Metal-organic frames (MOFs) have been recognized as one of the best candidates in the remediation of aqueous contaminants, while the fragile powder shape restricts the practical implementation. In this work, a shapeable, rebuildable, and multifunctional MOF composite (MIL-53@CF) was prepared from MIL-53 (Fe) and cellulose fiber (CF) using a simple ultrasonic method for adsorption and photocatalytic degradation of organic pollutants in wastewater. The results showed MIL-53(Fe) crystals were uniformly growth on CF surfaces and bonded with surface nanofibrils of CF through physical crosslinking and hydrogen bonding. Because of the high bonding strength, the MIL-53@CF composite exhibited an excellent compressive strength (3.53 MPa). More importantly, the MIL-53@CF composite was rebuildable through mechanical destruction followed by re-ultrasonication, suggesting the excellent reusability of MIL-53@CF for water remediation. The MIL-53@CF composite also had high adsorption capacities for methyl orange (884.6 mg·g−1), methylene blue (198.3 mg·g−1), and tetracycline (106.4 mg·g−1). MIL-53@CF composite could degrade TC through photocatalysis. The photocatalytic degradation mechanism was attributed to the Fe(II)/Fe(III) transform cycle reaction of MIL-53 crystal located on MIL-53@CF. Furthermore, the mechanical property and remoldability of MIL-53@CF composite increased its practicability. Comprehensively, MIL-53@CF composite provided a possible strategy to practically apply MOF in the remediation of aqueous contaminants.
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