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羧甲基纤维素/壳聚糖双层水凝胶包封的Rh-MOF用于增强和可重复使用地吸附去除亮绿染料的开发与表征:动力学、等温线、热力学评估以及通过Box-Behnken设计进行的优化过程

Development and characterization of Rh-MOF encapsulated on double layer hydrogel of carboxymethyl cellulose/chitosan for enhanced and reusable adsorptive removal of brilliant green dye: Kinetics, isotherms, thermodynamic evaluation and process of optimization via Box-Behnken Design.

作者信息

Alhalafi Mona H, Sallam Sahar, Al-Ahmed Zehbah A, Mogharbel Amal T, Jawhari Ahmed H, Sari Abdullah A A, Alatawi Ibrahim S S, El-Metwaly Nashwa M

机构信息

Department of Chemistry, College of Sciences, Majmaah University, Al Majmaah 11952, Saudi Arabia.

Department of Physical Sciences, Chemistry Division, College of Science, Jazan University, P.O. Box. 114, Jazan 45142, Saudi Arabia.

出版信息

Int J Biol Macromol. 2025 Sep;321(Pt 4):146611. doi: 10.1016/j.ijbiomac.2025.146611. Epub 2025 Aug 6.

Abstract

This research investigates the creation and optimization of a dual-layer hydrogel composite formed from carboxymethyl cellulose (CMC) and chitosan (CS), which incorporates a rhodium-based metal-organic framework (Rh-MOF). The composite is designed to facilitate the efficient elimination of the cationic dye Brilliant Green (BG) from solutions. The structural stability of the Rh-MOF/CMC-CS hydrogel beads was significantly improved over the use of epichlorohydrin cross-linking. This modification played a vital character in attractive the mechanical strength of the hydrogel, thereby facilitating its ability to efficiently withstand numerous sequences of adsorption and desorption. The composite underwent extensive characterization through a range of analytical methods, such as XRD, FT-IR, XPS, EDX, nitrogen adsorption-desorption isotherms, and FESEM. This comprehensive approach facilitated a detailed examination of the composite's physical and chemical properties, alongside its morphological characteristics. A sequence of methodical batch adsorption experimentations was directed to analyze the influence of several operational factors on performance. These factors include pH level, dosage of the adsorbent, period of contact, initial concentration of dye, and temperature. Kinetic analyses revealed that the adsorption processes were consistent with a pseudo-second-order model. Furthermore, the equilibrium data aligned most closely with the isotherm of Langmuir, suggesting that chemisorption takes place in a monolayer arrangement. Furthermore, the thermodynamic evaluation provided parameters (ΔH° = +77.67 kJ/mol and ΔS° = +268.5 J/mol.K) indicating that the adsorption mechanism is both endothermic as well as spontaneous in nature. The enhancement of the process was achieved by using a Box-Behnken design in combination with response surface methodology (RSM). This approach successfully determined the ideal parameters for adsorption, specifically under conditions of pH 8, a dosage of 0.02 g per 25 mL, resulting in an impressive maximum adsorption capacity of 529.2 mg/g. Evaluations of the hydrogel's reusability across six adsorption and desorption processes showed its high capacity for regeneration and stable structure. These results demonstrate that Rh-MOF/CMC-CS hydrogel beads have the potential to be a practical and effective treatment of wastewater solution.

摘要

本研究探讨了由羧甲基纤维素(CMC)和壳聚糖(CS)形成的双层水凝胶复合材料的制备及优化,该复合材料包含一种铑基金属有机框架(Rh-MOF)。该复合材料旨在促进从溶液中高效去除阳离子染料亮绿(BG)。与使用环氧氯丙烷交联相比,Rh-MOF/CMC-CS水凝胶珠的结构稳定性得到显著提高。这种改性在提高水凝胶的机械强度方面起着至关重要的作用,从而促进其有效承受多次吸附和解吸过程的能力。通过一系列分析方法,如XRD、FT-IR、XPS、EDX、氮吸附-脱附等温线和FESEM,对该复合材料进行了广泛的表征。这种综合方法有助于详细研究复合材料的物理和化学性质及其形态特征。进行了一系列系统的批量吸附实验,以分析几个操作因素对性能的影响。这些因素包括pH值、吸附剂用量、接触时间、染料初始浓度和温度。动力学分析表明,吸附过程符合准二级模型。此外,平衡数据与朗缪尔等温线最为吻合,表明化学吸附以单层排列发生。此外,热力学评估提供的参数(ΔH° = +77.67 kJ/mol和ΔS° = +268.5 J/mol·K)表明吸附机制在本质上既是吸热的也是自发的。通过结合Box-Behnken设计和响应面方法(RSM)实现了该过程的优化。这种方法成功确定了理想的吸附参数,具体为在pH 8、每25 mL用量0.02 g的条件下,最大吸附容量达到529.2 mg/g,令人印象深刻。对水凝胶在六个吸附和解吸过程中的可重复使用性评估表明其具有高再生能力和稳定的结构。这些结果表明,Rh-MOF/CMC-CS水凝胶珠有潜力成为处理废水溶液的实用有效方法。

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