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使用羧甲基纤维素-g-聚丙烯酰胺/蒙脱土纳米复合水凝胶去除孔雀石绿。

Removal of malachite green using carboxymethyl cellulose-g-polyacrylamide/montmorillonite nanocomposite hydrogel.

机构信息

Faculty of Chemical & Petroleum Engineering, University of Tabriz, Tabriz, Iran.

Faculty of Chemical & Petroleum Engineering, University of Tabriz, Tabriz, Iran.

出版信息

Int J Biol Macromol. 2020 Sep 15;159:1122-1131. doi: 10.1016/j.ijbiomac.2020.05.093. Epub 2020 May 16.

Abstract

In this study, carboxymethyl cellulose based graft poly(acrylamide) hydrogel (CMC-g-P(AAm)) and its nanocomposite with montmorillonite (CMC-g-P(AAm)/MMT) were produced by the free radical method and it was used to malachite green (MG) dye removal from aqueous solution. The properties and characterization of the adsorbents were investigated using FTIR, SEM, TGA, and XRD analyzes, and the results showed that MMT nanoparticles were successfully distributed in the hydrogel system. MMT nanoparticles were loaded into the hydrogel system with different weight percentages and the maximum adsorption efficiency of MG dye was determined at 10 wt% MMT. Also, the effect of temperature, contact time, initial concentration of MG dye and initial pH on the adsorption efficiency of MG dye was studied in a batch. Equilibrium behavior investigation of the adsorption process showed that the equilibrium data determined are in good agreement with the Langmuir isotherm model and the monolayer surfaces play an effective role in the adsorption process. The maximum monolayer adsorption capacity (q) determined using the Langmuir isotherm model for CMC-g-P(AAm) and CMC-g-P(AAm)/MMT were determined to be 158.1 mg/g and 172.4 mg/g, respectively. Also, the kinetic study showed that the pseudo-second- order kinetic model is more capable of describing the kinetic behavior of the process than other models. Also, the α parameter values for the MG dye adsorption process using CMC-g-P(AAm) and CMC-g-P(AAm)/MMT were determined to be 0.6337 mg/g·min and 31.04 mg/g·min, respectively. This indicates that the produced composite has a high adsorption value. Gibbs free energy (ΔG°) was negative for the adsorption processes in the range of 25-50 °C, indicating that the process was spontaneous. In addition, the enthalpy parameter (ΔH°) was determined for the adsorption process using CMC-g-P(AAm) and CMC-g-P(AAm)/MMT nanocomposite hydrogels at 39.859 KJ/mol and 74.736 KJ/mol, respectively. Positive ΔH° indicates that the process is endothermic in the range of 25-50 °C using both adsorbents. Also, the concentrations effect of Na+ and K+ ions on adsorption efficiency was investigated and it was concluded that the efficiency of the adsorption process decreased with the increase of ions concentration. Adsorption efficiency decrease can be due to the occupation of active sites and repulsive electrostatic interactions at the adsorbent surface with the MG dye molecule.

摘要

在这项研究中,通过自由基法制备了羧甲基纤维素接枝聚丙烯酰胺水凝胶(CMC-g-P(AAm))及其与蒙脱土的纳米复合材料(CMC-g-P(AAm)/MMT),并将其用于从水溶液中去除孔雀石绿(MG)染料。通过 FTIR、SEM、TGA 和 XRD 分析研究了吸附剂的性质和表征,结果表明蒙脱土纳米颗粒成功地分布在水凝胶体系中。将蒙脱土纳米颗粒以不同的重量百分比负载到水凝胶体系中,并确定 MG 染料的最大吸附效率为 10wt%MMT。此外,还研究了温度、接触时间、MG 染料初始浓度和初始 pH 值对 MG 染料吸附效率的影响。在批量吸附过程中,对吸附过程的平衡行为进行了研究,结果表明,确定的平衡数据与 Langmuir 等温线模型吻合较好,单层表面在吸附过程中起着重要作用。通过 Langmuir 等温线模型确定的 CMC-g-P(AAm)和 CMC-g-P(AAm)/MMT 的最大单层吸附容量(q)分别为 158.1mg/g 和 172.4mg/g。此外,动力学研究表明,准二级动力学模型比其他模型更能描述该过程的动力学行为。此外,使用 CMC-g-P(AAm)和 CMC-g-P(AAm)/MMT 确定 MG 染料吸附过程的α参数值分别为 0.6337mg/g·min 和 31.04mg/g·min。这表明所制备的复合材料具有较高的吸附值。对于 25-50°C 范围内的吸附过程,吉布斯自由能(ΔG°)为负值,表明该过程是自发的。此外,还分别确定了 CMC-g-P(AAm)和 CMC-g-P(AAm)/MMT 纳米复合水凝胶吸附过程的焓参数(ΔH°)为 39.859KJ/mol 和 74.736KJ/mol。正的ΔH°表明,使用两种吸附剂,在 25-50°C 范围内,该过程是吸热的。还研究了 Na+和 K+离子浓度对吸附效率的影响,结果表明,随着离子浓度的增加,吸附过程的效率降低。吸附效率的降低可能是由于活性位点的占据和在吸附剂表面与 MG 染料分子之间的静电排斥相互作用。

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