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2023, 01, v.35 67-75
双配体Zn-MOF/g-C_3N4复合材料的制备及光催化性能
基金项目(Foundation): 国家级大学生创新创业训练计划项目“g-C3N4/Zn-MOF复合材料的合成与光催化性能研究”(202010757023); 塔里木大学校长基金其他项目“g-C3N4/M-TiO2纳米复合材料的制备”(TDZKYB202003)
邮箱(Email): xjjjh78@163.com;
DOI:
发布时间: 2023-03-15
出版时间: 2023-03-15
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摘要:

为了进一步拓展MOF-5在光催化降解污染物方面的应用,本研究以MOF-5为原料,采用水解再生法使MOF-5水解并再生为一种新型、水稳定性好的双配体Zn-MOF(D-MOF),同时将其与g-C_3N4耦合,制备出性能优异的光催化材料D-MOF/g-C_3N4(DMG)。通过X-射线粉末衍射、扫描电镜、紫外-可见漫反射、N2吸附-脱附等手段对复合材料DMG进行表征;采用光催化降解亚甲基蓝(MB)来研究复合材料的光催化活性,同时优化复合材料的最佳配比。结果表明:复合材料DMG有优异的光催化性能,经300 W氙灯照射60 min后对MB的降解率可达到92.79%,其降解速率分别是纯D-MOF和g-C_3N4的1.62倍和6.49倍,同时对复合材料DMG进行光催化机理试验并提出其光催化降解MB的可能机理。本研究为水稳定性较差的金属-有机框架材料的优化提供了一种新的思路。

Abstract:

To further expand its application in photocatalytic degradation of pollutants, MOF-5 was hydrolyzed and regenerated into a new dual ligand Zn-MOF(D-MOF) with good water stability. After being coupled with g-C_3N4, a photocatalyst material D-MOF/g-C_3N4(DMG) with excellent performance was prepared. The composite materials of DMG was characterized through X-ray powder diffraction, scanning electron microscopy, UV-visible diffuse reflectance, N2adsorption-desorption, etc. The photocatalytic activity of DMG was investigated by photocatalytic degradation of methylene blue(MB). At the same time, the optimal ratio of DMG was optimized. The results showed that DMG had excellent photocatalytic performance. The degradation rate of MB could reach 92.79% after irradiation with a 300 W xenon lamp for 60 min, and its degradation rate was 1.62 and 6.49 times higher than that of pure D-MOF and g-C_3N4, respectively. The photocatalytic mechanism test of DMG was carried out and the possible photocatalytic degradation mechanism of MB was proposed. This study provides a new idea for the optimization of metal-organic framework materials with poor water stability.

参考文献

[1]卫栋慧,侯笛,魏徵文,等.复合光催化材料的制备及对染料废水的处理研究[J].应用化工,2020,49(9):2164-2167.

[2] LENG L J,YUAN X,HUANG H J,et al.Bio-char derived from sewage sludge by liquefaction:characterization and application for dye adsorption[J]. Applied surface science,2015,346(15):223-231.

[3] HASAN Z,CHO D W,ISLAM J G,et al.Catalytic decoloration of commercial azo dyes by copper-carbon composites derived from metal organic frameworks[J].Journal of alloys&compounds,2016,689:625-631.

[4] ZHANG X,HUO Y,SHAKEEL M,et al.Fabrication of BiOCl/ZnO/CN nanocomposite for visible-light photocatalytic degradation of dyes[J]. Chemistryselect,2020,5(5):1640-1647.

[5]刘鼐,冯庆革,陈考,等.Sn-TiO2气凝胶的制备及光催化性能研究[J].应用化工,2021,50(8):2062-2067,2075.

[6] AHMED S I,FURUSAWA T,SATO M,et al.Sonochemical synthesis,photocatalytic activity and optical properties of silica coated ZnO nanoparticles[J]. Ultrasonics sonochemistry,2012,19(4):750-755.

[7] FENG J,CHEN T T,LIU S N,et al.Improvement of gC3N4photocatalytic properties using the hummers method[J].Journal of colloid&interface science,2016,479:1-6.

[8]李玉玲,张嘉辉,郑丽萍,等.MOFs材料应用于光催化降解水中残留药物分子研究进展[J].应用化工,2020,49(5):1313-1315.

[9] ZHENG Y Y,GU B S,SUN S Q,et al.Preparation and visible light photocatalytic properties of modified graphene photocatalytic thin film[J]. Journal of materials science and engineering,2019,116(15):8579-8586.

[10] WANG C C,YI X H,WANG P.Powerful combination of MOFs and C3N4for enhanced photocatalytic performance[J]. Applied catalysis B:environmental,2019,247:24-48.

[11] ROY S,BHNUIA A,SCHUTH N,et al.Light-driven hydrogen evolution catalyzed by a cobaloxime catalyst incorporated in a MIL-101(Cr)metal-organic framework[J].Sustainable energy&fuels,2018,2(6):1148-1152.

[12]冯婷,王芳,姜建辉.MOFs衍生过渡金属氧化物材料的制备及其氧析出性能研究[J].塔里木大学学报,2021,33(1):56-65.

[13] ZHANG Y K,WANG G R,WANG M,et al. CdS p-n heterojunction co-boosting with Co3O4and Ni-MOF-74for photocatalytic hydrogen evolution[J].Dalton transactions an international journal of inorganic chemistry,2018,32(4):11176-11189.

[14] PAN Y,SUN K A,LIU S J,et al.Core-shell ZIF-8@ZIF-67 derived CoP nanoparticles-embedded N-doped carbon nanotube hollow polyhedron for efficient over-all water splitting[J]. Journal of the American chemical society,2018,140(7):2610-2618.

[15] ARAYA T,JIA M K,YANG J,et al. Resin modified MIL-53(Fe)MOF for improvement of photocatalytic performance[J].Applied catalysis B:environmental,2017,203:768-777.

[16] ZHAO Z X,MA X L,KASIK A,et al. Gas separation properties of metal organic framework(MOF-5)membranes[J]. Industrial&engineering chemistry research,2013,52(3):1102-1108.

[17] DENG L X,HE J J,LI B R,et al. Study of a new 3D MOF and its adsorption,slow release and biological activity in water-soluble and oil-soluble pesticides[J/OL].Polyhedron,2020,190(5):114752[2021-07-14]. https://doi.org/10.1016/j.poly.2020.114752.

[18] GONG Y,ZHAO X,ZHANG H,et al.MOF-derived nitrogen doped carbon modified g-C3N4heterostructure composite with enhanced photocatalytic activity for bisphenol A degradation with peroxymonosulfate under visible light irradiation[J].Applied catalysis B:environmental,2018,233:35-45.

[19] CHEN Q Y,LI S J,XU H Y,et al.Co-MOF as an electron donor for promoting visible-light photoactivities of g-C3N4nanosheets for CO2reduction[J].Chinese journal of catalysis,2020,41(3):514-523.

[20] GREATHOUSE J A,ALLENDORF M D. The interaction of water with MOF-5 simulated by molecular dynamics[J]. Journal of the american chemical society,2006,128(33):10678-10679.

[21] JEONG Y C,SEO J W,KIM J H,et al.Function-regeneration of non-porous hydrolyzed-MOF-derived materials[J].Nano research,2019,12(8):1921-1930.

[22] CUI L F,ZOU X H,LIU Y N,et al.Dramatic enhancement of photocatalytic H2evolution over hydrolyzed MOF-5 coupled Zn0.2Cd0.8S heterojunction[J].Journal of colloid and interface science,2020,577(5):233-241.

[23]孟佳意,文剑平,陈亦力,等.g-C3N4-Bi2WO6/沸石复合光催化材料的制备及氨氮降解研究[J].水处理技术,2021,47(8):43-47,53.

[24] RODRíGUEZ N A,PARRA R,GRELA M A,et al.Structural characterization,optical properties and photocatalytic activity of MOF-5 and its hydrolysis products:implications on their excitation mechanism[J]. RSC advances,2015,5(89):73112-73118.

[25] TRANCHEMONTAGNE D J,HUNT J R,YAGHI O M.Room temperature synthesis of metal-organic frameworks:MOF-5,MOF-74,MOF-177,MOF-199 and IRMOF-0[J].Tetrahedron,2008,64(36):8553-8557.

[26]王茀学.g-C3N4@Zn-MOF复合材料的制备及其光催化性能研究[D].北京:北京建筑大学,2018.

[27]吕攀.基于MOFs及其衍生物构建g-C3N4基复合光催化剂及光催化产氢性能研究[D].无锡:江南大学,2021.

[28]陈颖,翟勃银,梁宇宁,等.混合配体Cd-MOF的合成及其光催化降解性能[J].硅酸盐学报,2019,47(4):433-439.

[29] WANG H,YUAN X,WU Y,et al.Synthesis and applications of novel graphitic carbon nitride/metal-organic frameworks mesoporous photocatalyst for dyes removal[J].Applied catalysis B:environmental,2015,174:445-454.

[30]陈颖,翟勃银,梁宇宁,等.g-C3N4/Ti-MOF复合材料的合成及其光催化性能[J].石油学报(石油加工),2020,36(1):160-168.

[31] DONG X L,DING W,ZHANG X F.Mechanism and kinetics model of degradation of synthetic dyes by UV-vis/H2O2/Ferrioxalate complexes[J]. Dyes and pigments,2007,74(2):470-476.

[32] DONG F,ZHAO Z W,XIONG T,et al.In situ construction of g-C3N4/g-C3N4metal-free heterojunction for enhanced visible-light photocatalysis[J].ACS applied materials&interfaces,2013,5(21):11392-11401.

[33] JING H P,WANG C C,ZHANG Y W,et al.Photocatalytic degradation of methylene blue in ZIF-8[J].RSC advances,2014,4(9):54454-54462.

[34] DING M L,JIANG H L. Improving water stability of MOFs by a general surface hydrophobic polymerization[J].CCS chemistry,2020,3(8):1-23.

[35] TAYLOR J M,VAIDHYANATHAN R,IREMONGER S S,et al. Enhancing water stability of metal-organic frameworks via phosphonate monoester linkers[J]. Journal of the american chemical society,2012,134(35):14338-14340.

基本信息:

中图分类号:O643.36;O644.1;X703

引用信息:

[1]白怡航,齐少振,邹正丹,等.双配体Zn-MOF/g-C_3N_4复合材料的制备及光催化性能[J].塔里木大学学报,2023,35(01):67-75.

基金信息:

国家级大学生创新创业训练计划项目“g-C3N4/Zn-MOF复合材料的合成与光催化性能研究”(202010757023); 塔里木大学校长基金其他项目“g-C3N4/M-TiO2纳米复合材料的制备”(TDZKYB202003)

发布时间:

2023-03-15

出版时间:

2023-03-15

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