缺陷Zr基金属有机框架材料的制备、表征及其对四环素的吸附性能研究

黄继明; 刘润清; 吴思展; 秦航道; 陈 静

doi:10.13205/j.hjgc.202403004

缺陷Zr基金属有机框架材料的制备、表征及其对四环素的吸附性能研究

doi: 10.13205/j.hjgc.202403004

铜仁学院材料与化学工程学院, 贵州铜仁 554300

基金项目:

铜仁学院博士启动基金(trxyDH2202,trxyDH1506)

详细信息

作者简介:
黄继明(1986-),男,博士,副教授,主要研究方向为环境修复材料与技术。jim_huang@foxmail.com

通讯作者:
黄继明(1986-),男,博士,副教授,主要研究方向为环境修复材料与技术。jim_huang@foxmail.com

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出版历程
- 收稿日期: 2022-11-07
- 网络出版日期: 2024-05-31

PREPARATION AND CHARACTERIZATION OF DEFECTIVE Zr-BASED METAL-ORGANIC FRAMEWORKS AND THEIR ADSORPTION PROPERTIES FOR TETRACYCLINE

School of Material and Chemical Engineering, Tongren Unversity, Tongren 554300, China

摘要

摘要: 吸附具有成本低、能耗小、操作方便和环境友好等优点,在污水净化领域具有广泛应用潜力。通过简单的溶剂热法制备了缺陷Zr基金属有机框架(UiO-66-NH₂)吸附剂,并将其用于去除废水中四环素。利用X射线衍射仪(XRD)、场发射扫描电子显微镜(FESEM)、傅立叶变换红外光谱(FT-IR)、氮气吸附-脱附和X射线光电子能谱等手段对吸附剂进行表征。为获得吸附剂去除废水中四环素最佳条件,以四环素的吸附量为响应值,在单因素实验基础上,采用Box-Behnken设计(BBD)响应曲面法(RSM)考察吸附剂投加量、溶液pH值、四环素初始浓度以及吸附时间等因素相互作用和影响。结果表明,经实验修正后的最佳吸附条件:吸附剂投加量为10 mg,pH=3.80,四环素初始浓度为27 mg/L,吸附时间为3 h;此条件下,吸附剂对四环素的吸附量可达71.85 mg/g。此外,再生实验表明,经过5次循环吸附后,吸附剂仍具有较强的吸附能力(68.33 mg/g),是一种相对稳定的吸附材料。
- 金属有机框架 /
- 缺陷 /
- 吸附 /
- 响应面法 /
- 四环素
Abstract: Adsorption has the potential to be broadly applied in the field of sewage purification due to advantages such as low costs, less energy consumption, ease of operation and environmental friendliness. In this work, Zr-based metal-organic frameworks (UiO-66-NH₂) with defects were successfully prepared by a facile solvothermal method, which was used to removal tetracycline from wastewater. Defective UiO-66-NH₂ was characterized by X-ray diffraction (XRD), field emission electron microscope (FESEM), Fourier transform infrared (FT-IR), nitrogen adsorption-desorption and X-ray photoelectron spectroscopy. In order to achieve optimum conditions of tetracycline from aqueous solutions,based on single-factor tests, response surface methodology (RSM) and Box-Behnken design (BBD) were employed to examine the interaction of factors and optimize the adsorption operation parameters, including adsorbent dose, the initial concentration of tetracyclines, pH and contact time. The optimum conditions of maximum adsorption (71.85 mg/g) were found as follows: 10 mg of adsorbent dosage, initial tetracycline concentration of 27 mg/L, pH=3.8 and adsorption time of 3 h. In addition, regeneration experiments showed that the adsorption efficiency of tetracycline after five adsorption-desorption cycles with good uptake efficiency (68.33 mg/g) and UiO-66-NH₂ exhibited quite a good cyclic stability.
- metal-organic frameworks /
- defects /
- adsorption /
- response surface methodology /
- tetracycline

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参考文献(20)

[1]	王丹, 隋倩, 赵文涛, 等. 中国地表水环境中药物和个人护理品的研究进展[J]. 科学通报, 2014, 59(9):743-751.
[2]	WANG Z, KOIRALA B, HERNANDEZ Y, et al. A naturally inspired antibiotic to target multidrug-resistant pathogens[J]. Nature, 2022, 601(7894):606-611.
[3]	ROJAS S, HORCAJADA P. Metal-organic frameworks for the removal of emerging organic contaminants in water[J]. Chem Rev, 2020, 120(16):8378-8415.
[4]	KANDIAH M, NILSEN MH, USSEGLIO S, et al. Synthesis and stability of tagged UiO-66 Zr-MOFs[J]. Chem Mater, 2010, 22(24):6632-6640.
[5]	QIN M, SHI Y, LU D, et al. High-performance Hf/Ti-doped defective Zr-MOFs for cefoperazone adsorption:behavior and mechanisms[J]. Appl Surf Sci, 2022, 595:153494.
[6]	李莉, 张赛, 何强, 等. 响应面法在试验设计与优化中的应用[J]. 实验室研究与探索, 2015, 34(8):41-45.
[7]	WITEK-KROWIAK A, CHOJNACKA K, PODSTAWCZYK D, et al. Application of response surface methodology and artificial neural network methods in modelling and optimization of biosorption process[J]. Bioresour Technol, 2014, 160:150-160.
[8]	CLARK C A, HECK K N, POWELL C D, et al. Highly defective UiO-66 materials for the adsorptive removal of perfluorooctanesulfonate[J]. ACS Sustainable Chem Eng, 2019, 7(7):6619-6628.
[9]	SHEN L, LIANG S, WU W, et al. Multifunctional NH₂-mediated zirconium metal-organic framework as an efficient visible-light-driven photocatalyst for selective oxidation of alcohols and reduction of aqueous Cr(Ⅵ)[J]. Dalton Trans, 2013, 42(37):13649-13657.
[10]	HE X, DENG F, SHEN T, et al. Exceptional adsorption of arsenic by zirconium metal-organic frameworks:engineering exploration and mechanism insight[J]. J Colloid Interface Sci, 2019, 539:223-234.
[11]	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]. Chem Eng J, 2018, 331:124-131.
[12]	HUANG J, XUE P, WANG S, et al. Fabrication of zirconium-based metal-organic frameworks@tungsten trioxide (UiO-66-NH₂@WO₃) heterostructure on carbon cloth for efficient photocatalytic removal of tetracycline antibiotic under visible light[J]. J Colloid Interface Sci, 2022, 606:1509-1523.
[13]	LIANG Q, CUI S, LIU C, et al. Construction of CdS@UiO-66-NH₂ core-shell nanorods for enhanced photocatalytic activity with excellent photostability[J]. J Colloid Interface Sci, 2018, 524:379-387.
[14]	LU X, SHAO Y, GAO N, et al. Adsorption and removal of clofibric acid and diclofenac from water with MIEX resin[J]. Chemosphere, 2016, 161:400-411.
[15]	LIANG X, CHI J, YANG Z. The influence of the functional group on activated carbon for acetone adsorption property by molecular simulation study[J]. Microporous Mesoporous Mater, 2018, 262:77-88.
[16]	刘希, 张宇峰, 罗平. 改性花生壳对四环素类抗生素的吸附特性研究[J]. 环境污染与防治, 2013, 35(5):35-39 ,44.
[17]	KIM H G, CHOI K, LEE K, et al. Controlling the structural robustness of zirconium-based metal organic frameworks for efficient adsorption on tetracycline antibiotics[J]. Water, 2021, 13(13):1869.
[18]	KANG J K, KIM Y G, LEE S C, et al. Artificial neural network and response surface methodology modeling for diclofenac removal by quaternized mesoporous silica SBA-15 in aqueous solutions[J]. Microporous Mesoporous Mater, 2021, 328:111497.
[19]	DALVAND A, NABIZADEH R, REZA GANJALI M, et al. Modeling of reactive Blue 19 azo dye removal from colored textile wastewater using L-arginine-functionalized Fe₃O₄ nanoparticles:optimization, reusability, kinetic and equilibrium studies[J]. J Magn Magn Mater, 2016, 404:179-189.
[20]	YANG Y, LI X, GU Y, et al. Adsorption property of fluoride in water by metal organic framework:optimization of the process by response surface methodology technique[J]. Surf Interfaces, 2022, 28:101649.