Natural organic matter composition and nanomaterial surface coating determine the nature of platinum nanomaterial-natural organic matter corona
Natural organic matter composition and nanomaterial surface coating determine the nature of platinum nanomaterial-natural organic matter corona
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DOI：
10.1016/j.scitotenv.2021.150477
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发表时间：
2021-09-23
影响因子：
9.8
通讯作者：
Hess, Nancy J.
中科院分区：
文献类型：
--
作者：
Baalousha, Mohammed;Sikder, Mithun;Hess, Nancy J.
天然有机物电晕(NOM CORONA)是纳米材料(NMS)与周围环境之间的界面区域，决定了NMS独特的表面特性。虽然工程纳米材料(NMS)上天然有机物(NOM)电晕的形成对NM的行为、命运和毒性的重要性已经得到证实，但由于NOM的复杂性和异质性，对NOM分子性质如何影响NOM电晕组成的了解仍然很难理解。来自不同来源的名词的变化使情况变得更加复杂。我们用8个不同分子组成的NOM分离物和超高分辨率傅里叶变换离子回旋共振质谱仪(ESI-FT-ICR-MS)测定了铂NM-NOM电晕分子组成与NOM组成和表面涂层的关系。我们观察到，PtNM-NOM冠层的组成随原始NOM的组成而变化。形成PVP-PtNM-NOM电晕的NOM配方的百分比高于形成柠檬酸盐-PtNM-NOM电晕的NOM配方的百分比，这是因为NOM配方，特别是缩合碳氢化合物，在PVP涂层上的吸附增加。在PVP-PtNM-NOM-CORONA中，杂原子式(CHON、CHOS和CHOP)的相对丰度高于柠檬酸盐-PtNM-CORONA中的相对丰度，而柠檬酸盐-PtNM-CORONA中的相对丰度又高于原始NOM中的相对丰度，这表明富杂原子分子优先分配到NM表面。PtNM-NOM冠层中CHO、CHON、CHOS、CHOP和凝聚烃的相对丰度随其在NOM分离物中的增加而增加。此外，PtNM-NOM电晕富含高相对分子质量的化合物。研究表明，PtNM-NOM电晕的组成和性能取决于NOM的分子性质和PtNM表面涂层。这里的结果提供了NOM和NMS之间的分子相互作用的证据，这对于理解NM的胶体性质(例如，表面电荷和稳定性)、相互作用力(例如，范德华和疏水性)、环境行为(例如，聚集、溶解)至关重要。(C)2021年爱思唯尔B.V.保留所有权利。
Natural organic matter corona (NOM corona) is an interfacial area between nanomaterials (NMs) and the sur-rounding environment, which gives rise to NMs' unique surface identity. While the importance of the formation of natural organic matter (NOM) corona on engineered nanomaterials (NMs) to NM behavior, fate, and toxicity has been well-established, the understanding of how NOM molecular properties affect NOM corona composition remains elusive due to the complexity and heterogeneity of NOM. This is further complicated by the variation of NOMs from different origins. Here we use eight NOM isolates of different molecular composition and ultrahigh resolution Fourier-transform ion cyclotron resonance-mass spectrometry (ESI-FT-ICR-MS) to determine the mo-lecular composition of platinum NM-NOM corona as a function of NOM composition and NM surface coating. We observed that the composition of PtNM-NOM corona varied with the composition of the original NOM. The per-centage of NOM formulas that formed PVP-PtNM-NOM corona was higher than those formed citrate-PtNM-NOM corona, due to increased sorption of NOM formulas, in particular condensed hydrocarbons, to the PVP coating. The relative abundance of heteroatom formulas (CHON, CHOS, and CHOP) was higher in the PVP-PtNM-NOM co-rona than in citrate-PtNM-corona which was in turn higher than those in the original NOM isolate, indicating preferential partitioning of heteroatom-rich molecules to NM surfaces. The relative abundance of CHO, CHON, CHOS, CHOP and condensed hydrocarbons in PtNM-NOM corona increased with their increase in NOM isolates. Furthermore, PtNM-NOM corona is rich with compounds with high molecular weight. This study demonstrates that the composition and properties of PtNM-NOM corona depend on NOM molecular properties and PtNM surface coating. The results here provide evidence of molecular interactions between NOM and NMs, which are critical to understanding NM colloidal properties (e.g., surface charge and stability), interaction forces (e.g., van der Waals and hydrphobic), environmental behaviors (e.g., aggregation, disso. (c) 2021 Elsevier B.V. All rights reserved.