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Experimental measurements and numerical simulations of the transport and retention of nanocrystal CdSe/ZnS quantum dots in saturated porous media: effects of pH, organic ligand, and natural organic matter

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Abstract

The risks of environmental exposures of quantum dot (QD) nanoparticles are increasing, but these risks are difficult to assess because fundamental questions remain about factors affecting the mobility of QDs. The objective of this study is to help address this shortcoming by evaluating the physico-chemical mechanisms controlling the transport and retention of CdSe/ZnS QDs under various environmental conditions. The approach was to run a series of laboratory-scale column experiments where QDs were transported through saturated porous media with different pH values and concentrations of citrate and Suwannee River natural organic matter (SRNOM). Numerical simulations were then conducted and compared with the laboratory data in order to evaluate parameters controlling transport. QD suspensions were injected into the column in an upward direction and ICP-MS used to analyze Cd2+ concentrations (C) in column effluent and sand porous media samples. The increase in the background solution pH values enhanced the QD transport and decreased the QD retention. QD transport recovery percentages obtained from the column effluent samples were 2.6%, 83.2%, 101.7%, 96.5%, and 98.9%, at pH levels of 1.5, 3.5, 5, 7, and 9, respectively. The effects of citrate and SRNOM on the transport and retention of QDs were pH dependent as reflected in the influence of the electrostatic and steric interactions between QDs and sand surfaces. QDs were mobile under unfavorable deposition conditions at environmentally relevant pHs (i.e., 5, 7, and 9). Under favorable pH conditions for deposition (i.e., 1.5), QDs were completely retained within the porous media. The retention profiles of QDs showed a non-exponential decay with distance to the inlet, attributed to multiple deposition rates caused by the QD particles and surface heterogeneities of the quartz silica sand. Results of the diameter ratios of QDs to the median sand grains, in suspensions of DI water at pH 1.5, of citrate at pH 1.5, and of citrate at pH 3.5 indicate straining as the dominating mechanism for QD retention in porous media. The blocking effect and straining were significant under favorable deposition conditions and the detachment effect was non-negligible under unfavorable deposition conditions. Physico-chemical attachment and straining are the governing mechanisms that control the retention of QDs. Overall, experimental results indicate that aggregation, deposition, straining, blocking, and DLVO-type interactions affect the advective transport and retention of QDs in saturated porous media. The simulations were conducted using models that include terms describing attachment, detachment, and straining terms—model 1: M1-attachment, model 2: M2-attachment and detachment, model 3: M3-straining, and model 4: M4-attachment, detachment, and straining. The results from simulations with M2-attachment and detachment and M4-attachment, detachment, and straining matched best the observed breakthrough curves, but all four models inadequately described the retention profiles. Our findings demonstrate that QDs are mobile in porous media under a wide range of physico-chemical conditions representative of the natural environment. The mobility behavior of QDs in porous media indicated the potential risk of soil and groundwater contamination.

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Acknowledgments

We wish to convey our appreciation to Clemson University for supporting this research.

Availability of data

The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.

Funding

This material is based upon work supported by Clemson University.

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Authors and Affiliations

  1. Department of Environmental Engineering and Earth Sciences, Laboratory of Hydrogeoscience and Biological Engineering, L.G. Rich Environmental Laboratory, Clemson University, 342 Computer Court, Anderson, SC, 29625, USA

    Chunyan Li, Yu Xie, Brian A. Powell, Lawrence C. Murdoch & Christophe J. G. Darnault

  2. Department of Chemistry, University of Illinois at Chicago, 845 W. Taylor St, Chicago, IL, 60607, USA

    Asra Hassan, Marcell Palmai & Preston T. Snee

Authors
  1. Chunyan Li
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  2. Asra Hassan
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  3. Marcell Palmai
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  4. Yu Xie
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  5. Preston T. Snee
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  6. Brian A. Powell
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  7. Lawrence C. Murdoch
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  8. Christophe J. G. Darnault
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Contributions

Material preparation, data collection and analysis were performed by Chunyan Li, Asra Hassan, Marcell Palmai, Yu Xie, Preston T. Snee, Brian A. Powell, Lawrence C. Murdoch, and Christophe J. G. Darnault. The first draft of the manuscript was written by Chunyan Li and Christophe J. G. Darnault, and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Christophe J. G. Darnault.

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Li, C., Hassan, A., Palmai, M. et al. Experimental measurements and numerical simulations of the transport and retention of nanocrystal CdSe/ZnS quantum dots in saturated porous media: effects of pH, organic ligand, and natural organic matter. Environ Sci Pollut Res 28, 8050–8073 (2021). https://doi.org/10.1007/s11356-020-11097-0

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