Significance of Non-DLVO Interactions on the Co-Transport of Functionalized Multiwalled Carbon Nanotubes and Soil Nanoparticles in Porous Media
Significance of Non-DLVO Interactions on the Co-Transport of Functionalized Multiwalled Carbon Nanotubes and Soil Nanoparticles in Porous Media
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非 DLVO 相互作用对多孔介质中功能化多壁碳纳米管和土壤纳米颗粒共输运的意义
DOI：
10.1021/acs.est.2c00681
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发表时间：
2022
影响因子：
11.4
通讯作者：
Rongliang Qiu
中科院分区：
文献类型：
--
作者：
Miaoyue Zhang;Scott A. Bradford;Erwin Klumpp;Jiri Šimůnek;Shizhong Wang;Quan Wan;Chao Jin;Rongliang Qiu
Derjaguin-Landau-Verwey-Overbeek（DLVO）理论通常用于量化工程纳米颗粒（ENPs），土壤纳米颗粒（SNP）和/或多孔介质之间的表面相互作用，用于评估ENPs的环境风险和命运。本研究探讨了功能化多壁碳纳米管（MWCNTs）与正（针铁矿纳米颗粒，GNP）和负（膨润土纳米颗粒，BNP）带电的SNP在石英砂（QS）中的共输运行为。BNP的存在增加了MWCNTs的转运，但GNP抑制了MWCNTs的转运。此外，我们，第一次，观察到负（BNP）和正（GNP）电荷的SNP的运输是由多壁碳纳米管的存在下促进。与竞争性阻断、异源聚集和经典DLVO计算相关的传统机制无法解释此类现象。使用批实验和傅里叶变换红外（FTIR）光谱，耦合到UV和电感耦合等离子体质谱（AF 4-UV-ICP-MS）的不对称流场流分级（AF 4）和分子动力学（MD）模拟的直接检查表明，MWCNTs-BNP或MWCNT-GNP复合物或聚集体可以在共运输过程中形成。非DLVO相互作用（例如，氢键和刘易斯酸碱相互作用）有助于解释观察到的多壁碳纳米管沉积，多壁碳纳米管和两个SNP之间的关联（积极或消极），共运输。这项研究揭示了多孔介质中多壁碳纳米管和SNP的传输的新见解，并表明（i）胶体之间的相互作用（例如，异聚集，共运输和竞争性阻断）需要考虑在自然土壤中;和（ii）非DLVO相互作用时，应全面考虑环境风险和ENPs的命运。
Derjaguin-Landau-Verwey-Overbeek (DLVO) theory is typically used to quantify surface interactions between engineered nanoparticles (ENPs), soil nanoparticles (SNPs), and/or porous media, which are used to assess environmental risk and fate of ENPs. This study investigates the co-transport behavior of functionalized multiwalled carbon nanotubes (MWCNTs) with positively (goethite nanoparticles, GNPs) and negatively (bentonite nanoparticles, BNPs) charged SNPs in quartz sand (QS). The presence of BNPs increased the transport of MWCNTs, but GNPs inhibited the transport of MWCNTs. In addition, we, for the first time, observed that the transport of negatively (BNPs) and positively (GNPs) charged SNPs was facilitated by the presence of MWCNTs. Traditional mechanisms associated with competitive blocking, heteroaggregation, and classic DLVO calculations cannot explain such phenomena. Direct examination using batch experiments and Fourier transform infrared (FTIR) spectroscopy, asymmetric flow field flow fractionation (AF4) coupled to UV and inductively coupled plasma mass spectrometry (AF4-UV-ICP-MS), and molecular dynamics (MD) simulations demonstrated that MWCNTs-BNPs or MWCNT-GNPs complexes or aggregates can be formed during co-transport. Non-DLVO interactions (e.g., H-bonding and Lewis acid-base interaction) helped to explain observed MWCNT deposition, associations between MWCNTs and both SNPs (positively or negatively), and co-transport. This research sheds novel insight into the transport of MWCNTs and SNPs in porous media and suggests that (i) mutual effects between colloids (e.g., heteroaggregation, co-transport, and competitive blocking) need to be considered in natural soil; and (ii) non-DLVO interactions should be comprehensively considered when evaluating the environmental risk and fate of ENPs.