Department of Civil and Environmental Engineering, Duke University , Durham, North Carolina 27708, United States.
U.S. Geological Survey, Boulder, Colorado 80303, United States.
Environ Sci Technol. 2015 Oct 6;49(19):11476-84. doi: 10.1021/acs.est.5b02406. Epub 2015 Sep 23.
The dissolution of zinc oxide (ZnO) nanoparticles (NPs) is a key step of controlling their environmental fate, bioavailability, and toxicity. Rates of dissolution often depend upon factors such as interactions of NPs with natural organic matter (NOM). We examined the effects of 16 different NOM isolates on the dissolution kinetics of ZnO NPs in buffered potassium chloride solution using anodic stripping voltammetry to directly measure dissolved zinc concentrations. The observed dissolution rate constants (kobs) and dissolved zinc concentrations at equilibrium increased linearly with NOM concentration (from 0 to 40 mg C L(-1)) for Suwannee River humic and fulvic acids and Pony Lake fulvic acid. When dissolution rates were compared for the 16 NOM isolates, kobs was positively correlated with certain properties of NOM, including specific ultraviolet absorbance (SUVA), aromatic and carbonyl carbon contents, and molecular weight. Dissolution rate constants were negatively correlated to hydrogen/carbon ratio and aliphatic carbon content. The observed correlations indicate that aromatic carbon content is a key factor in determining the rate of NOM-promoted dissolution of ZnO NPs. The findings of this study facilitate a better understanding of the fate of ZnO NPs in organic-rich aquatic environments and highlight SUVA as a facile and useful indicator of NOM interactions with metal-based nanoparticles.
氧化锌(ZnO)纳米粒子(NPs)的溶解是控制其环境归宿、生物可利用性和毒性的关键步骤。溶解速率通常取决于 NPs 与天然有机物(NOM)的相互作用等因素。我们使用阳极溶出伏安法(anodic stripping voltammetry)直接测量溶解锌浓度,考察了 16 种不同 NOM 分离物对缓冲氯化钾溶液中 ZnO NPs 溶解动力学的影响。对于苏万尼河腐殖酸和富里酸以及庞尼湖富里酸,观察到的溶解速率常数(kobs)和平衡时的溶解锌浓度随 NOM 浓度(从 0 增加到 40 mg C L(-1))呈线性增加。当对 16 种 NOM 分离物进行溶解速率比较时,kobs 与 NOM 的某些特性呈正相关,包括特定紫外吸光度(SUVA)、芳香碳和羰基碳含量以及分子量。溶解速率常数与氢/碳比和脂肪碳含量呈负相关。观察到的相关性表明,芳香碳含量是决定 NOM 促进 ZnO NPs 溶解速率的关键因素。本研究的结果有助于更好地理解富含有机物的水生环境中 ZnO NPs 的命运,并强调 SUVA 是 NOM 与基于金属的纳米粒子相互作用的简便有用指标。