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Dissolution and Transformation of ZnO Nano- and Microparticles in Soil Mineral Suspensions

  • Ping Wu
    Ping Wu
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, Jiangsu 210008, People’s Republic of China
    University of Chinese Academy of Sciences, Beijing 100049, People’s Republic of China
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  • , 
  • Peixin Cui
    Peixin Cui
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, Jiangsu 210008, People’s Republic of China
    More by Peixin Cui
  • , 
  • Huan Du
    Huan Du
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, Jiangsu 210008, People’s Republic of China
    More by Huan Du
  • , 
  • Marcelo E. Alves
    Marcelo E. Alves
    Departamento de Ciencias Exatas, Escola Superior de Agricultura “Luiz de Queiroz”, Universidade de São Paulo, Piracicaba, São Paulo 13418-900, Brazil
    More by Marcelo E. Alves
  • , 
  • Cun Liu
    Cun Liu
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, Jiangsu 210008, People’s Republic of China
    More by Cun Liu
  • , 
  • Dongmei Zhou
    Dongmei Zhou
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, Jiangsu 210008, People’s Republic of China
    More by Dongmei Zhou
    Orcidhttp://orcid.org/0000-0002-7917-7954
  • , and 
  • Yujun Wang*
    Yujun Wang
    Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, Jiangsu 210008, People’s Republic of China
    *Telephone: 86-25-86881182. Fax: 86-25-86881000. E-mail: [email protected]
    More by Yujun Wang
    Orcidhttp://orcid.org/0000-0002-0921-0122
Cite this: ACS Earth Space Chem. 2019, 3, 4, 495–502
Publication Date (Web):January 31, 2019
https://doi.org/10.1021/acsearthspacechem.8b00165
Copyright © 2019 American Chemical Society
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    Abstract

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    The increasing use of ZnO nanoparticles (NPs) has generated serious concern about their fate, transportation, and toxicity in the environment. The present study focuses on the key geochemical processes controlling the environmental fate of NPs, that is, dissolution and transformation of ZnO NPs in a large time scale with two common soil mineral (γ-Al2O3 and goethite) suspensions in batch reactors for up to 360 days using synchrotron-radiation powder X-ray diffraction, extended X-ray absorption fine structure spectroscopy, and high-resolution transmission electron microscopy. The aqueous dissolution experiments showed that smaller size ZnO NPs dissolved faster at lower pH. The combined spectroscopic analyses revealed that the interaction between ZnO NPs and γ-Al2O3 promoted dissolution of ZnO NPs by transforming into the Zn–Al-layered double hydroxide (LDH) precipitate at pH 7.5 within 0.5 h, and the fraction of Zn–Al LDH precipitate increased with the incubation time. At pH 5.5, Zn–Al LDH precipitate was also observed, which was attributed to the locally elevated pH and Zn concentration near the ZnO NP surface during the dissolution. In the presence of goethite, ZnO NPs dissolved less and Zn mainly existed as ZnCO3 at pH 5.5, but at pH 7.5, ZnO NPs barely dissolved and transformed, even with a prolonged incubation time. The findings of this study will facilitate a better understanding of the fate of ZnO NPs in soil mineral suspensions, which can be leveraged for remediation of ZnO NP-polluted soils.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsearthspacechem.8b00165.

    • Detailed sampling process (Text S1), XAFS data analyses (Text S2), parameters of the principal component analysis of ZnO NPs reacted in γ-Al2O3 suspensions (Table S1), parameters of the principal component analysis of ZnO NPs reacted in goethite suspensions (Table S2), SPOIL values for target transformation of ZnO reacted in γ-Al2O3 suspensions (Table S3), SPOIL values for target transformation of ZnO reacted in goethite suspensions (Table S4), EXAFS-based ZnO speciation in goethite suspensions at pH 5.5 and 7.5 (Table S5), results of EXAFS spectra data analysis of ZnO NPs reacted in γ-Al2O3 suspensions at pH 5.5 including coordination number (N), interatomic distance (R), and Debye–Waller factor (σ2) for neighboring shells (Table S6), results of EXAFS spectra data analysis of ZnO NPs reacted in γ-Al2O3 suspensions at pH 7.5 including coordination number (N), interatomic distance (R), and Debye–Waller factor (σ2) for neighboring shells (Table S7), results of EXAFS spectra data analysis of ZnO NPs reacted in goethite suspensions at pH 5.5 and 7.5 including coordination number (N), interatomic distance (R), and Debye–Waller factor (σ2) for neighboring shells (Table S8), raw (black line) and fitted (red line) k3-weighted corresponding Fourier transforms of Zn containing reference compounds and reaction in γ-Al2O3 suspensions at (A) pH 5.5 and (B) pH 7.5 (Figure S1), raw (black line) and fitted (red line) k3-weighted corresponding Fourier transforms of Zn containing reference compounds and reaction in goethite suspensions (Figure S2), SEM images of γ-Al2O3 (Figure S3), and TEM images of ZnO NPs reacted with γ-Al2O3 at (A) pH 5.5 and (B) pH 7.5 and EDS analysis of total and selected regions (1, 2, and 3) (Figure S4) (PDF)

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