Understanding the Interactions of Nanoparticles and Dissolved Organic Matter at the Molecular Level by 1H 2D Multi-Exponential Transverse Relaxation NMR Spectroscopy.

IF 1.9 3区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY Magnetic Resonance in Chemistry Pub Date : 2024-10-16 DOI:10.1002/mrc.5487
Malak Dia, Jonathan Farjon, Clotilde Raveleau, André Simpson, Pierre-Emmanuel Peyneau, Béatrice Béchet, Denis Courtier-Murias
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Abstract

The interaction between humic acid (HA) and engineered nanoparticles (NPs) is critical in environmental sciences, especially for understanding the behavior of NPs in natural waters. This study employs 1H 2D Multi-Exponential Transverse Relaxation (METR) NMR spectroscopy to examine the molecular-level interactions between Pahokee Peat humic acid (HA) and carboxyl-functionalized iron oxide nanoparticles (NPCOs). First, 1H 2D METR NMR spectroscopy allowed not only the identification of HA in terms of its chemical composition but also the separation of molecules with the same chemical shift values but different rates of molecular tumbling. Then, using solutions with varying NPCO concentrations (0, 10, 40, and 100 μM), we observed significant changes in the T2 relaxation times of HA components, indicating interactions between HA and NPCO. Analysis showed the biggest effect on two chemical shift regions, corresponding to lipids and carbohydrates, revealing that smaller molecules within these regions exhibit the most significant changes in T2 values upon the addition of NPCO. This suggests that these molecules are the initial sites of interaction, with the entire HA system being affected at higher NPCO concentrations. These findings highlight the utility of METR NMR spectroscopy in studying complex environmental mixtures and provide insights into the behavior of HA and NPs, essential for understanding the fate of NPs in the environment.

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通过 1H 2D 多指数横向弛豫 NMR 光谱了解纳米粒子与溶解有机物在分子水平上的相互作用。
腐植酸(HA)与工程纳米粒子(NPs)之间的相互作用在环境科学中至关重要,特别是对于了解天然水体中 NPs 的行为。本研究采用 1H 2D 多指数横向弛豫(METR)核磁共振波谱来研究帕霍基泥炭腐植酸(HA)与羧基功能化氧化铁纳米粒子(NPCOs)之间的分子级相互作用。首先,通过 1H 2D METR NMR 光谱不仅可以识别 HA 的化学成分,还可以分离出化学位移值相同但分子翻滚速率不同的分子。然后,使用不同浓度的 NPCO 溶液(0、10、40 和 100 μM),我们观察到 HA 成分的 T2 弛豫时间发生了显著变化,这表明 HA 与 NPCO 之间存在相互作用。分析表明,与脂质和碳水化合物相对应的两个化学位移区域受到的影响最大,这表明在添加 NPCO 后,这些区域中的小分子在 T2 值上表现出最显著的变化。这表明这些分子是相互作用的初始位点,当 NPCO 浓度较高时,整个 HA 系统都会受到影响。这些发现凸显了 METR NMR 光谱在研究复杂环境混合物方面的实用性,并提供了有关 HA 和 NPs 行为的见解,这对了解 NPs 在环境中的归宿至关重要。
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来源期刊
CiteScore
4.70
自引率
10.00%
发文量
99
审稿时长
1 months
期刊介绍: MRC is devoted to the rapid publication of papers which are concerned with the development of magnetic resonance techniques, or in which the application of such techniques plays a pivotal part. Contributions from scientists working in all areas of NMR, ESR and NQR are invited, and papers describing applications in all branches of chemistry, structural biology and materials chemistry are published. The journal is of particular interest not only to scientists working in academic research, but also those working in commercial organisations who need to keep up-to-date with the latest practical applications of magnetic resonance techniques.
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