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Arsenite oxyanions affect CeO₂ nanoparticle dissolution and colloidal stability

Neil, Chelsea W. and Wu, Xuanhao and Kim, Doyoon and Jung, Haesung and Zhu, Yanzhe and Ray, Jessica R. and Jun, Young-Shin (2021) Arsenite oxyanions affect CeO₂ nanoparticle dissolution and colloidal stability. Environmental Science: Nano, 8 (1). pp. 233-244. ISSN 2051-8153. doi:10.1039/d0en00970a.

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While highly reactive cerium oxide nanoparticles (CeO₂ NPs) are widely used in industry, their transport in aquatic systems is not well understood. To fill this knowledge gap, the interactions of CeO₂ NPs with arsenite (As³⁺), a toxic metalloid and potential co-present contaminant, were investigated with respect to CeO₂ NP colloidal stability, dissolution, and surface redox reactions. Arsenite showed distinctive effects at different concentrations, with a high As³⁺ concentration (10⁻⁴ M) inducing 90% of CeO₂ NPs to settle from solution after 8 hours, while lower As³⁺ concentrations (10⁻⁵ or 10⁻⁶ M) led to only 20% of CeO₂ NPs settling. The dissolution of NPs was most significant in the 10⁻⁵ M As³⁺ system owing to a lesser extent of aggregation, exposing more CeO₂ surface for dissolution. In the three As³⁺ concentration systems, >97% of aqueous arsenic remained as As³⁺ over 6 hours. On the NP surface, adsorbed As^(III) was oxidized to As^V, resulting in 58–70% of the adsorbed arsenic remaining as As^(III). Simultaneously Ce^(IV) was reduced to Ce^(III), increasing Ce^(III) on the CeO₂ NP surface from 17% (without arsenite) to 21–25% (with arsenite). Further mechanistic analyses revealed that the adsorption of arsenite was the main contributor to neutralizing the CeO₂ NP surface potential, enhancing particle sedimentation. These findings suggest that the fate and transport of CeO₂ NPs in our experimental systems are strongly affected by arsenite concentration and its adsorption on NPs. The results also highlight the importance of the interplay between NP aggregation, oxidation, and dissolution in predicting the behaviors of CeO₂ NPs and associated toxic elements in aquatic systems.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Neil, Chelsea W.0000-0002-7679-157X
Wu, Xuanhao0000-0001-6177-6089
Kim, Doyoon0000-0001-9496-5556
Jung, Haesung0000-0002-8795-248X
Zhu, Yanzhe0000-0002-2260-1830
Ray, Jessica R.0000-0002-9964-3799
Jun, Young-Shin0000-0003-4648-2984
Alternate Title:Arsenite oxyanions affect CeO2 nanoparticle dissolution and colloidal stability
Additional Information:© The Royal Society of Chemistry 2021. Received 21st September 2020, Accepted 25th November 2020, First published 25 Nov 2020. This work is supported by the National Science Foundation's Environmental Chemical Science Program (CHE-1214090). J. R. R. was supported by an Environmental Protection Agency STAR Fellowship, and C. W. N. was supported by a Mr. and Mrs. Spencer T. Olin Fellowship. We wish to thank our Environmental NanoChemistry Group members for their valuable discussions. The authors acknowledge Professor James C. Ballard for reviewing the manuscript, and Washington University's Institute of Materials Science & Engineering (IMSE) for the use of XPS and TEM. Los Alamos National Laboratory, an affirmative action/equal opportunity employer, is operated by Triad National Security, LLC, for the National Nuclear Security Administration of U.S. Department of Energy (contract no. 89233218CNA000001). By approving this article, the publisher recognizes that the U.S. Government retains nonexclusive, royalty-free license to publish or reproduce the published form of this contribution, or to allow others to do so, for U.S. Government purposes. Los Alamos National Laboratory requests that the publisher identify this article as work performed under the auspices of the U.S. Department of Energy. Los Alamos National Laboratory strongly supports academic freedom and a researcher's right to publish; as an institution, however, the Laboratory does not endorse the viewpoint of a publication or guarantee its technical correctness. There are no conflicts to declare.
Funding AgencyGrant Number
Environmental Protection Agency (EPA)FP91749501
Mr. and Mrs. Spencer T. Olin FellowshipUNSPECIFIED
Department of Energy (DOE)89233218CNA000001
Issue or Number:1
Record Number:CaltechAUTHORS:20210311-141939061
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Official Citation:Arsenite oxyanions affect CeO₂ nanoparticle dissolution and colloidal stability. Environ. Sci.: Nano, 2021, 8, 233-244; DOI: 10.1039/d0en00970a
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108406
Deposited By: Tony Diaz
Deposited On:12 Mar 2021 18:56
Last Modified:16 Nov 2021 19:11

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