Degradable sugar-based magnetic hybrid nanoparticles for recovery of crude oil from aqueous environments
Degradable sugar-based magnetic hybrid nanoparticles for recovery of crude oil from aqueous environments
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DOI：
10.1039/d0py00029a
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发表时间：
2020-08-14
影响因子：
4.6
通讯作者：
Wooley, Karen L.
中科院分区：
文献类型：
--
作者：
Dong, Mei;Song, Yue;Wooley, Karen L.
在这项工作中，我们设计并制造了一种纳米级糖基磁性混合材料，该材料能够解决海洋漏油造成的环境污染，同时最大限度地减少微塑料污染可能发生的潜在二次问题。这些易于定义的磁性纳米复合材料是通过磁性氧化铁纳米颗粒（MIONs）和可降解的两亲性聚合物聚（poly）的共组装而构建的。（乙二醇）-b-多巴胺官能化聚（乙基炔丙基葡萄糖碳酸酯）-b-聚（乙基葡萄糖碳酸酯），PEG-b-PGC[（EPC-MPA）-co-（EPC-DOPA）]-b-PGC（EC），通过在水中的超分子共组装驱动，通过多巴胺和MION之间的络合提供增强的相互作用。复合纳米组装体具有假胶束结构，MION被捕获在聚合物框架内。通过PEG大分子引发剂引发的两种葡萄糖衍生的碳酸酯单体的顺序开环聚合（ROP）来合成三嵌段嵌段共聚物。随后通过首先使用硫醇-炔点击反应引入羧酸基团，然后用多巴胺酰胺化来安装多巴胺锚定基团。所得的两亲性三嵌段共聚物和MION的共组装，以提供杂化纳米复合材料使用溶剂交换过程从有机溶剂到水。与疏水相互作用相结合，多巴胺和氧化铁之间的连接稳定了整体纳米级结构，以允许建立均匀的球形形态，而尝试与缺乏多巴胺侧链的三嵌段前体共组装，未能提供明确的纳米结构。磁性杂化纳米颗粒表现出高的吸油能力，约。8倍于其初始干重，部分归因于大的表面积，导致纳米材料和碳氢化合物污染物之间的有效接触。此外，天然衍生的聚合物框架经历水解降解，如果在部署后未回收，则分解成包括葡萄糖、乙醇和多巴胺的副产物，从而减轻了对潜在微塑料产生和持久性的担忧。
In this work, we designed and fabricated a nanoscopic sugar-based magnetic hybrid material that is capable of tackling environmental pollution posed by marine oil spills, while minimizing potential secondary problems that may occur from microplastic contamination. These readily-defined magnetic nanocomposites were constructed through co-assembly of magnetic iron oxide nanoparticles (MIONs) and a degradable amphiphilic polymer, poly(ethylene glycol)-b-dopamine-functionalized poly(ethyl propargyl glucose carbonate)-b-poly(ethyl glucose carbonate), PEG-b-PGC[(EPC-MPA)-co-(EPC-DOPA)]-b-PGC (EC), driven by supramolecular co-assembly in water with enhanced interactions provided via complexation between dopamine and MIONs. The composite nanoscopic assemblies possessed a pseudo-micellar structure, with MIONs trapped within the polymer framework. The triblock terpolymer was synthesized by sequential ring-opening polymerizations (ROPs) of two glucose-derived carbonate monomers, initiated by a PEG macroinitiator. Dopamine anchoring groups were subsequently installed by first introducing carboxylic acid groups using a thiol-yne click reaction, followed by amidation with dopamine. The resulting amphiphilic triblock terpolymers and MIONs were co-assembled to afford hybrid nanocomposites using solvent exchange processes from organic solvent to water. In combination with hydrophobic interactions, the linkage between dopamine and iron oxide stabilized the overall nanoscopic structure to allow for the establishment of a uniform globular morphology, whereas attempts at co-assembly with the triblock terpolymer precursor, lacking dopamine side chains, failed to afford well-defined nanostructures. The magnetic hybrid nanoparticles demonstrated high oil sorption capacities, ca. 8 times their initial dry weight, attributed, in part, to large surface areas leading to effective contact between the nanomaterials and hydrocarbon pollutants. Moreover, the naturally-derived polymer framework undergoes hydrolytic degradation to break down into byproducts that include glucose, ethanol and dopamine if not recovered after deployment, alleviating concerns of potential microplastic generation and persistence.