金属有机骨架杂化泡沫对TC和Cu<sup>2+</sup>的吸附

李微; 胡淏婷; 刘宁; 叶友林; 高明杰; 冯青

doi:10.13205/j.hjgc.202406004

金属有机骨架杂化泡沫对TC和Cu²⁺的吸附

doi: 10.13205/j.hjgc.202406004

李微^1, ,,
胡淏婷¹,
刘宁²,
叶友林¹,
高明杰³,
冯青⁴

1. 沈阳建筑大学市政与环境工程学院, 沈阳 110168;
2. 碧桂园房地产开发有限公司, 沈阳 110013;
3. 辽宁省城乡建设规划设计院有限责任公司, 沈阳 110006;
4. 中国中建设计研究院有限公司, 北京 100037

基金项目:

辽宁省教育厅科学研究项目(lnqn202010)

沈阳市科技计划项目(22322310)

辽宁省科技厅自然科学基金(2019ZD0671)

详细信息

作者简介:
李微(1982-),女,教授,主要研究方向为低碳可持续污水处理技术、污水处理材料研发与应用。liweilengjinyue@163.com

通讯作者:
李微(1982-),女,教授,主要研究方向为低碳可持续污水处理技术、污水处理材料研发与应用。liweilengjinyue@163.com

计量
- 文章访问数: 137
- HTML全文浏览量: 16
- PDF下载量: 10
- 被引次数: 0
出版历程
- 收稿日期: 2023-01-19
- 网络出版日期: 2024-07-11

ADSORPTION PERFORMANCE OF TC AND Cu²⁺ BY METAL-ORGANIC SKELETON HYBRID FOAMS

1. College of Municipal and Environmental Engineering, Shenyang Jianzhu University, Shenyang 110168, China;
2. Country Garden Real Estate Development Co., Ltd., Shenyang 110013, China;
3. Liaoning Urban and Rural Construction Planning and Design Institute Co., Ltd., Shenyang 110006, China;
4. China Construction Engineering Design & Research Institute Co., Ltd., Beijing 100037, China

摘要

摘要: 针对医药废水中抗生素和重金属难以被有效去除的问题,采用金属有机骨架杂化泡沫MIL-100(Fe)/CMC吸附四环素(tetracycline, TC)和铜离子(Cu²⁺),利用X射线衍射、扫描电镜、氮气吸附脱附和热重分析技术,分析MOFs杂化泡沫理化性能,通过吸附试验研究杂化泡沫吸附性能影响因素、稳定性和吸附机理。结果表明:MIL-100(Fe)/CMC具有丰富的孔道结构和较高的热稳定性,在初始浓度为30 mg/L,MIL-100(Fe)/CMC投加量为40 mg,吸附时间为16 h,pH=6时,MIL-100(Fe)/CMC对TC和Cu²⁺的最大吸附容量分别为80.40,80.04 mg/g,且离子强度(NaCl)与吸附性能呈负相关。MIL-100(Fe)/CMC具有良好的吸附和循环再生性能,6次循环再生后对TC和Cu²⁺去除率均保持在70%以上;MIL-100(Fe)/CMC对TC与Cu²⁺的吸附为自发放热过程,符合Langmuir等温线模型和拟一级动力学模型。金属有机骨架杂化泡沫对于抗生素和重金属混合污染物去除效果表明其在处理医药废水方面具有广阔的应用前景。
- 金属有机骨架杂化泡沫 /
- 吸附 /
- 四环素 /
- Cu²⁺ /
- 循环再生
Abstract: The removal of antibiotics and heavy metals in the medicine wastewater is a tricky problem, and the metal-organic skeleton hybrid foam MIL-100(Fe)/CMC was used to remove tetracycline (TC) and copper ions (Cu²⁺). The physicochemical properties of the MOFs hybrid foams were analyzed by X-ray diffraction, scanning electron microscopy, nitrogen adsorption and desorption, as well as thermogravimetric analysis techniques; the influencing factors, stability, and adsorption mechanisms of hybrid foams were analyzed by adsorption experiments. The results showed that MIL-100(Fe)/CMC had porous structure and high thermal stability; MIL-100(Fe)/CMC had-maximum adsorption capacity of 80.40 and 80.04 mg/g for tetracycline (TC) and Cu²⁺, respectively, in the optimal working condition of 30 mg/L contaminants, 40 mg dosage of MIL-100(Fe)/CMC, 16 hours adsorption time, pH of 6 the ionic strength (NaCl) was negatively correlated with adsorption performance. MIL-100(Fe)/CMC had excellent adsorption and cyclic regeneration performance, and the removal rates of TC and Cu²⁺ maintained above 70% after six cycles of regeneration. The adsorption of TC and Cu²⁺ by MIL-100(Fe)/CMC was a self-exothermic process, matching the Langmuir isotherm model and the proposed first-order kinetic model. In conclusion, the metal organic skeleton hybrid foam is proven to have a broad research prospect in the removal of mixed contaminants of antibiotics and heavy metals in the treatment of pharmaceutical wastewater.
- metal-organic skeletal hybrid foam /
- adsorbent /
- tetracycline /
- Cu²⁺ /
- cyclic regeneration

HTML全文

参考文献(41)

[1]	LIANG Y T, PEI M, WANG D D, et al. Improvement of soil ecosystem multifunctionality by dissipating manure-induced antibiotics and resistance genes[J]. Environmental Science & Technology, 2017,51(9):4988-4998.
[2]	ELTAWEIL A, MAMDOUH I M, MONAEM E E, et al. Highly efficient removal for methylene blue and Cu²⁺ onto UiO-66 metal organic framework/carboxylated graphene oxide-incorporated sodium alginate beads[J]. ACS Omega, 2021,36(6):23528-23541.
[3]	AHMED M B, ZHOU J L, NGO H H, et al. Adsorptive removal of antibiotics from water and wastewater: progress and challenges[J]. Science of the Total Environment, 2015, 532(1):112-126.
[4]	ZHU Q L, XU Q. Metal-organic framework composites[J]. Chemical Society Reviews,2014,43(16):5468-5512.
[5]	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.
[6]	崔颖,孙国峰,任苏瑜,等.锆基MOF材料用于水中抗生素的吸附研究[J].环境科学与技术, 2019,42(3):103-108.
[7]	MIRSOLEIMANI S M, SETOODEH P, ZEINALI S, et al. Tetracycline antibiotic removal from aqueous solutions by MOF-5: adsorption isotherm, kinetic and thermodynamic studies[J]. Journal of Environmental Chemical Engineering,2018,6(5):6118-6130.
[8]	YANG J H, HAN L, YANG W Y, et al. In situ synthetic hierarchical porous MIL-53(Cr) as an efficient adsorbent for mesopores-controlled adsorption of tetracycline[J]. Microporous and Mesoporous Materials,2021,332:111667.
[9]	MAHDI B, MANOUCHEHR V, MOJTABA B, et al. MIL-100(Fe) a potent adsorbent of dacarbazine: experimental and molecular docking simulation[J]. Chemical Engineering Journal,2023,452(2):138987.
[10]	TAN T L, ABDUL S H, MOHAMMAD L M A, et al. One-pot solvothermal synthesis of Zr-based MOFs with enhanced adsorption capacity for Cu²⁺ ions removal[J]. Journal of Solid State Chemistry,2022,315(9):123429.
[11]	FORGHANI M, AZIZI A, LIVANI M J, et al. Adsorption of lead(Ⅱ) and chromium(Ⅵ) from aqueous environment onto metal-organic framework MIL-100(Fe): synthesis, kinetics, equilibrium and thermodynamics[J]. Journal of Solid State Chemistry,2020,291:121636.
[12]	BAKHTIARI N, AZIZIAN S. Adsorption of copper ion from aqueous solution by nanoporous MOF-5: a kinetic and equilibrium study[J]. Journal of Molecular Liquids,2015,206(1):114-118.
[13]	LESLEY J, MOUTOSHI S, KIM S, et al. Removal of Cu²⁺, Cd²⁺, and Pb²⁺ from aqueous solution by fabricated MIL-100(Fe) and MIL-101(Cr): experimental and molecular modeling study[J]. Journal of Environmental Chemical Engineering,2021,9(6):106663.
[14]	荆钰,郭金涛,王重庆,等.金属有机骨架材料MIL-100(Fe)的一氧化碳吸附性能[J].天然气化工(C1化学与化工),2011,36(5):33-36.
[15]	吴成晨,肖瑜,吴川,等.Zn-MOF-74对Cd(Ⅱ)的吸附性能及机理研究[J].工业水处理,2020,40(2):63-67.
[16]	CHEN Y F, HUANG X Q, ZHANG S H, et al. Shaping of metal-organic frameworks: from fluid to shaped bodies and robust foams[J]. Journal of the American Chemical Society,2016,138(34):10810-10813.
[17]	LEI C, GAO J K, REN W J, et al. Fabrication of metal-organic frameworks@cellulose aerogels composite materials for removal of heavy metal ions in water[J]. Carbohydrate Polymers,2018,205:35-41.
[18]	YANG W X, HAN Y, LI C H, et al. Shapeable three-dimensional CMC aerogels decorated with Ni/Co-MOF for rapid and highly efficient tetracycline hydrochloride removal[J]. Chemical Engineering Journal,2019,375:122076.
[19]	ZHANG C F, QIU L G, KE F. A novel magnetic recyclable photocatalyst based on a core-shell metal-organic framework Fe₃O₄@MIL-100(Fe) for the decolorization of methylene blue dye[J]. Journal of Materials Chemistry, A. Materials for Energy and Sustainability,2013,1(45):14329-14334.
[20]	YU S S, WAN J Q, CHEN K Z. A facile synthesis of superparamagnetic Fe₃O₄ supraparticles@MIL-100(Fe) core-shell nanostructures: preparation, characterization and biocompatibility[J]. Journal of Colloid and Interface Science,2016,461:173-178.
[21]	JIANG L H, LIU Y G, ZENG G M, et al. Removal of 17β-estradiol by few-layered graphene oxide nanosheets from aqueous solutions: external influence and adsorption mechanism[J]. Chemical Engineering Journal,2016,284:93-102.
[22]	TONG M M, LIU D H, YANG Q Y. Influence of framework metal ions on the dye capture behavior of MIL-100 (Fe, Cr) MOF type solids[J]. Journal of Materials Chemistry, A. Materials for Energy and Sustainability,2013,1(30):8534-8537.
[23]	KOHSARI I, SHARIATINIA Z, POURMORTAZAVI S M. Antibacterial electrospun chitosan-polyethylene oxide nanocomposite mats containing bioactive silver nanoparticles[J]. Carbohydrate Polymers,2016,140:287-298.
[24]	张琪欣,姚初清,徐天寒,等.新型MIL-100(Fe)基MOFs材料的制备及其对Sr²⁺的吸附[J].中国环境科学,2021,41(1):141-150.
[25]	XUAN W M, ZHU C F, LIU Y, et al. Mesoporous metal-organic framework materials[J]. Chemical Society Reviews, 2012, 41(5):1677-1695.
[26]	LONG D N, COLEMAN P J. NF/RO filtration of the hydrophobic ionogenic compound triclosan: transport mechanisms and the influence of membrane fouling[J]. Separation and Purification Technology,2008,62(3):709-716.
[27]	DARIUSH T S, MEHRNAZ A, JANET S. Efficient and eco-friendly cellulose-supported MIL-100(Fe) for wastewater treatment[J]. RSC Advances,2022,12(15):9023-9035.
[28]	XIE D H, MA Y, GU Y, et al. Bifunctional NH₂-MIL-88(Fe) metal-organic framework nanooctahedra for highly sensitive detection and efficient removal of arsenate in aqueous media[J]. Journal of Materials Chemistry A,2017,5(45):23794-23804.
[29]	MA Y, ZHOU Q, ZHOU S C, et al. A bifunctional adsorbent with high surface area and cation exchange property for synergistic removal of tetracycline and Cu²⁺[J]. Chemical Engineering Journal,2014,258:26-33.
[30]	KANG J, LIU H J, ZHENG Y M, et al. Systematic study of synergistic and antagonistic effects on adsorption of tetracycline and copper onto a chitosan[J]. Journal of Colloid and Interface Science,2009,344(1):117-125.
[31]	WANG D B, JIA F Y, WANG H, et al. Simultaneously efficient adsorption and photocatalytic degradation of tetracycline by Fe-based MOFs[J]. Journal of Colloid and Interface Science,2018,519:273-284.
[32]	ZHAO T P, TAN Y Y, GUO Y, et al. Interactions of tetracycline with Cd (Ⅱ), Cu (Ⅱ) and Pb (Ⅱ) and their cosorption behavior in soils[J]. Environmental Pollution,2013,180:206-213.
[33]	WANG Y, WANG X J, LI J, et al. Coadsorption of tetracycline and copper(Ⅱ) onto struvite loaded zeolite:an environmentally friendly product recovered from swine biogas slurry[J]. Chemical Engineering Journal,2019,371:366-377.
[34]	LI Z Q, YANG J C, SUI K W, et al. Facile synthesis of metal-organic framework MOF-808 for arsenic removal[J]. Materials Letters,2015,160:412-414.
[35]	GUO Z Q, YANG F J, YANG R R, et al. Preparation of novel ZnO-NP@Zn-MOF-74 composites for simultaneous removal of copper and tetracycline from aqueous solution[J]. Separation and Purification Technology,2021,274:118949.
[36]	CHATURVEDI G, KAUR A, UMAR A, Et al. Removal of fluoroquinolone drug, levofloxacin, from aqueous phase over iron based MOFs, MIL-100(Fe)[J]. Journal of Solid State Chemistry,2020,281(C):121029.
[37]	孙刘鑫,王培茗,杨俊浩,等.离子强度对吸附有机污染物影响的研究进展[J].化工进展,2021,40(6):3239-3257.
[38]	阳春,陈晓虹,王瀚,等.双金属掺杂UiO-66及其对四环素的吸附特性[J].中国给水排水,2023,39(21):78-85.
[39]	XIA S, SUN J M, SUN W T. Bimetallic metal-organic gel for effective removal of chlortetracycline hydrochloride from aqueous solution: adsorption isotherm, kinetic and mechanism studies[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects,2022,649:129403.
[40]	RAO M M, RAMANA D K, SESHAIAH K, et al. Removal of some metal ions by activated carbon prepared from phaseolus aureus hulls[J]. Journal of Hazardous Materials, 2009, 166(2/3):1006-1013.
[41]	DING K, WANG W, YU D, et al. Facile formation of flexible Ag/AgCl/polydopamine/cotton fabric composite photocatalysts as an efficient visible-light photocatalysts[J]. Applied Surface Science,2018,454:101-111.