将具有芬顿催化活性的普鲁士蓝类似物Fe-Co PBA负载到聚偏氟乙烯(PVDF)膜内,采用浸没沉淀相转化法制备了一种新型PVDF催化膜,用于去除水中盐酸四环素污染物。结果表明:负载Fe-Co PBA纳米粒子既能提高PVDF膜表面亲水性、孔隙率和水通量,又能赋予PVDF膜催化活性;当Fe-Co PBA负载量为10%(质量分数)时,PVDF催化膜的纯水通量达到418.47L/(m2·h),与纯PVDF膜相比提高了3.24倍。PVDF催化膜具有优异的抗生素去除性能和催化稳定性,当H2O2浓度为400mmol/L时,基于芬顿反应的PVDF催化膜对质量浓度20mg/L盐酸四环素的去除率达到90%;重复使用10次后,PVDF催化膜对盐酸四环素去除率仍保持在85%以上。
A novel polyvinylidene Fluoride (PVDF) catalytic membrane was prepared by loading Fe-Co PBA,a Prussian blue analogue with Fenton's catalytic activity,into polyvinylidene fluoride (PVDF) membrane using immersion precipitation phase transformation method for the removal of tetracycline hydrochloride pollutants in water.The results showed that the loading of Fe-Co PBA nanoparticles could both improve the hydrophilicity,porosity,and water flux of PVDF membrane,and endow the catalytic activity of PVDF membrane.As the Fe-Co PBA loading was 10wt%,the pure water flux of the PVDF catalytic membrane reached 418.47L/(m2·h),which was 3.24 times higher than that of the pure PVDF membrane.The PVDF catalytic membrane presented outstanding antibiotic removal efficiency and catalytic stability in treating wastewater containing tetracycline hydrochloride.When the concentration of H2O2 was 400mmol/L and the initial concentration of tetracycline hydrochloride was 20mg/L,the PVDF catalytic membrane based on the Fenton reaction presented 90% tetracycline hydrochloride removal efficiency.After ten times reuses,the removal efficiency of the catalytic membrane still remained above 85%.
[1] Wang X N,Jia J P,Wang Y L.Combination of photocatalysis with hydrodynamic cavitation for degradation of tetracycline[J].Chem Eng J,2017,315:274-282.
[2] Dai Y J,Liu M,Li J J,et al.A review on pollution situation and treatment methods of tetracycline in groundwater[J].Sep Sci Technol,2020,55(5):1005-1021.
[3] Anjali R,Shanthakumar S.Insights on the current status of occurrence and removal of antibiotics in wastewater by advanced oxidation processes[J].J Environ Manage,2019,246:51-62.
[4] Li S,Wu Y A,Zheng H S,et al.Antibiotics degradation by advanced oxidation process (AOPs):recent advances in ecoto-xicity and antibiotic-resistance genes induction of degradation products[J].Chemosphere,2023,311:136977.
[5] Jung H,Park H,Kim J,et al.Preparation of riotic and abiotic iron oxide nanoparticles (ionps) and their properties and applications in heterogeneous catalytic oxidation[J].Environ Sci Technol,2007,41(13):4741-4747.
[6] Li N,Chen G Y,Zhao J H,et al.Self-cleaning PDA/ZIF-67@pp membrane for dye wastewater remediation with peroxy-monosulfate and visible light activation[J].J Membr Sci,2019,591:117341.
[7] Xie R,Luo F,Zhang L,et al.A novel thermoresponsive catalytic membrane with multiscale pores prepared via vapor-induced phase separation[J].Small,2018,14(18):1703650.
[8] Hatat-Fraile M,Liang R,Arlos M J,et al.Concurrent photocatalytic and filtration processes using doped TiO2 coated quartz fiber membranes in a photocatalytic membrane reactor[J].Chem Eng J,2017,330:531-540.
[9] Zhang L P,Liu Z,Zhou X L,et al.Novel composite membranes for simultaneous catalytic degradation of organic contaminants and adsorption of heavy metal ions[J].Sep Purif Technol,2020,237:116364.
[10] Sajjadi A,Ravandi S,Izadan H,et al.Purification of methylene blue via photocatalytic nanofibrous membranes containing TiO2 nanoparticles[J].J Eng Fiber Fabr,2016,11(4):43-55.
[11] Simonov A,de Baerdemaeker T,Bostrom H,et al.Hidden diversity of vacancy networks in prussian blue analogues[J].Nature,2020,578(7794):256.
[12] Nai J W,Lou X W.Hollow structures based on prussian blue and its analogs for electrochemical energy storage and conversion[J].Adv Mater,2019,31(38):1706825.
[13] Li X N,Liu J Y,Rykov A I,et al.Excellent photo-fenton catalysts of Fe-Co prussian blue analogues and their reaction mechanism study[J].Appl Catal B,2015,179:196-205.
[14] Liu J Y,Li X N,Liu B,et al.Shape-controlled synthesis of metal-organic frameworks with adjustable fenton-like cataly-tic activity[J].ACS Appl Mater Interfaces,2018,10(44):38051-38056.
[15] Ayers J B,Waggoner W H.Synthesis and properties of two series of heavy metal hexacyanoferrates[J].Journal of Inorganic and Nuclear Chemistry,1971,33(3):721-733.
[16] Wang G W,Wang D,Dong X L,et al.Sodium persulfate based PVDF membrane for concurrent advanced oxidation and ultrafiltration of ofloxacin in water[J].Chem Eng J,2017,315:509-515.
基金资助
国家自然科学基金面上项目(22278177)
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