4.7 Article

Phosphate adsorption on amorphous aluminum hydroxide-yielded transition aluminas: Insights on fundamental chemistry and making engineering adsorbents

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DOI: 10.1016/j.jwpe.2023.103677

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Transition alumina; Phosphate adsorption; Fraction of amorphous contents; Al -O arrangement; Gibbs energy of adsorption

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Transition aluminas (TAs) are alumina polymorphs used for water remediation. This study investigates the structure-binding activity of pollutants and phosphate adsorption on TAs. It is found that the structure disorders of TAs affect adsorption, but do not follow the expected trend. The fraction of amorphous content is identified as the key feature for phosphate adsorption on TAs. Strategic measures for producing promising alumina adsorbents are suggested. Overall, this work provides insights into the chemistry of phosphate on TAs and offers guidance for the development of alumina remediation materials.
Transition aluminas (TAs) are evolved alumina polymorphs during mineral phase transformation from amor-phous to crystalline structure, which have been extensively used as engineering adsorbents or platforms of functional materials for pollutants (e.g. eutrophication nutrient PO43-) mitigation in water remediation. A well-understanding of structure-binding activity of pollutants on transition aluminas is essential for developing promising water remediation materials. In this work, TAs were synthesized through annealing amorphous aluminum (oxy)hydroxide, and a decreased trend of phosphate (PO43-) adsorption was observed, which was not in pace with the changes of specific surface areas and site densities. The structure disorders of TAs deteriorated continuously peaked at 700 degrees C and TA at 700 degrees C has the largest extent of structural disorder, but does not present the highest adsorption capacity, which is not consistent with the consensus that oxides' structural disorder facilitate adsorption. Multiple techniques including pair distribution function, selective chemical extraction, Al-27 NMR and quantum chemistry calculations were employed to reveal the underlying mechanism differences of phosphate adsorption on TAs. The results indicated the fraction of amorphous contents is the key feature gov-erning PO(4)(3-)adsorption, regardless of mineral phase, structural disorder, AlO4/AlO6 arrangement, and Gibbs free energy of adsorption. Three strategic measures are suggested on making promising alumina engineering ad-sorbents, including tuning transition temperature, introducing non-tetrahedral and non-octahedral nano-structured grains, and employing more potential methods for synthesizing amorphous nanocrystalline composite. This work sheds lights on understanding the fundamental chemistry of phosphate on transition alumina and producing prospective alumina remediation materials.

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