Chemical trigger toward phase separation in the aqueous Al(III) system revealed

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Science Advances ; 6 (2020), 23. - eaba6878. - American Association for the Advancement of Science (AAAS). - eISSN 2375-2548
Abstract
Although Al(III) hydrolysis, condensation, and nucleation play pivotal roles in the synthesis of Al-based compounds and determine their chemical behavior, we still lack experimental evidence regarding the chemistry of nucleation from solution. Here, by combining advanced titration assays, high-resolution transmission electron microscopy (HR-TEM), and 27Al–nuclear magnetic resonance spectroscopy, we show that highly dynamic solute prenucleation clusters (PNCs) are fundamental precursors of nanosolid formation. Chemical changes from olation to oxolation bridging within PNCs rely on the formation of tetrahedral AlO4 in solution and trigger phase separation at low driving force (supersaturation). This does not include the formation of Keggin-Al13 ions, at least during the earliest stages. The PNC pathway of the formation of Al(III) (oxy)(hydr)oxides offers new possibilities toward the development of strategies for controlling the entire crystallization process.
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ISO 690LUKIĆ, Miodrag J., Eduard WIEDENBECK, Holger REINER, Denis GEBAUER, 2020. Chemical trigger toward phase separation in the aqueous Al(III) system revealed. In: Science Advances. American Association for the Advancement of Science (AAAS). 6(23), eaba6878. eISSN 2375-2548. Available under: doi: 10.1126/sciadv.aba6878
BibTex
@article{Lukic2020-06Chemi-50255,
  year={2020},
  doi={10.1126/sciadv.aba6878},
  title={Chemical trigger toward phase separation in the aqueous Al(III) system revealed},
  number={23},
  volume={6},
  journal={Science Advances},
  author={Lukić, Miodrag J. and Wiedenbeck, Eduard and Reiner, Holger and Gebauer, Denis},
  note={Article Number: eaba6878}
}
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    <dcterms:abstract xml:lang="eng">Although Al(III) hydrolysis, condensation, and nucleation play pivotal roles in the synthesis of Al-based compounds and determine their chemical behavior, we still lack experimental evidence regarding the chemistry of nucleation from solution. Here, by combining advanced titration assays, high-resolution transmission electron microscopy (HR-TEM), and 27Al–nuclear magnetic resonance spectroscopy, we show that highly dynamic solute prenucleation clusters (PNCs) are fundamental precursors of nanosolid formation. Chemical changes from olation to oxolation bridging within PNCs rely on the formation of tetrahedral AlO4 in solution and trigger phase separation at low driving force (supersaturation). This does not include the formation of Keggin-Al13 ions, at least during the earliest stages. The PNC pathway of the formation of Al(III) (oxy)(hydr)oxides offers new possibilities toward the development of strategies for controlling the entire crystallization process.</dcterms:abstract>
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