Department of Plant, Soil and Insect Sciences, University of Massachusetts, Amherst, Massachusetts 01003, USA.
Langmuir. 2011 Jul 5;27(13):8036-43. doi: 10.1021/la200772e. Epub 2011 Jun 8.
The colloidal behavior of natural organic matter (NOM) and synthetic poly(acrylic acid) (PAA)-coated ferrimagnetic (γFe(2)O(3)) nanoparticles (NPs) was investigated. Humic acid (HA), an important component of NOM, was extracted from a peat soil. Two different molecular weight PAAs were also used for coating. The colloidal stability of the coated magnetic NPs was evaluated as a resultant of the attractive magnetic dipolar and van der Waals forces and the repulsive electrostatic and steric-electrosteric interactions. The conformational alterations of the polyelectrolytes adsorbed on magnetic γFe(2)O(3) NPs and their role in colloidal stability were determined. Pure γFe(2)O(3) NPs were extremely unstable because of aggregation in aqueous solution, but a significant stability enhancement was observed after coating with polyelectrolytes. The steric stabilization factor induced by the polyelectrolyte coating strongly dictated the colloidal stability. The pH-induced conformational change of the adsorbed, weakly charged polyelectrolytes had a significant effect on the colloidal stability. Atomic force microscopy (AFM) revealed the stretched conformation of the HA molecular chains adsorbed on the γFe(2)O(3) NP surface at pH 9, which enhanced the colloidal stability through long-range electrosteric stabilization. The depletion of the polyelectrolyte during the dilution of the NP suspension decreased the colloidal stability under acidic solution conditions. The conformation of the polyelectrolytes adsorbed on the NP surface was altered as a function of the substrate surface charge as viewed from AFM imaging. The polyelectrolyte coating also led to a reduction in magnetic moments and decreased the coercivity of the coated γFe(2)O(3) NPs. Thus, the enhanced stabilization of the coated maghematite NPs may facilitate their delivery in the groundwater for the effective removal of contaminants.
研究了天然有机物 (NOM) 和合成聚 (丙烯酸) (PAA)-包覆的亚铁磁性 (γFe(2)O(3)) 纳米粒子 (NPs) 的胶体行为。腐殖酸 (HA) 是 NOM 的重要组成部分,从泥炭土中提取得到。还使用了两种不同分子量的 PAA 进行包覆。评估了包覆磁性 NPs 的胶体稳定性,这是由于吸引力磁偶极和范德华力以及排斥静电和空间位阻 - 静电相互作用的结果。确定了吸附在磁性 γFe(2)O(3) NPs 上的高分子的构象变化及其在胶体稳定性中的作用。由于在水溶液中聚集,纯 γFe(2)O(3) NPs 极不稳定,但在涂覆聚电解质后观察到显著的稳定性增强。聚电解质涂层引起的空间稳定因子强烈决定了胶体稳定性。吸附的弱带电聚电解质的 pH 诱导构象变化对胶体稳定性有显著影响。原子力显微镜 (AFM) 揭示了在 pH 9 时吸附在 γFe(2)O(3) NP 表面上的 HA 分子链的伸展构象,通过长程静电稳定作用增强了胶体稳定性。在酸性溶液条件下,NP 悬浮液稀释过程中聚电解质的耗散降低了胶体稳定性。从 AFM 成像可以看出,吸附在 NP 表面上的聚电解质的构象随基质表面电荷的变化而变化。聚电解质涂层还导致包覆的 γFe(2)O(3) NPs 的磁矩降低和矫顽力减小。因此,包覆磁赤铁矿 NPs 的稳定性增强可能有助于它们在地下水环境中的输送,从而有效去除污染物。