混合配体Cd-MOF的合成及其光催化降解性能
|
摘要
以四水硝酸镉、均苯三甲酸、乳酸和N,N-二甲基甲酰胺为原料,采用溶剂热合成方法,制备得到混合配体Cd-金属有机框架(MOF)材料。利用偏光显微镜、扫描电子显微镜、热重分析仪、Fourier红外光谱、X射线衍射仪、N_2吸附–脱附分析、紫外–可见漫反射光谱等手段对其进行表征。以亚甲基蓝(MB)溶液为模拟污染物,室温条件下考察了该材料在紫外光下的光催化活性。研究表明:当混合配体Cd-MOF作为光催化剂时,当其用量为70 mg,MB初始浓度为40 mg/L、pH=8～10时,在2 h内降解率可达80%左右,而且混合配体Cd-MOF经过5次循环试验后仍能保持较稳定的光催化活性。
A mixed ligand Cd-MOF hybrid material was prepared by a solvothermal synthesis method using cadmium tetrahydrate tetrahydrate, trimesic acid, lactic acid and N,N-dime-thylformamide as polarizing materials.The as-obtained samples were characterized by polarizing microscopy, X-ray diffraction, scanning electron microscopy and energy dispersive X-ray spectroscopy,Fourier transform infrared spectroscopy, thermogravimetric analysis, N_2 absorption-desorption and ultraviolet-visible diffuse reflection spectroscopy.The methylene blue(MB) was used as a model organic pollutant, and the photocatalytic activity of the hybrid material under ultraviolet light at room temperature was examined.The results show that the degradation rate can reach 80% within 2 h when the mixed ligand Cd-MOF is used as a photocatalyst at the amount of 70 mg, the MB initial concentration of 40 mg/L,and the pH values of 8-10.Furthermore, the mixed ligand Cd-MOF can keep its photocatalytic stability after five recycles.
A mixed ligand Cd-MOF hybrid material was prepared by a solvothermal synthesis method using cadmium tetrahydrate tetrahydrate, trimesic acid, lactic acid and N,N-dime-thylformamide as polarizing materials.The as-obtained samples were characterized by polarizing microscopy, X-ray diffraction, scanning electron microscopy and energy dispersive X-ray spectroscopy,Fourier transform infrared spectroscopy, thermogravimetric analysis, N_2 absorption-desorption and ultraviolet-visible diffuse reflection spectroscopy.The methylene blue(MB) was used as a model organic pollutant, and the photocatalytic activity of the hybrid material under ultraviolet light at room temperature was examined.The results show that the degradation rate can reach 80% within 2 h when the mixed ligand Cd-MOF is used as a photocatalyst at the amount of 70 mg, the MB initial concentration of 40 mg/L,and the pH values of 8-10.Furthermore, the mixed ligand Cd-MOF can keep its photocatalytic stability after five recycles.
引文
[1]DONG C,LU J,QIU B,et al.Developing stretchable and graphene-oxide-based hydrogel for the removal of organic pollutants and metal ions[J].Appl Catal B,2018,222:146-156.
[2]DAYI B,KYZY A D,ABDULOGLU Y,et al.Investigation of the ability of immobilized cells to different carriers in removal of selected dye and characterization of environmentally friendly laccase of Morchella esculenta[J].Dyes Pigments,2018,151:15-21.
[3]GHANEIAN M T,EHRAMPOUSH M H,EHSANZADEH E,et al.Upgrading secondary wastewater plant effluent by modified coagulation and flocculation,for water reuse in irrigation[J].J Water Reuse Desal,2017,7(3):298-306.
[4]MALEKI A,HAYATI B,NAGHIZADEH M,et al.Adsorption of hexavalent chromium by metal organic frameworks from aqueous solution[J].J Ind Eng Chem,2015,28:211-216.
[5]高续春,代宏哲,赵鹏,等.微波法合成的氮化碳光催化降解苯酚及其机理[J].硅酸盐学报,2017,45(10):1503-1509.GAO Lianchun,DAI Hongzhe,ZHAO Peng,et al.J Chin Ceram Soc,2017,45(10):1503-1509.
[6]KAMENEV I,VIIROJA A,KALLAS J.Aerobic bio-oxidation with ozonation for recalcitrant wastewater treatment[J].J Adv Oxid Technol,2016,11(2):338-347.
[7]TEH C Y,BUDIMAN P M,SHAK K P Y,et al.Recent advancement of coagulation-flocculation and its application in wastewater treatment[J].Ind Eng Chem Res,2016,55(16):4363-4389.
[8]ASGHAR A,RAMAN A A A,DAUD W M A W.Advanced oxidation processes for in-situ production of hydrogen peroxide/hydroxyl radical for textile wastewater treatment:a review[J].J Clean Prod,2015,87(2):826-838.
[9]Omorogie M O,Babalola J O,Unuabonah E I,et al.Efficient chromium abstraction from aqueous solution using a low-cost biosorbent:Nauclea diderrichii,seed biomass waste[J].J Saudi Chem Soc,2016,20(1):49-57.
[10]陶丽琴,赵义侠,康卫民,等.聚四氟乙烯超细纤维负载二氧化钛光催化性能[J].硅酸盐学报,2016,44(1):89-94.TAO Liqin,ZHAO Yixia,KANG Weimin,et al.J Chin Ceram Soc,2016,44(1):89-94.
[11]PRAKASH K,KUMAR P S,LATHA P,et al.Design and fabrication of a novel metal-free SiO2/g-C3N4 nanocomposite:A robust photocatalyst for the degradation of organic contaminants[J].J Inorg Organomet P,2018,28(1):268-278.
[12]李翠霞,吴强红,曾鹏飞,等.氧化石墨烯-镝掺杂二氧化钛复合光催化材料的制备及光催化性能[J].硅酸盐学报,2016,44(6):872-877.LI Cuixia,WU Qianghong,ZENG Pengfei,et al.J Chin Ceram Soc,2016,44(6):872-877.
[13]BHATTACHARYA S,BALA S,MONDAL R.Design of chiral Co(Ⅱ)-MOFs and their application in environmental remediation and waste water treatment[J].Rsc Adv,2016,6(30):25149-25158.
[14]NASALEVICH M,BECKER R,FERNANDEZ E V R,et al.Co@NH2-MIL-125(Ti):Cobaloxime-derived metal-organic framework-based composite for light-driven H2 production[J].Energy Environ Sci,2015,8(1):364-375.
[15]BHATTACHARYA S,BALA S,MONDAL R.Design of chiral Co(Ⅱ)-MOFs and their application in environmental remediation and waste water treatment[J].Rsc Adv,2016,6(30):25149-25158.
[16]JHUNG S H,KHAN N A,HASAN Z.Analogous porous metal-organic frameworks:synthesis,stability and application in adsorption[J].Crystengcomm,2012,14(21):7099-7109.
[17]GE Y,LI N Y,JI X Y,et al.Assembly of a series of zinc coordination polymers based on 1,4-bis[2-(4-pyridyl)ethenyl]-2,3,5,6-tetramethylbenzene and 1,3-benzenedicarboxylate derivatives[J].Crystengcomm,2014,16(29):6621-6629.
[18]DAI M,SU X R,WANG X,et al.Three zinc(Ⅱ)coordination polymers based on tetrakis(4-pyridyl)cyclobutane and naphthalenedicarboxylate linkers:Solvothermal syntheses,structures,and photocatalytic properties[J].Cryst Growth Des,2013,14(1):240-248.
[19]YIN W Y,HUANG Z L,TANG X Y,et al.Structural diversification and photocatalytic properties of zinc(Ⅱ)polymers modified by auxiliary N-containing ligands[J].New J Chem,2015,39(9):7130-7139.
[20]DU J Q,DONG J L,XIE F,et al.Syntheses,structures,and properties of three mixed-ligand complexes based on 3,6-bis(imidazole-1-yl)pyridazine[J].J Mol Struct,2019,1175:754-762.
[21]ZHU W,YANG X Y,LI Y H,et al.A novel porous molybdophosphate-based FeⅡ,Ⅲ-MOF showing selective dye degradation as a recyclable photocatalyst[J].Inorg Chem Commun,2014,49:159-162.
[22]QIN L,CHEN H Z,LEI J,et al.Photodegradation of some organic dyes over two metal-organic frameworks with especially high efficiency for safranine T[J].Cryst Growth Des,2017,17(3):1293-1298.
[23]LI H,HE Y,ZHAO W,et al.Designing different functional frameworks from 0D to 3D for exploring structural correlation with photocatalytic activity[J].Polyhedron,2017,133:412-418.
[24]高倩,谢亚勃,张超艳,等.5,6-二羧基苯并咪唑双核铕配合物的合成、结构及荧光性能[J].无机化学学报,2009,25(5):924-928.GAO Qian,XIE Yabo,ZHANG Chaoyan,et al.Chin J Inorg Chem(in Chinese),2009,25(5):924-928.
[25]郭征楠,刘峥,魏席,等.以1,2,4,5-苯四甲酸或1,2,3,4-丁烷四羧酸为配体的金属有机框架的合成、表征及性质[J].无机化学学报,2016,32(1):9-17.GUO Zhengnan,LIU Zheng,WEI Xi,et al.Chin J Inorg Chem(in Chinese),2016,32(1):9-17.
[26]陈颖,赵宇,李静,等.共模板法一步合成绣球状BiOCl/Br固溶体光催化剂[J].高等学校化学学报,2017,38(11):2045-2052.CHEN Ying,ZHAO Yu,LI Jing,et al.Chem J Chin Univ(in Chinese),2017,38(11):2045-2052.
[2]DAYI B,KYZY A D,ABDULOGLU Y,et al.Investigation of the ability of immobilized cells to different carriers in removal of selected dye and characterization of environmentally friendly laccase of Morchella esculenta[J].Dyes Pigments,2018,151:15-21.
[3]GHANEIAN M T,EHRAMPOUSH M H,EHSANZADEH E,et al.Upgrading secondary wastewater plant effluent by modified coagulation and flocculation,for water reuse in irrigation[J].J Water Reuse Desal,2017,7(3):298-306.
[4]MALEKI A,HAYATI B,NAGHIZADEH M,et al.Adsorption of hexavalent chromium by metal organic frameworks from aqueous solution[J].J Ind Eng Chem,2015,28:211-216.
[5]高续春,代宏哲,赵鹏,等.微波法合成的氮化碳光催化降解苯酚及其机理[J].硅酸盐学报,2017,45(10):1503-1509.GAO Lianchun,DAI Hongzhe,ZHAO Peng,et al.J Chin Ceram Soc,2017,45(10):1503-1509.
[6]KAMENEV I,VIIROJA A,KALLAS J.Aerobic bio-oxidation with ozonation for recalcitrant wastewater treatment[J].J Adv Oxid Technol,2016,11(2):338-347.
[7]TEH C Y,BUDIMAN P M,SHAK K P Y,et al.Recent advancement of coagulation-flocculation and its application in wastewater treatment[J].Ind Eng Chem Res,2016,55(16):4363-4389.
[8]ASGHAR A,RAMAN A A A,DAUD W M A W.Advanced oxidation processes for in-situ production of hydrogen peroxide/hydroxyl radical for textile wastewater treatment:a review[J].J Clean Prod,2015,87(2):826-838.
[9]Omorogie M O,Babalola J O,Unuabonah E I,et al.Efficient chromium abstraction from aqueous solution using a low-cost biosorbent:Nauclea diderrichii,seed biomass waste[J].J Saudi Chem Soc,2016,20(1):49-57.
[10]陶丽琴,赵义侠,康卫民,等.聚四氟乙烯超细纤维负载二氧化钛光催化性能[J].硅酸盐学报,2016,44(1):89-94.TAO Liqin,ZHAO Yixia,KANG Weimin,et al.J Chin Ceram Soc,2016,44(1):89-94.
[11]PRAKASH K,KUMAR P S,LATHA P,et al.Design and fabrication of a novel metal-free SiO2/g-C3N4 nanocomposite:A robust photocatalyst for the degradation of organic contaminants[J].J Inorg Organomet P,2018,28(1):268-278.
[12]李翠霞,吴强红,曾鹏飞,等.氧化石墨烯-镝掺杂二氧化钛复合光催化材料的制备及光催化性能[J].硅酸盐学报,2016,44(6):872-877.LI Cuixia,WU Qianghong,ZENG Pengfei,et al.J Chin Ceram Soc,2016,44(6):872-877.
[13]BHATTACHARYA S,BALA S,MONDAL R.Design of chiral Co(Ⅱ)-MOFs and their application in environmental remediation and waste water treatment[J].Rsc Adv,2016,6(30):25149-25158.
[14]NASALEVICH M,BECKER R,FERNANDEZ E V R,et al.Co@NH2-MIL-125(Ti):Cobaloxime-derived metal-organic framework-based composite for light-driven H2 production[J].Energy Environ Sci,2015,8(1):364-375.
[15]BHATTACHARYA S,BALA S,MONDAL R.Design of chiral Co(Ⅱ)-MOFs and their application in environmental remediation and waste water treatment[J].Rsc Adv,2016,6(30):25149-25158.
[16]JHUNG S H,KHAN N A,HASAN Z.Analogous porous metal-organic frameworks:synthesis,stability and application in adsorption[J].Crystengcomm,2012,14(21):7099-7109.
[17]GE Y,LI N Y,JI X Y,et al.Assembly of a series of zinc coordination polymers based on 1,4-bis[2-(4-pyridyl)ethenyl]-2,3,5,6-tetramethylbenzene and 1,3-benzenedicarboxylate derivatives[J].Crystengcomm,2014,16(29):6621-6629.
[18]DAI M,SU X R,WANG X,et al.Three zinc(Ⅱ)coordination polymers based on tetrakis(4-pyridyl)cyclobutane and naphthalenedicarboxylate linkers:Solvothermal syntheses,structures,and photocatalytic properties[J].Cryst Growth Des,2013,14(1):240-248.
[19]YIN W Y,HUANG Z L,TANG X Y,et al.Structural diversification and photocatalytic properties of zinc(Ⅱ)polymers modified by auxiliary N-containing ligands[J].New J Chem,2015,39(9):7130-7139.
[20]DU J Q,DONG J L,XIE F,et al.Syntheses,structures,and properties of three mixed-ligand complexes based on 3,6-bis(imidazole-1-yl)pyridazine[J].J Mol Struct,2019,1175:754-762.
[21]ZHU W,YANG X Y,LI Y H,et al.A novel porous molybdophosphate-based FeⅡ,Ⅲ-MOF showing selective dye degradation as a recyclable photocatalyst[J].Inorg Chem Commun,2014,49:159-162.
[22]QIN L,CHEN H Z,LEI J,et al.Photodegradation of some organic dyes over two metal-organic frameworks with especially high efficiency for safranine T[J].Cryst Growth Des,2017,17(3):1293-1298.
[23]LI H,HE Y,ZHAO W,et al.Designing different functional frameworks from 0D to 3D for exploring structural correlation with photocatalytic activity[J].Polyhedron,2017,133:412-418.
[24]高倩,谢亚勃,张超艳,等.5,6-二羧基苯并咪唑双核铕配合物的合成、结构及荧光性能[J].无机化学学报,2009,25(5):924-928.GAO Qian,XIE Yabo,ZHANG Chaoyan,et al.Chin J Inorg Chem(in Chinese),2009,25(5):924-928.
[25]郭征楠,刘峥,魏席,等.以1,2,4,5-苯四甲酸或1,2,3,4-丁烷四羧酸为配体的金属有机框架的合成、表征及性质[J].无机化学学报,2016,32(1):9-17.GUO Zhengnan,LIU Zheng,WEI Xi,et al.Chin J Inorg Chem(in Chinese),2016,32(1):9-17.
[26]陈颖,赵宇,李静,等.共模板法一步合成绣球状BiOCl/Br固溶体光催化剂[J].高等学校化学学报,2017,38(11):2045-2052.CHEN Ying,ZHAO Yu,LI Jing,et al.Chem J Chin Univ(in Chinese),2017,38(11):2045-2052.