Gutierrez Angela M, Leniz Francisco C, Wang Xinya, Dziubla Thomas D, Hilt J Zach
Department of Chemical and Materials Engineering, University of Kentucky, Lexington, KY, 40506, USA.
Superfund Research Center, University of Kentucky, Lexington, KY, 40506, USA.
Mater Sci Eng B Solid State Mater Adv Technol. 2022 Mar;277. doi: 10.1016/j.mseb.2021.115577. Epub 2021 Dec 24.
Water pollution continues to be one of the greatest challenges humankind faces worldwide. Increasing population growth, fast industrialization and modernization risk the worsening of water accessibility and quality in the coming years. Nanoadsorbents have steadily gained attention as remediation technologies that can meet stringent water quality demands. In this work, core-shell magnetic nanoparticles (MNPs) comprised of an iron oxide magnetic core and a styrene based polymer shell were synthesized via surface initiated atom transfer radical polymerization (SI-ATRP), and characterized them for their binding of polychlorinated biphenyls (PCBs), as model organic contaminants. Acrylated plant derived polyphenols, curcumin multiacrylate (CMA) and quercetin multiacrylate (QMA), and divinylbenzene (DVB) were incorporated into the polymeric shell to create high affinity binding sites for PCBs. The affinity of these novel materials for PCB 126 was evaluated and fitted to the nonlinear Langmuir model to determine binding affinities (K). The K values obtained for all the MNP systems showed higher binding affinities for PCB 126 that carbonaceous materials, like activated carbon and graphene oxide, the most widely used adsorption materials for water remediation today. The effect of increasing ATRP reaction time on the binding affinity of MNPs demonstrated the ability to tune polymer shell thickness by modifying the reaction extent and initial crosslinker concentrations in order to maximize pollutant binding. The enhancement in binding affinity and capacity for PCB 126 was demonstrated by the use of hydrophobic, aromatic rich molecules like styrene, CMA, QMA and DVB, within the polymeric shell provides more sites for π-π interactions to occur between the MNP surface and the PCB molecules. Overall, the high affinities for PCBs, as model organic pollutants, and magnetic capabilities of the core-shell MNPs synthesized provide a strong rationale for their application as nanoadsorbents in the environmental remediation of specific harmful contaminants.
水污染仍然是全世界人类面临的最大挑战之一。人口增长不断加快、快速工业化和现代化，有可能在未来几年使水的可获取性和质量恶化。纳米吸附剂作为能够满足严格水质要求的修复技术，已逐渐受到关注。在这项工作中，通过表面引发原子转移自由基聚合（SI-ATRP）合成了由氧化铁磁核和苯乙烯基聚合物壳组成的核壳磁性纳米颗粒（MNP），并对其结合多氯联苯（PCB）作为典型有机污染物的性能进行了表征。将丙烯酸化的植物源多酚、姜黄素多丙烯酸酯（CMA）和槲皮素多丙烯酸酯（QMA）以及二乙烯基苯（DVB）引入聚合物壳中，以创建对PCB具有高亲和力的结合位点。评估了这些新型材料对PCB 126的亲和力，并将其拟合到非线性朗缪尔模型以确定结合亲和力（K）。所有MNP系统获得的K值表明，它们对PCB 126的结合亲和力高于碳质材料，如活性炭和氧化石墨烯，而活性炭和氧化石墨烯是目前水修复中使用最广泛的吸附材料。增加ATRP反应时间对MNP结合亲和力的影响表明，通过改变反应程度和初始交联剂浓度来调节聚合物壳厚度的能力，以便使污染物结合最大化。在聚合物壳中使用苯乙烯、CMA、QMA和DVB等富含疏水芳香族分子，为MNP表面与PCB分子之间发生更多的π-π相互作用提供了更多位点，从而证明了对PCB 126结合亲和力和容量的增强。总体而言，合成的核壳MNP对作为典型有机污染物的PCB具有高亲和力以及磁性，为其作为纳米吸附剂应用于特定有害污染物的环境修复提供了有力的理论依据。
