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功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理

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崔巍, 张卫, 刘淋, 温东东, 沈根祥, 胡双庆. 功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理[J]. 环境化学, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
引用本文: 崔巍, 张卫, 刘淋, 温东东, 沈根祥, 胡双庆. 功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理[J]. 环境化学, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
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CUI Wei, ZHANG Wei, LIU Lin, WEN Dongdong, SHEN Genxiang, HU Shuangqing. Adsorption behavior and mechanism of functional mental organic frameworks for sulfachloropyridazine in water[J]. Environmental Chemistry, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
Citation: CUI Wei, ZHANG Wei, LIU Lin, WEN Dongdong, SHEN Genxiang, HU Shuangqing. Adsorption behavior and mechanism of functional mental organic frameworks for sulfachloropyridazine in water[J]. Environmental Chemistry, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
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功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理

  • 1. 华东理工大学资源与环境工程学院, 上海, 200237;

  • 2. 同济大学环境科学与工程学院, 上海, 200092;

  • 3. 上海市环境科学研究院, 上海, 200233

    • 通讯作者: 张卫, E-mail: wzhang@ecust.edu.cn ; 
  • 基金项目:

    国家"十三五"水体污染控制与治理科技重大专项（2017ZX07207002）和国家自然科学基金（41877124，21737005）资助.

Adsorption behavior and mechanism of functional mental organic frameworks for sulfachloropyridazine in water

  • 1. School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai, 200237, China;

  • 2. School of Environmental Science and Engineering, Tongji University, Shanghai, 200092, China;

  • 3. Shanghai Academy of Environmental Sciences, Shanghai, 200233, China

    • Corresponding author: ZHANG Wei, wzhang@ecust.edu.cn ; 
  • Fund Project: Supported by National Water Pollution Control and Treatment Science and Technology Major Project (2017ZX07207002) and the National Natural Science Foundation of China (41877124, 21737005).

  • 摘要: 近年来，抗生素的大量使用对生态环境和人类健康构成了严重威胁.抗生素去除技术开发引起了人们的广泛关注.本研究制备了4种具有良好水热稳定性的锆基金属骨架有机材料（UiO-66，UiO-66-NH2，UiO-66-Cl和UiO-66-NO2），通过比较4种材料对水中痕量磺胺氯哒嗪（SCP）的吸附性能，从中筛选出最佳吸附剂，进而探究了温度、pH、共存阴离子、腐殖酸和可再生性等因素对其吸附性能的影响，探讨了作用机制.研究结果表明，功能基团的引入提升了金属骨架有机材料对SCP的吸附性能，其中氨基的引入效果最为显著（去除率从11.62%提升至71.12%），这主要是由于氢键的作用；UiO-66-NH2对SCP的吸附符合拟二级动力学，温度的升高抑制了吸附的进行，pH=6时吸附效果最好；Cl-和SO42-对UiO-66-NH2吸附性能起到了抑制作用，而腐殖酸影响较小；CO32-的水解导致路易斯酸碱反应，从而极大地干扰了SCP的吸附过程；UiO-66-NH2经过四次循环使用后，SCP去除率下降不到10%.本研究为采用功能化金属有机骨架材料去除水中污染物提供了新思路.
    Abstract: In recent years, extensive use of antibiotics has greatly threatened the ecological environment and human health, so the removal of antibiotics has been widely investigated. In this study, four zirconium-based metal organic framework (MOF) materials (UiO-66, UiO-66-NH2, UiO-66-Cl and UiO-66-NO2) with good hydrothermal stability were synthesized to compare their adsorption performance in removing sulfachloropyridazine (SCP) from water. The effects of temperature, pH, coexisting anion, and humic acid on the adsorption performance of the optimal material were explored. The results show that the introduction of functional groups into MOF enhanced the adsorption ability of UiO-66 for SCP, and the effect of amino group was the most significant (SCP removal rate increased from 11.62% to 71.12%), which might be due to hydrogen bonding. The adsorption of SCP by UiO-66-NH2 accorded with the pseudo-second order kinetics model, and the adsorption process was inhibited at high temperatures. Co-existing anions including Cl-, SO42- and CO32- reduced the adsorption ability, and the presence of CO32- inhibited the adsorption process the most because of the Lewis acid-base reaction. Humic acid had no influences on the adsorption performance of UiO-66-NH2, and the removal efficiency of UiO-66-NH2 decreased by less than 10% after four cycles of use. This study provides a new idea for using functionalized metal-organic framework materials to remove contaminants in water body.
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  • [1] 殷哲云,闵露娟,金立涛,等. HPLC-MS/MS测定3类污水处理厂污泥及污水中的8种药物[J]. 环境化学,2018,37(8):1720-1727.

    YIN Z Y, MIN L J, JIN L T, et al. HPLC-MS/MS was used to determine 8 drugs in sludge and sewage of 3 kinds of sewage treatment plants[J]. Environmental Chemistry, 2018, 37(8):1720-1727(in Chinese).

    [2] ZHANG Q, YING G, PAN C, et al. Comprehensive evaluation of antibiotics emission and fate in the river basins of China:Source analysis, multimedia modeling, and linkage to bacterial resistance[J]. Environmental Science & Technology, 2015, 49:6772-6782.
    [3] 洪蕾洁,石璐,张亚雷,等. 固相萃取-高效液相色谱法同时测定水体中的10种磺胺类抗生素[J]. 环境科学,2012,33(2):652-657.

    HONG L J, SHI L, ZHANG Y L, et al. Simultaneous determination of 10 sulfa antibiotics in water by solid phase extraction and high performance liquid chromatography[J]. Environmental Chemistry, 2012, 33(2):652-657(in Chinese).

    [4] DERYLO-MARCZEWSKA A, BLACHNIO M, MARCZEWSKI A W, et al. Phenoxyacid pesticide adsorption on activated carbon-Equilibrium and kinetics[J]. Chemosphere, 2019, 214:349-360.
    [5] BRIONES R M, ZHUANG W Q, SARMAH A K. Biodegradation of metformin and guanylurea by aerobic cultures enriched from sludge[J]. Environmental Pollution, 2018, 243:255-262.
    [6] KHAN M F, YU L L, ACHARI G, et al. Degradation of sulfolane in aqueous media by integrating activated sludge and advanced oxidation process[J]. Chemosphere, 2019, 222:1-8.
    [7] LU J, SUN J, CHEN X, et al. Efficient mineralization of aqueous antibiotics by simultaneous catalytic ozonation and photocatalysis using MgMnO3 as a bifunctional catalyst[J]. Chemical Engineering Journal, 2019, 358:48-57.
    [8] SHARMA V, KUMAR R V, PAKSHIRAJAN K, et al. Integrated adsorption-membrane filtration process for antibiotic removal from aqueous solution[J]. Powder Technology, 2017, 321:259-269.
    [9] LIANG C, ZHANG X, FENG P, et al. ZIF-67 derived hollow cobalt sulfide as superior adsorbent for effective adsorption removal of ciprofloxacin antibiotics[J]. Chemical Engineering Journal, 2018, 344:95-104.
    [10] 王娅南,彭洁,黄合田,等. 贵阳市城市河流典型抗生素的分布特征[J]. 环境化学,2018,37(9):2039-2048.

    WANG Y N, PENG J, HUANG H T, et al. Distribution characteristics of typical antibiotics in urban rivers of Guiyang City[J]. Environmental Chemistry, 2018, 37(9):2039-2048(in Chinese).

    [11] PENG J, WU E, WANG N, et al. Removal of sulfonamide antibiotics from water by adsorption and persulfate oxidation process[J]. Journal of Molecular Liquids, 2019, 274:632-638.
    [12] CHEN X, JIANG X, YIN C, et al. Facile fabrication of hierarchical porous ZIF-8 for enhanced adsorption of antibiotics[J]. Journal of Hazardous Materials, 2019, 367:194-204.
    [13] LUO Y, CHEN J, WU C, et al. Effect of particle size on adsorption of norfloxacin and tetracycline onto suspended particulate matter in lake[J]. Environmental Pollution, 2019, 244:549-559.
    [14] DHAKA S, KUMAR R, DEEP A, et al. Metal-organic frameworks (MOFs) for the removal of emerging contaminants from aquatic environments[J]. Coordination Chemistry Reviews, 2019, 380:330-352.
    [15] ZHANG X F, WANG Z, FENG Y, et al. Adsorptive desulfurization from the model fuels by functionalized UiO-66(Zr)[J]. Fuel, 2018, 234:256-262.
    [16] JHUNG S H, LEE J H, YOON J W, et al. Microwave synthesis of chromium terephthalate MIL-101 and its benzene sorption ability[J]. Advanced Materials, 2007, 19:121-124.
    [17] HAQUE E, LEE J E, JANG I T, et al. Adsorptive removal of methyl orange from aqueous solution with metal-organic frameworks, porous chromium-benzenedicarboxylates[J]. Journal of Hazardous Materials, 2010, 181:535-542.
    [18] HAQUE E, JUN A W, JHUNG S H. Adsorptive removal of methyl orange and methylene blue from aqueous solution with a metal-organic framework material, iron terephthalate (MOF-235)[J]. Journal of Hazardous Materials, 2011, 185:507-511.
    [19] GUO T M, QIU M, QI X H. Selective conversion of biomass-derived levulinic acid to ethyl levulinate catalyzed by metal organic framework (MOF)-supported polyoxometalates[J]. Applied Catalysis A:General, 2019, 572:168-175.
    [20] WANG R, XU H J, ZHANG K, et al. High-quality Al@Fe-MOF prepared using Fe-MOF as a micro-reactor to improve adsorption performance for selenite[J]. Journal of Hazardous Materials, 2019, 364:272-280.
    [21] SARKER M, SONG J Y, JHUNG S H. Carboxylic-acid-functionalized UiO-66-NH2:A promising adsorbent for both aqueous- and non-aqueous-phase adsorptions[J]. Chemical Engineering Journal, 2018, 331:124-131.
    [22] HASAN Z, TONG M, JUNG B K, et al. Adsorption of pyridine overamino-functionalized metal-organic frameworks:Attraction viahydrgen-bonding versus base-base repulsion[J]. Journal of Physical Chemistry C, 2014, 118:21049-21056.
    [23] ZHAO P W, LIU X H, TIAN W L, et al. Adsolubilization of 2,4,6-Trichlorophenol from aqueous solution by surfactant intercalated ZnAl layered double hydroxides[J]. Chemical Engineering Journal, 2015, 279:597-604.
    [24] ZLOTEA C, PHANON D, MATJAZ M, et al. Effect of NH2 and CF3 functionalization on the hydrogen sorption properties of MOFs[J]. Dalton Transactions, 2011, 40(18):4879-4881.
    [25] ZHU H L, HUANG J P, ZHOU Q Y, et al. Enhanced luminescence of NH2-UiO-66 for selectively sensing fluoride anion in water medium[J]. Journal of Mnescence, 2019, 208:67-74.
    [26] 刘宇航,周珠贤,江黎明,等. 氨基修饰的锆基金属有机框架材料对香料的吸附和缓控释[J]. 中国科学:化学, 2018, 49(4):41-46.

    LIU Y H, ZHOU Z X, JIANG L M, et al. Adsorption and slow controlled release of amine-modified zirconium base materials on spices were studied[J]. Chian Science:Chemical, 2018, 49(4):41-46(in Chinese).

    [27] LIN K Y, LIU Y T, CHEN S Y. Adsorption of fluoride to UiO-66-NH2 in water:Stability, kinetic, isotherm and thermodynamic studies. Journal of Colloid and Interface Science, 2016, 461:79-87.
    [28] AKSU Z, TUNC O. Application of biosorption for penicillin G removal:comparison with activated carbon[J]. Process Biochemistry, 2005, 40:831-847.
    [29] 常春,王胜利,郭景阳, 等. 不同热解条件下合成生物炭对铜离子的吸附动力学研究[J]. 环境科学学报,2016,36(7):2491-2502.

    CHANG C, WANG S L, GUO J Y, et al. Adsorption kinetics of Cu+ on biochar under different pyrolysis conditions[J]. Journal of Environmental Sciences, 2016, 36(7):2491-2502(in Chinese).

    [30] TAMBAT SNEHA N, SANE PRIYANKA K, SURESH S, et al. Hydrothermal synthesis of NH2-UiO-66 and its application for adsorptive removal of dye[J]. Advanced Powder Technology, 2018, 29:2626-2632.
    [31] ADAMS C, WANG Y, LOFTIN K, et al. Removal of antibiotics from surface and distilled water in conventional water treatment processes[J]. Journal of Environmental Engineering, 2002, 128(3):253-260.
    [32] LIU L, LIN S, ZHANG W, et al. Kinetic and mechanistic investigations of the degradation of sulfachloropyridazine in heat-activated persulfate oxidation process[J]. Chemical Engineering Journal, 2018, 346:515-524.
    [33] LIN S, WANG G X, ZHONG Y N, 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.
    [34] AZHAR M R, ABID H R, PERIASAMY V, et al. Adsorptive removal of antibiotic sulfonamide by UiO-66 and ZIF-67 for wastewater treatment[J]. Journal of Colloid and Interface Science, 2017, 500:88-95.
    [35] AZHAR M R, ABID H R, SUN H Q, et al. Excellent performance of copper based metal organic framework in adsorptive removal of toxic sulfonamide antibiotics from wastewater[J]. Journal of Colloid and Interface Science, 2016, 478:344-352.
    [36] 马福臻,周少奇,刘泽珺, 等. 三维网状HZO@SGH对水中氟离子的吸附作用和机制[J]. 环境科学,2018,39(2):828-837.

    MA F Z, ZHOU S Q, LIU Z J, et al. Adsorption and mechanism of 3d mesh HZO@SGH on fluorine ions in water[J]. Environmental Science, 2018, 39(2):828-837(in Chinese).

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  • 收稿日期:  2019-01-27
  • 刊出日期:  2020-01-01

功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理

    通讯作者: 张卫, E-mail: wzhang@ecust.edu.cn ; 
  • 1. 华东理工大学资源与环境工程学院, 上海, 200237;
  • 2. 同济大学环境科学与工程学院, 上海, 200092;
  • 3. 上海市环境科学研究院, 上海, 200233
  • 收稿日期:  2019-01-27
  • 网络出版日期:  2020-01-01
基金项目:

国家"十三五"水体污染控制与治理科技重大专项（2017ZX07207002）和国家自然科学基金（41877124，21737005）资助.

摘要: 近年来，抗生素的大量使用对生态环境和人类健康构成了严重威胁.抗生素去除技术开发引起了人们的广泛关注.本研究制备了4种具有良好水热稳定性的锆基金属骨架有机材料（UiO-66，UiO-66-NH2，UiO-66-Cl和UiO-66-NO2），通过比较4种材料对水中痕量磺胺氯哒嗪（SCP）的吸附性能，从中筛选出最佳吸附剂，进而探究了温度、pH、共存阴离子、腐殖酸和可再生性等因素对其吸附性能的影响，探讨了作用机制.研究结果表明，功能基团的引入提升了金属骨架有机材料对SCP的吸附性能，其中氨基的引入效果最为显著（去除率从11.62%提升至71.12%），这主要是由于氢键的作用；UiO-66-NH2对SCP的吸附符合拟二级动力学，温度的升高抑制了吸附的进行，pH=6时吸附效果最好；Cl-和SO42-对UiO-66-NH2吸附性能起到了抑制作用，而腐殖酸影响较小；CO32-的水解导致路易斯酸碱反应，从而极大地干扰了SCP的吸附过程；UiO-66-NH2经过四次循环使用后，SCP去除率下降不到10%.本研究为采用功能化金属有机骨架材料去除水中污染物提供了新思路.

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