通过溶剂热法合成了一系列新型铁掺杂UIO-66纳米材料(xFe-UIO-66),并进行X射线衍射(XRD)、扫描电镜(SEM)、红外光谱(FT-IR)、N2吸附脱附等温线等表征及用于水中盐酸四环素(TCH)吸附。通过静态吸附实验,考察了Fe掺杂量、pH、反应温度、吸附剂添加量等对吸附性能的影响,结果表明:当Fe∶Zr=0.8∶1(摩尔比)时(0.8Fe-UIO-66),在TCH初始浓度为20mg/L,温度298K,吸附剂投加量为0.3g/L条件下,0.8Fe-UIO-66对TCH的吸附性能最好、去除率可达到99.64%,最大吸附量为227.45mg/g。此外,共存离子实验中发现,在含有Cl-、NO-3、SO2-4、CO2-3的水体中,0.8Fe-UIO-66仍具有较强的吸附TCH能力,吸附机理涵盖有离子间静电作用、芳香环间π-π相互作用,吸附过程符合准二级动力学和Freundlich模型,5次循环实验后依然保持80%吸附性能。
A series of novel Fe-doped UIO-66 (xFe-UIO-66) nanoparticles were synthesized by solvothermal method,and were characterized by XRD,SEM,FT-IR,N2-adsorption/desorption isotherms.The xFe-UIO-66 nanoparticles were utilized for the adsorption of tetracycline hydrochloride (TCH) in water.The effects of Fe doping amount,pH value,reaction temperature and adsorbent dosage on the adsorption performance were investigated by static adsorption experiments.The results revealed that when Fe∶Zr=0.8∶1 (molar ratio) (0.8Fe-UIO-66),the initial TCH concentration was 20mg/L,temperature was 298K,and adsorbent dosage was 0.3g/L,0.8Fe-UIO-66 exhibited the best adsorption performance for TCH,and the removal rate and the maximum adsorption capacity of 0.8Fe-UIO-66 for TCH could reach 99.64% and 227.45mg/g.Furthermore,the coexisting ion experiments exhibited that 0.8Fe-UIO-66 displayed excellent adsorption ability in the presence of Cl-,NO-3,SO2-4 and CO2-3.The main adsorption mechanism included electrostatic interaction,π-π interaction between aromatic rings.The adsorption process conformed to the pseudo-second-order kinetic model and Freundlich model.After five cycles of experiments,the adsorption performance still maintained 80%.
[1] Yang C,Zhu Y M,Wang J,et al.A novel granular MOF composite with dense and ordered MIL-100(Fe) nanoparticles grown on porous alumina:green synthesis and enhanced adsorption of tetracycline hydrochloride[J].Chemical Engineering Journal,2021,426:131724.
[2] Abejon R,De Cazes M,Belleville M P,et al.Large-scale enzymatic membrane reactors for tetracycline degradation in WWTP effluents[J].Water Research,2015,73:118-131.
[3] Yang J,Lin Y,Yang X,et al.Degradation of tetracycline by immobilized laccase and the proposed transformation pathway[J].Journal of Hazardous Materials,2017,322:525-531.
[4] Khan M H,Bae H,Jung J Y.Tetracycline degradation by ozonation in the aqueous phase:proposed degradation intermediates and pathway[J].Journal of Hazardous Materials,2010,181:659-665.
[5] Liu Z M,Zhu M F,Zhao L,et al.Aqueous tetracycline degradation by coal-based carbon electrocatalytic filtration membrane:effect of nano antimony-doped tin dioxide coating[J].Chemical Engineering Journal,2017,314:59-68.
[6] Wang D B,Jia F Y,Wang H,et al.Simultaneously efficient adsorption and photocatalytic degradation of tetracycline by Fe-based MOFs[J].Journal of Colloid and Interface Science,2018,519:273-284.
[7] Homem V,Santos L.Degradation and removal methods of antibiotics from aqueous matrices—a review[J].Journal of Environmental Management,2011,92:2304-2347.
[8] Nadar S S,Vaidya L,Maurya S,et al.Polysaccharide based metal organic frameworks (polysaccharide-MOF):a review[J].Coordination Chemistry Reviews,2019,396:1-21.
[9] Yang Z H,Cao J,Chen Y P,et al.Mn-doped zirconium metal-organic framework as an effective adsorbent for removal of tetracycline and Cr(Ⅵ) from aqueous solution[J].Microporous and Mesoporous Materials,2019,277:277-285.
[10] Cao J,Yang Z H,Xiong W P,et al.One-step synthesis of Co-doped UIO-66 nanoparticle with enhanced removal efficiency of tetracycline:simultaneous adsorption and photocatalysis[J].Chemical Engineering Journal,2018,353:126-137.
[11] Hu Q,Cao J,Yang Z H,et al.Fabrication of Fe-doped cobalt zeolitic imidazolate framework derived from Co(OH)2 for degradation of tetracycline via peroxymonosulfate activation[J].Separation and Purification Technology,2021,259:118059.
[12] Fu G D,Wu P,Yang J G,et al.Cr-doped UIO-66 with enhanced water adsorption for adsorption heat transformation[J].Microporous and Mesoporous Materials,2022,331:111642.
[13] Saleem H,Rafique U,Davies R P.Investigations on post-synthetically modified UIO-66-NH 2 for the adsorptive removal of heavy metal ions from aqueous solution[J].Microporous and Mesoporous Materials,2016,221:238-244.
[14] Xiao L,Xiong Y,Tian S D,et al.One-dimensional coordination supramolecular polymer [Cu(bipy)(SO4)]n as an adsorbent for adsorption and kinetic separation of anionic dyes[J].Chemical Engineering Journal,2015,265:157-163.
[15] Shi Y Y,Yang Z W,Wang B,et al.Adsorption and photocatalytic degradation of tetracycline hydrochloride using a palygorskite-supported Cu2O-TiO2 composite[J].Applied Clay Science,2016,119:311-320.
[16] Liang J,Fang Y,Luo Y,et al.Magnetic nanoferromanganese oxides modified biochar derived from pine sawdust for adsorption of tetracycline hydrochloride[J].Environmental Science and Pollution Research International,2019,26:5892-5903.
[17] Deng R,Huang D,Zeng G,et al.Decontamination of lead and tetracycline from aqueous solution by a promising carbonaceous nanocomposite:interaction and mechanisms insight[J].Bioresource Technology,2019,283:277-285.
[18] Zhang P,Li Y,Cao Y,et al.Characteristics of tetracycline adsorption by cow manure biochar prepared at different pyrolysis temperatures[J].Bioresource Technology,2019,285:121348.
[19] Shan H R,Si Y,Yu J Y,et al.Facile access to highly flexible and mesoporous structured silica fibrous membranes for tetracyclines removal[J].Chemical Engineering Journal,2021,417:129211.
[20] Liu Y,Li J,Wu L,et al.Magnetic spent bleaching earth carbon (Mag-SBE@C) for efficient adsorption of tetracycline hydrochloride:response surface methodology for optimization and mechanism of action[J].The Science of the Total Environment,2020,722:137817.
[21] Oveisi M,Asli M A,Mahmoodi N M.MIL-Ti metal-organic frameworks(MOFs) nanomaterials as superior adsorbents:synthesis and ultrasound-aided dye adsorption from multicomponent wastewater systems[J].Journal of Hazardous Materials,2018,347:123-140.
[22] Lin S,Wang G X,Na Z Y,et al.Long-root Eichhornia crassipes as a biodegradable adsorbent for aqueous As(Ⅲ) and As(Ⅴ)[J].Chemical Engineering Journal,2012,183:365-371.
PDF
