Efficient adsorption of phosphate on magnetic Fe3O4@MOF@LDH superstructures: Kinetics, thermodynamics, and mechanisms

Phosphorus contamination in water systems poses a significant environmental threat, necessitating the need for effective phosphate removal methods. A novel magnetic composite, magnetic Fe3O4@MIL-100(Fe)@Mg-Al layered double hydroxide (LDH), synthesized through a solid-state transformation of MIL-100...

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Detalles Bibliográficos
Autores: Liu, Zhang, Han, Wei, Marquina, Clara, Kwan, Joseph Kai Cho, Ibarra, M. Ricardo, Yeung, King Lun
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2025
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/399226
Acceso en línea:http://hdl.handle.net/10261/399226
Access Level:acceso embargado
Palabra clave:Magnetic core/shell structure
Fe3O4@MOF@LDH
Phosphate adsorption
Adsorption kinetics
Thermodynamic parameters
Adsorption configuration
Descripción
Sumario:Phosphorus contamination in water systems poses a significant environmental threat, necessitating the need for effective phosphate removal methods. A novel magnetic composite, magnetic Fe3O4@MIL-100(Fe)@Mg-Al layered double hydroxide (LDH), synthesized through a solid-state transformation of MIL-100(Fe) from Fe3O4 followed by in-situ growth of Mg-Al LDH. This innovative hierarchical core/shell/shell structure leverages the magnetic properties of Fe3O4 for easy separation, utilizes MIL-100(Fe) to grow and orient the LDH, and exploits the large ion exchange capacity of Mg-Al LDH nanosheets for efficient phosphate capture. Our experiments demonstrated rapid phosphate removal exceeding 95 % within 10 min, achieving a final concentration of 25.5 μg/L from an initial concentration of 1 mg/L. The adsorption kinetics conformed to a pseudo-second order model, and isothermal data fit the Langmuir model. Thermodynamic analysis indicated spontaneous and exothermic adsorption, with an activation energy of 15.76 kJ mol−1. Enthalpy and entropy findings suggest a decrease in randomness during the adsorption process. Density Functional Theory (DFT) calculations revealed that phosphate ions interact strongly with Al sites in the LDH and Fe-O nodes in MIL-100(Fe). Phosphate recovery and sorbent regeneration are accomplished through a simple alkaline wash, which concentrates the recovered phosphate by 4.8 times. This study highlights the potential of Fe3O4@MIL-100(Fe)@Mg-Al LDH as a sustainable and efficient adsorbent for phosphate pollution mitigation, offering significant contributions to environmental protection and resource conservation.