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过程工程学报 ›› 2023, Vol. 23 ›› Issue (4): 590-601.DOI: 10.12034/j.issn.1009-606X.222124

• 研究论文 • 上一篇    下一篇

CCS-DETA凝胶球的制备及其对甲基橙的吸附性能

殷慧卿1,2， 武少杰1,2， 李明阳1,2， 龙红明1,2， 王松月3， 邱志新3， 高翔鹏1,2,3*
  

  1. 1. 安徽工业大学冶金工程学院，安徽 马鞍山 243002 2. 安徽工业大学冶金减排与资源综合利用教育部重点实验室，安徽 马鞍山 243002 3. 江苏苏讯新材料科技股份有限公司，江苏 宿迁 223699
  • 收稿日期:2022-04-11 修回日期:2022-06-08 出版日期:2023-04-28 发布日期:2023-05-04
  • 通讯作者: 高翔鹏 gxp1992@ahut.edu.cn
  • 作者简介:殷慧卿，硕士研究生，材料科学与工程专业，E-mail: 1823644806@qq.com；通讯联系人，高翔鹏，副教授，研究方向为天然聚合物对贵重金属吸附及水处理，E-mail: gxp1992@ahut.edu.cn
  • 基金资助:
    国家自然科学基金资助项目;中国博士后科学基金面上资助项目

Preparation and adsorption properties of CCS-DETA hydrogel beads for methyl orange

Huiqing YIN1,2,  Shaojie WU1,2,  Mingyang LI1,2,  Hongming LONG1,2,  Songyue WANG3, Zhixin QIU3,  Xiangpeng GAO1,2,3*   

  1. 1. School of Metallurgical Engineering, Anhui University of Technology, Ma'anshan, Anhui 243002, China 2. Key Laboratory of Metallurgical Emission Reduction & Resources Recycling, Ministry of Education, Anhui University of Technology, Ma'anshan, Anhui 243002, China 3. Jiangsu Suxun New Material Co., Ltd., Suqian, Jiangsu 223699, China
  • Received:2022-04-11 Revised:2022-06-08 Online:2023-04-28 Published:2023-05-04

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摘要： 壳聚糖是天然多糖甲壳素经脱乙酰作用获得的聚合物，具有生物降解性、生物相容性、无毒等多种生理功能。壳聚糖广泛应用于食品添加剂、纺织、农业、环保、美容保健、化妆品等行业。其分子中的羟基和氨基可以形成活性界面，吸附染料分子，但由于机械强度和化学稳定性较弱，直接应用受到限制，需要进行化学改性。本工作以壳聚糖(CS)为基体，戊二醛(GA)为交联剂，二乙烯三胺(DETA)为改性剂，采用溶胶-凝胶法制备壳聚糖(CCS-DETA)水凝胶珠，研究了CCS-DETA水凝胶珠对废水中甲基橙(MO)的吸附性能，讨论了pH值、初始浓度、吸附等温线和动力学等因素的影响，并采用傅立叶红外光谱(FTIR)、场发射扫描电镜(FESEM)和X射线光电子能谱(XPS)对CCS-DETA水凝胶微球的微观结构和吸附机理进行了表征分析。结果表明，CCS-DETA在低pH条件下发生质子化，吸附过程中与带负电荷的MO分子发生静电作用。在较高pH值下，MO上的O和N原子可与CCS-DETA上的羟基形成氢键。吸附结果表明，CCS-DETA水凝胶珠对MO有良好的吸附效果。当CCS-DETA水凝胶珠的剂量为30 mg、MO的初始浓度为20 mg/L、pH值为2、反应时间为12 h时，MO去除率可达91.33%，且CCS-DETA水凝胶珠表现出良好的稳定性。吸附动力学和热力学表明，吸附过程符合准一级动力学模型和Langmuir等温吸附模型。在温度为313.15 K时，MO的最大吸附量可达到209.68 mg/g。本研究表明，CCS-DETA可以通过氨基和羟基有效地吸附水中的MO，为染料废水的处理提供了一种潜在的方法。

关键词: 壳聚糖, 凝胶, 甲基橙, 吸附, 化学改性

Abstract: Chitosan is a polymer obtained by deacetylation of the natural polysaccharide chitin. It has various physiological functions such as biodegradability, biocompatibility, and non-toxicity. The hydroxyl and amino groups in their molecules can form active interfaces to adsorb dye molecules. However, direct application is limited due to its weak mechanical strength and chemical stability, thus requiring chemical modification. In this work, chitosan hydrogel beads (CCS-DETA) were prepared by sol-gel method using chitosan (CS) as matrix, glutaraldehyde (GA) as crosslinking agent, and diethylenetriamine (DETA) as modifier. The adsorption performance of CCS-DETA hydrogel beads on methyl orange (MO) dye in wastewater was studied. Effects of pH value, initial concentration, adsorption isotherm, and kinetics were discussed with mathematical model fitting results. The microstructure and adsorption mechanism of CCS-DETA hydrogel beads were characterized by Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscope (FESEM), and X-ray photoelectron spectroscopy (XPS). The results showed that CCS-DETA was protonated under low pH values that electrostatically interacted with negatively charged MO molecules in the adsorption process. It was showed that CCS-DETA was protonated at low pH and electrostatically interacted with negatively charged MO molecules during the adsorption process. Furthermore, at higher pH, O and N ions on MO can form hydrogen bonds with hydroxyl groups on CCS-DETA. The adsorption results showed that CCS-DETA hydrogel beads had excellent adsorption effect on MO. When the dosage of CCS-DETA hydrogel beads was 30 mg, the initial concentration of MO was 20 mg/L, pH was 2, and the reaction time was 12 h, the MO removal rate could reach 91.33%, and CCS-DETA hydrogel beads had exhibited good stability. The adsorption kinetics and thermodynamics showed that the adsorption process was more consistent with the pseudo-first-order kinetics model and Langmuir isothermal adsorption model. The maximum adsorption capacity of MO reached 209.68 mg/g at 313.15 K. This study suggested that CCS-DETA can efficiently adsorb MO from aqueous solutions via amino and hydroxyl groups.

Key words: chitosan, hydrogel, methyl orange, adsorbent, chemical modification