Liang Weiyu, Zhang Wen, Shao Xuechun, Gong Kailin, Su Chengpeng, Zhang Wei, Peng Cheng
State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resource and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China.
John A. Reif, Jr. Department of Civil and Environmental Engineering, New Jersey Institute of Technology, Newark, NJ, United States.
J Hazard Mater. 2024 Apr 5;467:133769. doi: 10.1016/j.jhazmat.2024.133769. Epub 2024 Feb 13.
The widespread use of Cd-based quantum dots (Cd-QDs) has led to their inevitable release into the environment, and the prevalent iron oxides and natural organic matter (NOM) are the key factors affecting the environmental behavior and fate of Cd-QDs. However, the impact of NOM adsorbed on iron oxides on the behavior of Cd-QDs with iron oxides and the mechanism of its interaction are not clear. In this study, two kinds of water-soluble QDs (CdSe QDs and core-shell CdSe/ZnS QDs) were selected to study the aggregation and adsorption behavior on goethite (Goe) and goethite-humic acid/fulvic acid composites (Goe-HA/FA). Aggregation kinetics and adsorption experiments between QDs and Goe(-HA/FA), characterization, and extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory calculations indicated that electrostatic interaction was the dominant force for QDs adsorption on Goe(-HA/FA). HA/FA changed the surface charge of Goe and increased the electrostatic repulsion and steric hindrance between the particles, which in turn inhibited the adsorption of QDs on Goe. Besides, unsubstituted aromatic carbons, carboxy carbons, and carbonyl carbons played an important role in the adsorption process, and chemisorption occurred between QDs and Goe(-HA/FA). Our findings are important for better assessing the transport, fate, and potential environmental impacts and risks of Cd-QDs in iron-rich environments.
基于镉的量子点(Cd-QDs)的广泛使用导致其不可避免地释放到环境中,而普遍存在的铁氧化物和天然有机物(NOM)是影响Cd-QDs环境行为和归宿的关键因素。然而,吸附在铁氧化物上的NOM对Cd-QDs与铁氧化物行为的影响及其相互作用机制尚不清楚。本研究选择了两种水溶性量子点(CdSe量子点和核壳型CdSe/ZnS量子点),研究其在针铁矿(Goe)以及针铁矿-腐殖酸/富里酸复合材料(Goe-HA/FA)上的聚集和吸附行为。量子点与Goe(-HA/FA)之间的聚集动力学和吸附实验、表征以及扩展的Derjaguin-Landau-Verwey-Overbeek(XDLVO)理论计算表明,静电相互作用是量子点吸附在Goe(-HA/FA)上的主导力。HA/FA改变了Goe的表面电荷,增加了颗粒间的静电排斥和空间位阻,进而抑制了量子点在Goe上的吸附。此外,未取代的芳香碳、羧基碳和羰基碳在吸附过程中起重要作用,量子点与Goe(-HA/FA)之间发生了化学吸附。我们的研究结果对于更好地评估富铁环境中Cd-QDs的迁移、归宿以及潜在的环境影响和风险具有重要意义。