped with high permeation flux, separation performance, anti-fouling property and stability, indicating potential application in water treatment .
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ACS ES&T Water
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2024
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IF 4.8
Kang Xu,Yi Tu,Yanhong Feng,Xiaochun Yin,Guizhen Zhang
This paper presents a highly efficient method for preparing ultrathin, high-strength photocatalytic membranes with a three-layer structure and high-loading catalysts on both sides. The photocatalytic membranes were prepared by simultaneous biaxial stretching using ultrahigh-molecular-weight polyethylene as the matrix, TiO2 nanoparticles as the catalyst (80 wt %), and liquid paraffin as the plasticizer. The mechanical properties of these membranes were tested, and the tensile strength of the membrane with a biaxial stretching ratio of 7 × 7 reached 62 MPa. Three types of dyes, methyl orange, methylene blue, and Congo red, and their mixed solutions were selected as model pollutants to investigate the photocatalytic properties of the prepared photocatalytic membranes. Results show that the 7 × 7 membrane can almost degrade the above pollutants within 100 min. Moreover, this membrane exhibits remarkable stability in cyclic photodegradation tests, with a degradation rate reaching 95.9% after five cycles. This preparation method is anticipated to provide a good carrier for various photocatalysts, making the photocatalytic membrane suitable for a wide range of applications in the treatment of water contamination.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Zan Li,Xing Li,Yongwang Liu,Zhiwei Zhou,Jiawei Ren,Zedong Lu,Jianyong Feng
Membrane fouling induced by natural organic matter (NOM) is a challenge for wider application of photocatalytic membranes (PMs). In this study, Bi 2 O 3 -TiO 2 (BT) and powdered activated carbon (PAC) were coated on the ultrafiltration (UF) membrane surface with sandwich structure (BT/PAC-UF), to mitigate membrane fouling of PMs under the ultraviolet (UV) irradiation. When exposed to UV irradiation, the BT/PAC coating demonstrated superior performance in mitigating membrane fouling, achieving a higher flux recovery rate of 43.1 % and a lower irreversible fouling rate of 57.5 %, compared to individual PAC and BT coating layers. Additionally, after BT/PAC coating under UV irradiation, the removal efficiencies of dissolved organic carbon (DOC), UV 254 , and protein-like fluorescents improved to 63 %, 59 %, and 73.4 %, respectively, and the interfacial energy also increased to 6.30 mJ/m 2 , surpassing that achieved by PAC and BT coatings. In contrast to BT-UF under UV irradiation, the removal efficiencies of low molecular weight (LMW) Acids and Neutrals were increased 21 % and 66 % in BT/PAC-UF, respectively. The Lifshiitz-van der Waals energy (ΔG LW ) had the highest Mantel correlation with the membrane resistance, followed by surface hydrophilicity energy (ΔG sls ). The removal efficiencies of humic-like and protein-like fluorescents showed high negative correlation with ΔG LW and ΔG sls (Pearson’s r = -0.98). The BT/PAC coating can reduce the content of humic-like and protein-like fluorescents, leading to a reduced attraction of the natural organic matter (NOM) to the membrane. Meanwhile, the required volume for the changed from pore blocking to cake filtration was reduced most from 320 ml to 180 ml by the BT/PAC coating. The UF membrane fouling of PMs caused by NOM was mitigated eventually.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Chi Zhang,Yi Li,Jie Li
Waterborne human viruses, with ubiquitous prevalence in aquatic environments, extremely low infectious doses, and high resistance to common disinfection processes, pose a substantial threat to human health. Herein, for the first time, a photocatalytic membrane reactor (PMR) driven by visible light emitting diodes (Vis-LEDs) was applied for effective water disinfection of human adenoviruses. The photocatalyst used in the PMR was selected to be a metal-free heterojunction (named as CNO) with the advantages of visible-light-response, efficient virucidal effects, green properties and easy recovery via microfiltration. The disinfection performance of the Vis-LED PMR towards human adenoviruses was improved by adjusting operation with response surface methodology (RSM). Based on twenty sets of operating data, a semi-empirical model was established with a high accuracy of R 2 = 0.9622 for predicting the final adenovirus inactivation after 300-min operation. The optimal operating solution was found to be 5.00-log MPN/mL, 320.30 mg/L and 502.65 min for initial virus concentration (IVC), photocatalyst loading (PL) and hydraulic retention time (HRT), respectively. Under the optimized operation, all human adenoviruses were completely inactivated without regrowth, accompanied by severe damage to capsids, within 600 min in the Vis-LED PMR. In addition, the CNO photocatalyst could be retained inside the reactor via low-energy microfiltration with excellent recovery (99.9 wt%) but without obvious chemical or structural changes. Our work can offer a simple, effective, economical and eco-friendly water disinfection device against resistant pathogenic microbes, with controllable efficiency by facilely varying operating solutions.
研究领域:
环境科学
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公共卫生
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生物工程
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2023
·Vol. 98
·期 9
·2136-2145
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IF 3.4
Long Wang,Liu-Lin Zhao,Qin-Yuan He,Dan-Dan Shao,Shi-Peng Sun,Xue-Li Cao
BACKGROUND Desalination membranes have been widely in demand for separating dyes and salts. However, dyes are easily adsorbed on/in the membranes, deteriorating membrane performance. Coupling photocatalysis and membrane separation might be a promising strategy for efficiently alleviating membrane fouling. Aiming at the defects of single catalyst, this work constructed photocatalytic membranes based on heterostructured Fe 3 O 4 -doped g-C 3 N 4 (FeCN)/TiO 2 catalysts by successively filtrating FeCN aqueous dispersion and titanium butoxide/isopropanol solution on the hydrolyzed polyacrylonitrile substrate. RESULTS The H-bonds among TiO 2 , FeCN and substrate lead to excellent load stability of the photoresponsive layer. Due to the low-potential conduction band and high conductivity of Fe 3 O 4 and the low-potential conduction band of TiO 2 in FeCN/TiO 2 , electrons can be more easily transferred to guarantee the high separation efficiency of electrons and holes. Hence the membrane not only exhibited superior permeability (104 L m −2 h −1 bar −1 ) and dye desalting performance (Coomassie brilliant blue R250 rejection of >98.80% and NaCl rejection of <7.00%), but also displayed highly efficient and stable dye photodegradation. CONCLUSION The degradation efficiency surpassed that reported in the literature in comparable circumstances, and the recovery rate of permeability still reached 89.12% after three fouling–photodegradation cycles. This work provides new opportunities for designing high-efficiency self-cleaning membranes to solve membrane fouling based on low-cost materials. © 2023 Society of Chemical Industry (SCI).
研究领域:
材料科学
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环境工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qieyuan Gao,Bo Weng,Pengrui Jin,Shushan Yuan,Xiahui Gui,Junfeng Zheng,Daliang Xu,Yue Wang,Alexander Volodine,Li Sun,Bart Van der Bruggen
Separation of dyes and salts from textile wastewater is essential for the secondary utilization of resources. Here in, with supramolecular β-cyclodextrin (β-CD) and mussel-inspired polydopamine (pDA) as building blocks, an super-selectiveand highly water permeable photocatalytic membrane with a stable intermediate layer of AgBr-Ag 3 PO 4 photocatalyst was developed by in-situ formation of AgBr-Ag 3 PO 4 photocatalyst via in-situ formation, in which the β-CD with an inherent cavity was used to formed honeycomb microstructures via host–guest interaction with pDA. The optimized photocatalytic membrane, demonstrated a superior-separation performance with a water permeance of 101.3 LMH bar −1 , while achieved a high rejection of all tested dyes of up to 99% and high salt transport of from synthetic dyes textile wastewater. Under visible light, the AgBr-Ag 3 PO 4 layer exhibited ∼ 100% degradation of dyes attaching on the membrane surface, endowing the membrane with excellent photocatalytic self-cleaning ability. Combining with material and membrane characterization, the separation performance of the membrane was rationalized, demonstrating the advantages of the host–guest interaction between β-CD and pDA and in-situ photocatalytic functionalization. This study guides the rapid separation of angstrom-sized molecules in the membrane separation process.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Guodong Tian,Chao Duan,Shasha Che,Baoke Zhao,Bingxu Zhou,Yonghao Ni
Advanced oxidation processes have extensive applications in the degradation of organic pollutants in wastewater. However, conventional powder photochemical catalysts have limited utility due to their susceptibility to agglomeration, electron-hole recombination, and challenges in recycling. In this work, we herein propose an integration tactic to facilely fabricate a cellulose-based photocatalytic electrospun membrane (ZPP/CA-ENM) via synchronous electrospinning of acetate cellulose (CA) and electrospray of core-shell PMMA@PDA@ZIF-67 (ZPP) photocatalysts. This hybrid membrane is capable of synergistic PMS activation and photocatalytic degradation of tetracycline (TC) and methylene blue (MB). For the ZPP catalysts, the PDA@ZIF-67 heterojunctions greatly promote the adsorption of visible light and the separation of photogenerated electron-hole pairs, leading to excellent catalytic efficiency. The synchronous electrospinning and electrospray not only lead to the formation of porous and spiderweb-like membrane structure, but also facilitates the dispersion and recycling of these catalysts. Results reveal that under the presence of light irradiation and PMS, various oxidative species, including 1 O 2 , SO 4 − , OH and O 2 − are generated, resulting in rapid degradations of TC (93.31 % within 30 min) and MB (99.90 % within 15 min), which also exhibits a rapid degradation and high efficiency in a cascade continuous lab setup. This work provides a new strategy for exploring novel and efficient material for wastewater purification.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
OPTICAL MATERIALS
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2021
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IF 3.08
Xuyang Li,Zongxue Yu,Liangyan Shao,Xiaofang Feng,Haojie Zeng,Yuchuan Liu,Runxuan Long,Ximei Zhu
In order to effectively solve the two major problems of photocatalyst recovery and membrane fouling , this research combines photocatalyst and membrane separation technology . In this study, the NH 2 -MIL-88B(Fe)/CDs@GO material with good photocatalytic properties was synthesized by hydrothermal method and mechanical stirring, and the photocatalytic membrane was obtained by vacuum filtration. The results show that the NH 2 -MIL-88B(Fe)/CDs@GO membrane can effectively intercept and degrade methylene blue (MB). After 10 cycles, the rejection rate of MB can still reach 99.5%, which is about 2.5 times of pure GO membrane (40%). After 15 min of visible light irradiation, the Flux recovery rate (FRR) of NH 2 -MIL-88B(Fe)/CDs@GO membrane can reach 95%, and the antifouling performance is excellent. In this study, the composite photocatalytic membrane shows excellent stability, photocatalytic performance and self-cleaning property, which is conducive to widening the application prospect of wastewater treatment .
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）