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核心技术专利：CN118964589B侵权必究
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用于从水溶液中吸附去除双氯芬酸的氧化石墨烯-壳聚糖水凝胶：制备、表征、动力学和热力学建模

Graphene oxide-chitosan hydrogel for adsorptive removal of diclofenac from aqueous solution: preparation, characterization, kinetic and thermodynamic modelling.

作者信息

Mahmoodi Hossein, Fattahi Moslem, Motevassel Mohsen

机构信息

Chemical Engineering Department, Abadan Faculty of Petroleum Engineering, Petroleum University of Technology Abadan Iran

出版信息

RSC Adv. 2021 Nov 11;11(57):36289-36304. doi: 10.1039/d1ra06069d. eCollection 2021 Nov 4.

DOI:10.1039/d1ra06069d
PMID:35492754
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9043336/
Abstract

This work aimed at developing a natural compound-based hydrogel adsorbent to remove diclofenac as a model pharmaceutical from water. First, graphene oxide-chitosan (GO-CTS) and amine graphene oxide-chitosan (AGO-CTS) hydrogel adsorbents were synthesized a facile mechanical mixing method. The synthesized materials were characterized through Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), scanning and transmission electron microscopy (SEM and TEM), Raman spectroscopy, and thermogravimetric analysis (TGA) techniques. In the second stage, adsorption experiments were conducted to determine the best GO to CTS ratio and find the optimized adsorption parameters, including the initial drug concentration, adsorbent dosage, pH, and temperature. The results showed that the optimal GO to CTS mass ratio is 2 : 5 and thus the same ratio was selected as the AGO to CTS mass ratio to understand the effect of amine-functionalization on removal efficiency. The optimal adsorption parameters were determined to be pH of 5, of 100 ppm and dosage of 1.5 g L, where 90.42% and 97.06% removal was achieved for optimal GO-CTS and AGO-CTS hydrogel adsorbents, respectively. Langmuir and Freundlich isotherms models were employed to investigate the adsorption behavior of diclofenac onto the synthesized hydrogels. The results revealed that the adsorption tends to be of the monolayer type and homogeneous, as the results were in better accordance with the Langmuir model than the Freundlich model. The thermodynamics of adsorption demonstrated that the adsorption is exothermic, exhibiting higher removal efficiency at lower temperatures. Furthermore, Gibb's free energy change of adsorption (Δ) suggested that the adsorption is spontaneous, being more spontaneous for AGO-CTS than GO-CTS hydrogels. Finally, the regeneration ability of the hydrogel adsorbents was studied in five consecutive cycles. The adsorbent maintained its efficiency at a relatively high level for three cycles but a considerable decrease was observed between the third and the fourth cycle, indicating that the hydrogels were recoverable for three cycles.

摘要

这项工作旨在开发一种基于天然化合物的水凝胶吸附剂，以从水中去除作为模型药物的双氯芬酸。首先，通过简便的机械混合方法合成了氧化石墨烯-壳聚糖（GO-CTS）和胺基氧化石墨烯-壳聚糖（AGO-CTS）水凝胶吸附剂。通过傅里叶变换红外光谱（FTIR）、X射线衍射（XRD）、布鲁诺尔-埃米特-泰勒（BET）、扫描和透射电子显微镜（SEM和TEM）、拉曼光谱以及热重分析（TGA）技术对合成材料进行了表征。在第二阶段，进行了吸附实验，以确定GO与CTS的最佳比例，并找到优化的吸附参数，包括初始药物浓度、吸附剂用量、pH值和温度。结果表明，GO与CTS的最佳质量比为2∶5，因此选择相同比例作为AGO与CTS的质量比，以了解胺功能化对去除效率的影响。确定最佳吸附参数为pH值5、初始药物浓度100 ppm和用量1.5 g/L，其中最佳GO-CTS和AGO-CTS水凝胶吸附剂的去除率分别达到90.42%和97.06%。采用朗缪尔和弗伦德利希等温线模型研究双氯芬酸在合成水凝胶上的吸附行为。结果表明，吸附倾向于单层且均匀，因为结果与朗缪尔模型的符合程度优于弗伦德利希模型。吸附热力学表明吸附是放热的，在较低温度下表现出更高的去除效率。此外，吸附的吉布斯自由能变化（Δ）表明吸附是自发的，AGO-CTS水凝胶比GO-CTS水凝胶更自发。最后，研究了水凝胶吸附剂在五个连续循环中的再生能力。吸附剂在三个循环中保持相对较高的效率，但在第三个和第四个循环之间观察到显著下降，表明水凝胶可回收三个循环。

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[2]
Optimization, equilibrium, adsorption behavior and role of surface functional groups on graphene oxide-based nanocomposite towards diclofenac drug.

J Environ Sci (China). 2020-2-19

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Synthesis of Poly(methacrylic acid)/Montmorillonite Hydrogel Nanocomposite for Efficient Adsorption of Amoxicillin and Diclofenac from Aqueous Environment: Kinetic, Isotherm, Reusability, and Thermodynamic Investigations.

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Preparation of a carboxymethylcellulose-iron composite for uptake of atorvastatin in water.

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Self-assembled three-dimensional reduced graphene oxide-based hydrogel for highly efficient and facile removal of pharmaceutical compounds from aqueous solution.

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