Tzereme Areti, Christodoulou Evi, Kyzas George Z, Kostoglou Margaritis, Bikiaris Dimitrios N, Lambropoulou Dimitra A
Laboratory of Environmental Pollution Control, Department of Chemistry, Aristotle University of Thessaloniki, GR⁻541 24 Thessaloniki, Greece.
Laboratory of Polymer Chemistry and Technology, Department of Chemistry, Aristotle University of Thessaloniki, GR-541 24 Thessaloniki, Greece.
Polymers (Basel). 2019 Mar 14;11(3):497. doi: 10.3390/polym11030497.
The main purpose of this study was to investigate the synthesis of some cross-linked carboxyl-grafted chitosan derivatives to be used as selective adsorbents for diclofenac (DCF) pharmaceutical compounds from aqueous mixtures. Four different materials were synthesized using succinic anhydride (CsSUC), maleic anhydride (CsMAL), itaconic acid (CsITA), and -aconitic acid (CsTACON) as grafting agents. After synthesis, scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), and X-ray diffraction (XRD) were performed before and after DCF adsorption. In addition, a complete adsorption evaluation was carried out for all materials studying some important parameters. The optimum pH was 4; the amino groups of DCF can be protonated at pH = 4 (⁻NH⁺), so this groups can easily attract the clear negatively carboxyl moieties (⁻COO) of the chitosan adsorbents. The for CsTACON was higher than those of the other materials, at all temperatures studied. By altering the temperature from 25 to 35 °C, an increase (16%) of (from 84.56 to 98.34 mg g) was noted, while similar behavior was revealed after a further increase of temperature from 35 to 45 °C, improving by 5% (from 98.34 to 102.75 mg g). All isotherms were fitted to Langmuir, Freundlich, and Langmuir-Freundlich (L-F) models). In addition, a kinetic model was proposed taking into account not only the interactions but also the diffusivity of the molecule (DCF) into the polymeric network. The behavior of the prepared chitosan materials in simultaneously removing other compounds (synergetic or antagonistic) was also evaluated by experiments performed in mixtures. DCF presented the highest removal from the mixture in the order: CsTACON (92.8%) > CsITA (89.5%) > CsSUC (80.9%) > CsMAL (66.2%) compared to other pharmaceutical compounds (salicylic acid, ibuprofen and ketoprofen). Desorption was achieved by using different eluants (either water or organic). The highest desorption ability was found for acetone (100% for CsTACON, CsSUC, CsMAL and 77% for CsITA) for all materials.
本研究的主要目的是研究一些交联羧基接枝壳聚糖衍生物的合成,以用作从水性混合物中选择性吸附双氯芬酸(DCF)药物化合物的吸附剂。使用琥珀酸酐(CsSUC)、马来酸酐(CsMAL)、衣康酸(CsITA)和乌头酸(CsTACON)作为接枝剂合成了四种不同的材料。合成后,在DCF吸附前后进行了扫描电子显微镜(SEM)、傅里叶变换红外光谱(FTIR)和X射线衍射(XRD)分析。此外,对所有材料进行了完整的吸附评估,研究了一些重要参数。最佳pH值为4;DCF的氨基在pH = 4时可质子化(⁻NH⁺),因此该基团可轻松吸引壳聚糖吸附剂中明显带负电的羧基部分(⁻COO)。在所有研究温度下,CsTACON的吸附量均高于其他材料。将温度从25℃改变至35℃时,吸附量增加了16%(从84.56 mg/g增至98.34 mg/g),而温度进一步从35℃升至45℃后,吸附量出现类似变化,提高了5%(从98.34 mg/g增至102.75 mg/g)。所有等温线均拟合到朗缪尔、弗伦德利希和朗缪尔 - 弗伦德利希(L - F)模型。此外,提出了一个动力学模型,该模型不仅考虑了分子(DCF)与聚合物网络之间的相互作用,还考虑了分子扩散。通过在混合物中进行实验,还评估了制备的壳聚糖材料同时去除其他化合物(协同或拮抗)的行为。与其他药物化合物(水杨酸、布洛芬和酮洛芬)相比,DCF在混合物中的去除率最高,顺序为:CsTACON(92.8%)> CsITA(89.5%)> CsSUC(80.9%)> CsMAL(66.2%)。通过使用不同的洗脱剂(水或有机溶剂)实现了解吸。对于所有材料,发现丙酮的解吸能力最高(CsTACON、CsSUC、CsMAL为100%,CsITA为77%)。