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交联壳聚糖的机械化学合成及其作为吸附剂从模拟电镀废水中去除全氟和多氟烷基物质的应用

Mechanochemical Synthesis of Cross-Linked Chitosan and Its Application as Adsorbent for Removal of Per- and Polyfluoroalkyl Substances from Simulated Electroplating Wastewater.

作者信息

Cagnetta Giovanni, Yin Zhou, Qiu Wen, Vakili Mohammadtaghi

机构信息

Faculty of Geosciences and Environmental Engineering, Southwest Jiaotong University, Chengdu 610031, China.

State Key Joint Laboratory of Environment Simulation and Pollution Control (SKLESPC), Beijing Key Laboratory for Emerging Organic Contaminants Control, School of Environment, Tsinghua University, Beijing 100084, China.

出版信息

Materials (Basel). 2024 Jun 19;17(12):3006. doi: 10.3390/ma17123006.

DOI:10.3390/ma17123006
PMID:38930375
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11205816/
Abstract

Chitosan is a promising adsorbent for removing a wide range of pollutants from wastewater. However, its practical application is hindered by instability in acidic environments, which significantly impairs its adsorption capacity and limits its utilization in water purification. While cross-linking can enhance the acid stability of chitosan, current solvent-based methods are often costly and environmentally unfriendly. In this study, a solvent-free mechanochemical process was developed using high-energy ball milling to cross-link chitosan with various polyanionic linkers, including dextran sulfate (DS), poly[4-styrenesulfonic acid-co-maleic acid] (PSSM), and tripolyphosphate (TPP). The mechanochemically cross-linked (MCCL) chitosan products exhibited superior adsorption capacity and stability in acidic solutions compared to pristine chitosan. Chitosan cross-linked with DS (Cht-DS) showed the highest Reactive Red 2 (RR2) adsorption capacity, reaching 1559 mg·g at pH 3, followed by Cht-PSSM (1352 mg·g) and Cht-TPP (1074 mg·g). The stability of MCCL chitosan was visually confirmed by the negligible mass loss of Cht-DS and Cht-PSSM tablets in pH 3 solution, unlike the complete dissolution of the pristine chitosan tablet. The MCCL significantly increased the microhardness of chitosan, with the order Cht-DS > Cht-PSSM > Cht-TPP, consistent with the RR2 adsorption capacity. When tested on simulated rinsing wastewater from chromium electroplating, Cht-DS effectively removed Cr(VI) (98.75% removal) and three per- and polyfluoroalkyl substances (87.40-95.87% removal), following pseudo-second-order adsorption kinetics. This study demonstrates the potential of the cost-effective and scalable MCCL approach to produce chitosan-based adsorbents with enhanced stability, mechanical strength, and adsorption performance for treating highly acidic industrial wastewater containing a mixture of toxic pollutants.

摘要

壳聚糖是一种很有前景的吸附剂，可用于去除废水中的多种污染物。然而，其在酸性环境中的不稳定性阻碍了它的实际应用，这显著损害了其吸附能力，并限制了其在水净化中的应用。虽然交联可以提高壳聚糖的酸稳定性，但目前基于溶剂的方法往往成本高昂且对环境不友好。在本研究中，通过高能球磨开发了一种无溶剂机械化学工艺，用于使壳聚糖与各种聚阴离子交联剂交联，包括硫酸葡聚糖（DS）、聚[4-苯乙烯磺酸-co-马来酸]（PSSM）和三聚磷酸钠（TPP）。与原始壳聚糖相比，机械化学交联（MCCL）壳聚糖产品在酸性溶液中表现出优异的吸附能力和稳定性。与DS交联的壳聚糖（Cht-DS）对活性红2（RR2）的吸附能力最高，在pH 3时达到1559 mg·g，其次是Cht-PSSM（1352 mg·g）和Cht-TPP（1074 mg·g）。通过观察Cht-DS和Cht-PSSM片剂在pH 3溶液中的质量损失可忽略不计，直观地证实了MCCL壳聚糖的稳定性，这与原始壳聚糖片剂的完全溶解不同。MCCL显著提高了壳聚糖的显微硬度，顺序为Cht-DS > Cht-PSSM > Cht-TPP，这与RR2吸附能力一致。在对镀铬模拟漂洗废水进行测试时，Cht-DS遵循准二级吸附动力学，有效去除了Cr(VI)（去除率98.75%）和三种全氟和多氟烷基物质（去除率87.40 - 95.87%）。本研究证明了具有成本效益且可扩展的MCCL方法在生产基于壳聚糖的吸附剂方面的潜力，这些吸附剂具有增强的稳定性、机械强度和吸附性能，可用于处理含有有毒污染物混合物的高酸性工业废水。

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