以铜离子为金属中心,1,3,5-苯甲酸和4,4′-联吡啶为有机配体,构建羧酸、吡啶双配体金属-有机框架(MOFs)材料。通过傅里叶变换红外光谱仪、扫描电子显微镜和X射线衍射仪对铜基MOFs材料Cu3(BTC)2和双配体MOFs材料进行了表征。结果表明:双配体MOFs材料在酸性条件下表现出良好的吸附性能,该材料对Cr(Ⅵ)的吸附更符合准二级动力学方程和Freundlich等温吸附方程。经过5次吸附-解吸循环后,吸附量基本恒定,该材料可以重复使用。
Based on Cu-BTC metal-organic frameworks(MOFs),double-ligand functionalized materials were prepared.Then,the Cu3(BTC)2 and the functionalized materials were characterized by FT-IR,SEM and X-ray diffraction analysis.The adsorption properties of the functionalized materials for Cr(Ⅵ) were investigated.The functionalized materials shown good adsorption under acidic conditions.Through adsorption model analysis,the adsorption of Cr(Ⅵ) by the functionalized materials were more in line with the pseudo-second-order kinetic equation and Freundlich isothermal equation.After five adsorption-desorption cycles,the adsorption capacity was basically constant and the materials can be reused.The results shown that the functionalized MOFs had good application prospects in the adsorption and removal of heavy metal Cr(Ⅵ) in aqueous solution.
[1] Zhang C,Xia F,Long J,et al.An integrated technology to minimize the pollution of chromium in wet-end process of leather manufacture[J].Journal of Cleaner Production,2017,154(15):276-283.
[2] Paul D.Research on heavy metal pollution of river Ganga:a review[J].Annals of Agrarian Science,2017,15(2):278-286.
[3] Chen S,Yue Q,Gao B,et al.Removal of Cr(Ⅵ) from aqueous solution using modified corn stalks:characteristic,equilibrium,kinetic and thermodynamic study[J].Chemical Enginee-ring Journal,2011,168(2):909-917.
[4] Gheju M,Balcu I.Assisted green remediation of chromium pollution[J].Journal of Environmental Management,2017,203(3):920-924.
[5] Jin X Y,Liu Y,Jeanette T,et al.Removal of Cr(Ⅵ) from aqueous solutions via reduction and absorption by green synthesized iron nanoparticles[J].Journal of Cleaner Production,2018,176:929-936.
[6] Mirbagheri S A,Hosseini S N.Pilot plant investigation on petrochemical waste water treatment for the removal of copper and chromium with the objective of reuse[J].Desalination,2005,171(1):85-93.
[7] Pulkka S,Martikainen M,Bhatnagar A,et al.Electrochemical methods for the removal of anionic contaminants from water-a review[J].Separation & Purification Technology,2014,132:252-271.
[8] Cifuentes L,García I,Arriagada P,et al.The use of electrodialysis for metal separation and water recovery from CuSO4-H2SO4-Fe solutions[J].Separation & Purification Technology,2009,68(1):105-108.
[9] Kononova O N,Bryuzgina G L,Apchitaeva O V,et al.Ion exchange recovery of chromium(Ⅵ) and manganese(Ⅱ) from aqueous solutions[J].Arabian Journal of Chemistry,2019(12):2713-2720.
[10] Wahid F,Mohammadzai I U,Khan A,et al.Removal of toxic metals with activated carbon prepared from salvadora persica[J].Arabian Journal of Chemistry,2017,10(S2):2205-2212.
[11] Liu X L,Ma R,Wang X X,et al.Graphene oxide-based materials for efficient removal of heavy metal ions from aqueous solution:a review[J].Environ Pollut,2019,252:62-73.
[12] Yurekli Y.Removal of heavy metals in waste water by using zeolite nano-particles impregnated polysulfone membranes[J].Hazard Mater,2016,309:53-64.
[13] Anirudhan T S,Jalajamony S,Sreekumari S S.Adsorption of heavy metal ions from aqueous solutions by amine and carboxylate functionalised bentonites[J].Applied Clay Science,2012,65-66:67-71.
[14] Zhu B,Fan T,Zhang D.Adsorption of copper ions from aqueous solution by citric acid modified soybean straw[J].Journal of Hazardous Materials,2008,153(1/2):300-308.
[15] Wu Y H,Pang H W,Liu Y,et al.Environmental remediation of heavy metal ions by novel-nanomaterials:a review[J].Environmental Pollution,2019,246:608-620.
[16] Duan X,Wang H,Ji Z,et al.A novel metal-organic framework for high storage and separation of acetylene at room temperature[J].Journal of Solid State Chemistry,2016,241:152-156.
[17] Chen X Y,Vinh-Thang H,Rodrigue D,et al.Amine-functionalized MIL-53 metal-organic framework in polyimide mixed matrix membranes for CO2/CH4 separation[J].Industrial & Engineering Chemistry Research,2012,51(19):6895-6906.
[18] Wu J,Xu J W,Liu W C,et al.Designed metal corganic framework based on metal corganic polyhedron:drug delivery[J].Inorganic Chemistryunications,2016,71:32-34.
[19] Crawford S E,Ellis J E,Ohodnicki P R,et al.Influence of the anionic zinc-adeninate metal-organic framework structure on the luminescent detection of rare earth ions in aqueous streams[J].ACS Applied Materials & Interfaces,2021,13(6):7268-7277.
[20] Kumar P,Deep A,Kim K H.Metal organic frameworks for sensing applications[J].TrAC Trends in Analytical Chemistry,2015,73:39-53.
[21] Zhang X,Huang P,Liu A,et al.A metal-organic framework for oxidative desulfurization:UIO-66(Zr) as a catalyst[J].Fuel,2017,209(1):417-423.
[22] Jeong Yong Lee,Omark K Farha,John Roberts,et al.Metal-organic framework materials as catalysts[J].Chemical Society Reviews,2009,38(1):1450-1459.
[23] Oisaki K,Li Q,Furukawa H,et al.A metal-organic framework with covalently bound organometallic complexes[J].Journal of the American Chemical Society,2010,132(27):9262-9264.
[24] Omar Farha K,Ibrahim Eryazici,Ozgur Yazaydin A.De novel synthesis of a metal-organic framework material featuring ultrahigh surface area and gas storage capacities[J].Nature Chemistry,2010,2(11):944-948.
[25] Schlichte K,Kratzke T,Kaskel S.Improved synthesis,thermal stability and catalytic properties of the metal-organic framework compound Cu3(BTC)2[J].Microporous & Mesoporous Materials,2004,73(1/2):81-88.
[26] Li H L,Eddaoudi M M,O'Keeffe M,et al.Design and synthesis of an exceptionally stable and highly porous metal-organic framework[J].Nature,1999,402(6759):276-279.
[27] Stöber W,Fink A E,Bohn E.Development of a novel sensitive molecularly imprinted polymer sensor based on electropolymerization of a microporous-metal-organic framework for tetracycline detection in honey[J].Food Control,2016,59:424-429.
[28] Zheng Y,Li Y,Huang L,et al.A facile fabrication of MOF for selective removal of chromium(Ⅲ) from aqueous solution[J].Journal of Dispersion Science and Technology,2019,40:1-7.
[29] Deng Y Y,Xiao X F,Wang D,et al.Adsorption of Cr(Ⅵ) from aqueous solution by ethylenediaminetetraacetic acid-chitosan-modified metal-organic framework[J].Journal of Nanoscience and Nanotechnology,2020,20:1660-1669.
[30] Hu X J,Wang J S,Liu Y G,et al.Adsorption of chromium(Ⅵ) by ethylenediamine-modified cross-linked magnetic chitosan resin:isotherms,kinetics and thermodynamics[J].Journal of Hazardous Materials,2011,185(1):306-314.
[31] Zhang J M,Xiong Z H,Li C,et al.Exploring a thiol-functionalized MOF for elimination of lead and cadmium from aqueous solution[J].Journal of Molecular Liquids,2016,221:43-50.
[32] Nobar,Najafi S.Cu-BTC synthesis,characterization and pre-paration for adsorption studies[J].Materials Chemistry and Physics,2018,213:343-351.
[33] Giselle Autié-Castro,Reguera E,Jr C L C,et al.Surface acid-base properties of Cu-BTC and Fe-BTC MOFs.An inverse gas chromatography and n-butylamine thermo desorption study[J].Inorganica Chimica Acta,2020,507:119590.
[34] Xiao X,Deng Y,Xue J,et al.Adsorption of chromium by functionalized metal organic frameworks from aqueous solution[J].Environmental Technology,2019(1):1-26.
[35] Ahalya N,Kanamadi R D,Ramachandra T V.Biosorption of chromium(Ⅵ) from aqueous solutions by the husk of bengal gram (Cicer arientinum)[J].Electronic Journal of Biotechno-logy Ejb,2005,8(3):258-264.
基金资助
上海市科委地方院校能力建设项目(N19050502000)
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