采用共沉淀法制备了氧化生物炭(OBC)-水滑石(LDHs)纳米颗粒, 通过相转化法将其负载在聚醚砜(PES)膜中, 得到OBC-LDHs纳米颗粒杂化聚醚砜(OBC-LDHs/PES)复合膜。通过傅里叶变换红外光谱仪、X射线衍射仪、全自动比表面积及孔隙率分析仪、扫描电子显微镜对复合膜进行了表征, 并测试了其拉伸性能。结果表明:OBC-LDHs/PES复合膜具有良好的机械性能和亲水性;当膜内负载质量分数4.76%的OBC-LDHs、1mmol/L过氧单硫酸氢钾(PMS)和0.05mmol/L金橙G(OG)时, 20min内复合膜对OG的去除率可达98.47%。OBC-LDHs/PES复合膜的金属离子浸出量小于其他催化材料, 重复使用4次, 复合膜仍具有良好的催化性能。自由基捕获实验和X射线光电子能谱分析证明, OBC-LDHs/PES/PMS体系同时含有硫酸根自由基(SO·-4)和单线态氧自由基(1O2), 其中 1O2在OG降解中发挥了重要作用。
Oxidized biochar (OBC)-hydrotalcite (LDHs) nanoparticles were prepared by coprecipitation method, and then loaded into polyethersulfone (PES) membranes by phase inversion method to obtain OBC-LDHs nanoparticles hybrid polyethersulfone composite membranes (OBC-LDHs/PES).The products were characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), fully automatic specific surface area, porosity analyzer (BET), and scanning electron microscopy (SEM), and their tensile properties were tested.The results showed that the OBC-LDHs/PES membranes had excellent mechanical property and hydrophilicity.As the mass fraction of OBC-LDHs doped in the membrane was 4.76%, and the dosage of PMS and OG was 1mmol/L and 0.05mmol/L, respectively, the removal rate of orange G(OG) could reach 98.47% within 20 minutes.The metal ion leaching of the OBC-LDHs/PES was much less than that of other catalytic materials, and the OBC-LDHs/PES still showed good catalytic performance after four repeated uses.Radical trapping experiments and XPS analysis demonstrated that sulfate radical (SO·-4) and singlet oxygen radical(1O2) were simultaneously produced in the OBC-LDHs/PES/PMS system, among which 1O2 played an important role in the degradation of OG.
[1] Zhai X,Chen X,Shi X,et al.Simultaneously enhancing purification,catalysis and in situ separation in a continuous cross-flow catalytic degradation process of multi-component organic pollutants by a double-layer PVDF composite membrane[J].Journal of Environmental Chemical Engineering,2022,10(2):107160-107174.
[2] Karim A V,Hassani A,Eghbali P,et al.Nanostructured modified layered double hydroxides (LDHs)-based catalysts:a review on synthesis,characterization,and applications in water remediation by advanced oxidation processes[J].Current Opinion in Solid State and Materials Science,2022,26(1):100965-100991.
[3] Ma R,Yan X,Mi X,et al.Enhanced catalytic degradation of aqueous doxycycline (DOX) in Mg-Fe-LDH@biochar com-posite-activated peroxymonosulfate system:performances,degradation pathways,mechanisms and environmental implications[J].Chemical Engineering Journal,2021,425:131457-131471.
[4] Gholami P,Khataee A,Soltani R D C,et al.Photocatalytic degradation of gemifloxacin antibiotic using Zn-Co-LDH@biochar nanocomposite[J].J Hazard Mater,2020,382:121070-121082.
[5] Wang T,De Vos W M,De Grooth J.CoFe2O4-peroxymonosulfate based catalytic UF and NF polymeric membranes for naproxen removal:the role of residence time[J].Journal of Membrane Science,2022,646:120209-120219.
[6] Abdel-Karim A,Ismail S H,Bayoumy A M,et al.Antifouling PES/Cu@Fe3O4 mixed matrix membranes:quantitative structure-activity relationship (QSAR) modeling and wastewater treatment potentiality[J].Chemical Engineering Journal,2021,407:126501-126515.
[7] Li B,Chen X,Ma Y,et al.Catalytic behavior of a thermo-responsive PVDF/microgel@Pd membrane for 2-nitroaniline degradation[J].Journal of Environmental Chemical Engineering,2021,9(2):104757-104769.
[8] Yue R,Sun X.A self-cleaning,catalytic titanium carbide (MXene) membrane for efficient tetracycline degradation through peroxymonosulfate activation:performance evaluation and mechanism study[J].Separation and Purification Technology,2021,279:119796-119807.
[9] Huang Z H,Zhang X,Wang Y X,et al.Fe3O4/PVDF catalytic membrane treatment organic wastewater with simultaneously improved permeability,catalytic property and anti-fouling[J].Environ Res,2020,187:109617-109625.
[10] Zhang Y,Song Q,Liang X,et al.High-flux,high-selectivity loose nanofiltration membrane mixed with zwitterionic functionalized silica for dye/salt separation[J].Applied Surface Science,2020,515:146005-146014.
[11] Legentil P,Leroux F,Therias S,et al.Reliability study under thermal and photonic stresses of sulforhodamine B (SRB) confined in layered double hydroxide (LDH)[J].Applied Clay Science,2021,201:105922-105933.
[12] Wei J,Bi J,Zhang L,et al.Gravity-driven Fe-doped CoTiO3/SiO2 fiber membrane with open catalytic network:activation of peroxymonosulfate and efficient pollutants removal[J].Separation and Purification Technology,2022,280:119975-119987.
[13] Li B,Wang Y F,Zhang L,et al.Enhancement strategies for efficient activation of persulfate by heterogeneous cobalt-containing catalysts:a review[J].Chemosphere,2021,291:132954-132968.
[14] Zheng X,Niu X,Zhang D,et al.Metal-based catalysts for persulfate and peroxymonosulfate activation in heterogeneous ways:a review[J].Chemical Engineering Journal,2022,429:132323-132345.
[15] Ma Q,Nengzi L C,Li B,et al.Heterogeneously catalyzed persulfate with activated carbon coated with CoFe layered double hydroxide (AC@CoFe-LDH) for the degradation of lomefloxacin[J].Separation and Purification Technology,2020,235:116204-116214.
基金资助
苏州区域水质改善和水生态安全技术与综合示范项目(2017ZX07205);苏州市产业化前瞻项目(SYG201744)
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