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Coating ligand-mediated dynamic formation of natural organic matter (NOM) corona on engineered nanoparticles in natural environments
Environmental Science: Nano ( IF 5.8 ) Pub Date : 2021-3-8 , DOI: 10.1039/d0en01223h
Chuan-Wang Yang 1, 2, 3, 4, 5 , Li Yuan 1, 2, 3, 4, 5 , Hong-Zhi Zhou 1, 2, 3, 4, 5 , Xin Zhang 1, 2, 3, 4, 5 , Guo-Ping Sheng 1, 2, 3, 4, 5
Affiliation  

Natural organic matter (NOM) can adsorb onto engineered nanoparticles (ENPs) and form NOM-corona on the ENP–solution interface, thus affecting the performance and ecotoxicity of ENPs in natural environments. Nevertheless, the formation dynamics of the NOM-corona on ENP surfaces as well as the role of coating ligands during the dynamic adsorption process are largely unknown. In this study, with silver nanoparticles (AgNPs) as the representative ENPs, the interaction between NOM and ENPs and the dynamic formation of NOM-corona were systematically investigated. NOM showed high adsorption affinity toward AgNPs with a large adsorption equilibrium constant (0.18 ± 0.01 L per mg C), thus leading to the fast formation of NOM-corona in several minutes and the enhanced nanoparticle stability under high salinity. As the important intermediary on the ENP–solution interface, coating ligands, such as citrate and polyvinylpyrrolidone, can substantially affect the dynamics and the equilibrium constant of NOM-corona formation. Moreover, NOM-corona formation was also reshaped by the coating ligands through adsorption, ligand exchange, and overcoating mechanisms. These mechanisms were illuminated by spectral investigations and theoretical calculations that NOM and polyvinylpyrrolidone have high binding abilities toward AgNP surfaces while citrate is more susceptible to replacement. This work provides a deeper understanding of the formation dynamics of the NOM-corona and the important role of coating ligands, which will facilitate the rational design of the surface chemistry of ENPs for nano-based environmental applications and the accurate prediction of the ENP fates in natural environments.

中文翻译:

在自然环境中,涂层配体介导的工程纳米颗粒上天然有机物(NOM)电晕的动态形成

天然有机物(NOM)可以吸附到工程纳米颗粒(ENP)上,并在ENP-溶液界面上形成NOM电晕,从而影响ENP在自然环境中的性能和生态毒性。尽管如此,在ENP表面上NOM电晕的形成动力学以及在动态吸附过程中涂层配体的作用仍是未知之数。在这项研究中,以银纳米颗粒(AgNPs)为代表的ENP,系统地研究了NOM和ENP之间的相互作用以及NOM电晕的动态形成。NOM对具有较大吸附平衡常数(0.18±0.01 L / mg C)的AgNPs表现出高吸附亲和力,因此导致几分钟内NOM电晕快速形成,并在高盐度下增强了纳米颗粒的稳定性。作为ENP-溶液界面上的重要中间物,涂层配体(例如柠檬酸盐和聚乙烯吡咯烷酮)会大大影响NOM电晕形成的动力学和平衡常数。而且,NOM-电晕的形成也通过涂层配体通过吸附,配体交换和重涂机制而得以重塑。通过光谱研究和理论计算阐明了这些机制,即NOM和聚乙烯吡咯烷酮对AgNP表面具有高结合能力,而柠檬酸盐更易于替代。这项工作可更深入地了解NOM电晕的形成动力学以及涂层配体的重要作用,
更新日期:2021-03-25
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