基于选择性吸附实现有机染料分离的一种金属有机框架薄膜材料制备与表征
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摘要
采用层层喷涂法(layer-by-layer),在经过16-巯基十六烷基酸(—COOH基团)表面处理的镀金硅基体表面,定向生长了一种金属有机框架薄膜材料(HKUST-1 SURMOF),并利用XRD、SEM等分析手段表征其结构和形貌,同时利用动态UV-vis技术分析该薄膜材料选择性吸附亚甲基蓝(MB)和核固红(NFR)染料分子能力。实验结果表明:在MB和NFR的混合溶液中,HKUST-1 SURMOF薄膜可以对含有噻嗪结构的MB分子显示出较强的选择性吸附能力,而很难吸附不含噻嗪结构的NFR分子,基于上述现象可以利用这种新型薄膜材料实现有机染料的选择性分离。
A layer-by-layer method was employed for the synthesis of the HKUST-1 which deposition on functionalized organic surfaces(HKUST-1 SURMOF). The XRD and SEM techniques were used to investigated the morphologies and structures of the SURMOF, the UV-vis technique was used to investigated the capacity of selective adsorption of dye molecules of type methylene blue(MB) and nuclearfast red(NFR). It can be assumed that the different adsorption behavior of MB and NFR was caused by thedifferent chemical structure. It might be assumed that the pyridyl moiety of the MB dye strongly adsorbed with HKUST-1 structure, while NFR did not build such interaction. While most of the MB molecules were removed from the mixture, the NFR molecules remained in the solution.
A layer-by-layer method was employed for the synthesis of the HKUST-1 which deposition on functionalized organic surfaces(HKUST-1 SURMOF). The XRD and SEM techniques were used to investigated the morphologies and structures of the SURMOF, the UV-vis technique was used to investigated the capacity of selective adsorption of dye molecules of type methylene blue(MB) and nuclearfast red(NFR). It can be assumed that the different adsorption behavior of MB and NFR was caused by thedifferent chemical structure. It might be assumed that the pyridyl moiety of the MB dye strongly adsorbed with HKUST-1 structure, while NFR did not build such interaction. While most of the MB molecules were removed from the mixture, the NFR molecules remained in the solution.
引文
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[17]栾琼,薛春峰,祝红叶,等.以金属有机骨架材料HKUST-1/聚苯胺电极及其超级电容器性能研究[J].电化学, 2017, 23(1):13-20.LUAN Qiong, XUE Chunfeng, ZHU Hongye, et al. Performance ofmetallic organic matrix material HKUST-1/polyaniline electrode andits supercapacitor were studied[J]. Electrochenistry, 2017, 23(1):13-20.
[18]何燕萍,谭衍曦,张健.基于尺寸识别和离子交换实现有机染料分离的一例阴离子型MOF[J].化学学报, 2014, 72:1228-1232.HE Yanping, TAN Yanxi, ZHNAG Jian. A case of anionic MOF fororganic dye separation based on size recognition and ion exchange[J].ACTA Chemical SINICA, 2014, 72:1228-1232.
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[20] SHEKHAH O, WANG H, KOWARIK S, et al. Step-by-step route forthe synthesis of metal-organic frameworks[J]. Journal of the AmericanChemical Society, 2007(129):15118-15124.
[21] ZHOU W, LI C, HEINKE L. Liquid and gas-phase diffusion offerrocene in thin films of metal-organic frameworks[J]. Materials, 2015(8):3767-3775.-
[2]申洋洋,刘锐,徐灿灿,等.印染及染料行业废水生物处理系统中的AOX污染研究[J].环境科学, 2015, 36(9):3304-3310.SHEN Yangyang, LIU Rui, XU Cancan, et al. AOX pollution inwastewater treatment process of dye and dyestuff chemical industries[J]. Environmental Science, 2015, 36(9):3304-3310.
[3] LINDEMANN P, TSOTSALAS M, SHISHATSKIY S, et al. Preparationof freestanding conjugated microporous polymer nanomembranes forgas separation[J]. Chem. Mat., 2014, 7(26):7189-7194.
[4] AMABILINO D. Nucleation&crystallisation[J]. Chemical SocietyReviews, 2014, 43(7):29-212.
[5] YU A, PISARENKO L, SHUWALOV A. Reactive distillation design:analysis of the process statics[J]. Reviews in Chemical Engineering,2001(17):253-259.
[6]程凤莲,孟范平,周游,等.大型海藻浒苔对碱性染料亚甲基蓝的吸附性能[J].化工进展, 2011, 30(s1):896-900.CHENG Fenglian, MENG Fanping, ZHOU You, et al. Adsorptioncapacity of large enteromorpha on alkaline dye methylene blue[J].Chemical Industry and Engineering Progress, 2011, 30(s1):896-900.
[7]俞洁,张海涛,陆泉芳,等.坡缕石/聚乙二醇/丙烯酸水凝胶的表征及其对阳离子染料的吸附性能[J].化工进展, 2015, 34(4):1115-1121.YU Jie, ZHANG Haitao, LU Quanfang, et al. Characterization ofpalygorskite acrylic acid hydrogel and itsapplication as an adsorbent for cationic dyes[J]. Chemical Industryand Engineering Progress, 2015, 34(4):1115-1121.
[8]史艳茹,李奇,王丽,等.三维网络水凝胶在重金属和染料吸附方面的研究进展[J].化工进展, 2011, 30(10):2294-2303.SHI Yanru, LI Qi, WANG Li, et al. Progress in hydrogels with three-dimensional cross-linked polymeric networks for the adsorption ofheavy metal ions and dyes[J]. Chemical Industry and EngineeringProgress, 2011, 30(10):2294-2303.
[9]宋晓东,程昌敬,余海溶.阴离子聚电解质修饰磁性氧化石墨烯对碱性品红的吸附性能[J].化工进展, 2016, 35(9):2973-2981.SONG Xiaodong, CHENG Changjing, YU Hairong. Adsorptionperformance of an anionic polyelectrolyte-functionlized magneticgraphene oxide for basic fuchsin[J]. Chemical Industry andEngineering Progress, 2016, 35(9):2973-2981.
[10]刘有毅,黄艳,何嘉杰,等. CO/N2/CO2在MOF-74(Ni)上吸附相平衡和选择性[J].化工学报, 2015, 66(11):4469-4475.LIU Youyi, HUANG Yan, HE Jiajie, et al. The adsorption phaseequilibrium and selectivity of CO/N2/CO2in the MOF-74(Ni)[J].CIESC Journal, 2015, 66(11):4469-4475.
[11] LI H L. Design and synthesis of an exceptionally stable and highlydesign and synthesis of an exceptionally stable and highly porousmetal-organic framework[J]. Nature, 1999(402):276-283.
[12] MAKIURA R, MOTOYAMA S, UMEMURA Y, et al. Surface nano-architecture of a metal-organic framework[J]. Nature Materials, 2010(9):565-573.
[13] EDDAOUDI M, KIM J, ROSI N, et al. Systematic design of pore sizeand functionality in isoreticular MOFs and their application inmethane storage[J]. Chem. Soc. Rev., 2012(41):1088-1095.
[14] LONG G, YAGHI O. 2009 Metal-organic frameworks issue[J]. Chem.Soc. Rev., 2009(38):1450-1459.
[15] EDDAOUDI M, KIM J, ROSI N, et al. Systematic design of pore sizeand functionality in isoreticular MOFs and their application inmethane storage[J]. Science, 2002(18):295-303..
[16]董寒,张晓东,李红欣,等.金属有机骨架材料HKUST-1的制备及其应用进展[J].材料导报, 2016(23):117-122,142.DONG Han, ZHANG Xiaodong, LI Hongxin, et al. Progress in/poly(ethylene glycol)/preparation of metal organic frameworks HKUST-1 and its application[J]. Material Guide A:Summary, 2016(23):117-122,142.
[17]栾琼,薛春峰,祝红叶,等.以金属有机骨架材料HKUST-1/聚苯胺电极及其超级电容器性能研究[J].电化学, 2017, 23(1):13-20.LUAN Qiong, XUE Chunfeng, ZHU Hongye, et al. Performance ofmetallic organic matrix material HKUST-1/polyaniline electrode andits supercapacitor were studied[J]. Electrochenistry, 2017, 23(1):13-20.
[18]何燕萍,谭衍曦,张健.基于尺寸识别和离子交换实现有机染料分离的一例阴离子型MOF[J].化学学报, 2014, 72:1228-1232.HE Yanping, TAN Yanxi, ZHNAG Jian. A case of anionic MOF fororganic dye separation based on size recognition and ion exchange[J].ACTA Chemical SINICA, 2014, 72:1228-1232.
[19] ARSLAN H, SHEKHAH O, WIELAND D, et al. Intercalation inlayered metal-organic frameworks:reversible inclusion of an extendedπ-system[J]. Journal of the American Chemical Society, 2011, 133(21):8158-8161.
[20] SHEKHAH O, WANG H, KOWARIK S, et al. Step-by-step route forthe synthesis of metal-organic frameworks[J]. Journal of the AmericanChemical Society, 2007(129):15118-15124.
[21] ZHOU W, LI C, HEINKE L. Liquid and gas-phase diffusion offerrocene in thin films of metal-organic frameworks[J]. Materials, 2015(8):3767-3775.-