Fe-chitosan complexes for oxidative degradation of emerging contaminants in water: Structure, activity, and reaction mechanism

JOURNAL OF HAZARDOUS MATERIALS

卷:408

Article

Farinelli, Giulio¹  Di Luca, Andrea²  Kaila, Ville R., I²  MacLachlan, Mark J.³  Tiraferri, Alberto¹ 

[1] Politecn Torino, Dept Environm Land & Infrastruct Engn DIATI, Corso Duca Abruzzi 24, I-10129 Turin, Italy

[2] Stockholm Univ, Dept Biochem & Biophys, Svante Arrhenius Vag 16C, S-10691 Stockholm, Sweden

[3] Univ British Columbia, Dept Chem, 2036 Main Mall, Vancouver, BC V6T 1Z1, Canada

关键词: Chitosan;    Contaminants of emerging concern;    Water treatment;    Ferryl;    Catalysis;   

DOI  :  10.1016/j.jhazmat.2020.124662

来源: Elsevier

【 摘 要 】

Versatile and ecofriendly methods to perform oxidations at near-neutral pH are of crucial importance for processes aimed at purifying water. Chitosan, a deacetylated form of chitin, is a promising starting material owing to its biocompatibility and ability to form stable films and complexes with metals. Here, we report a novel chitosanbased organometallic complex that was tested both as homogeneous and heterogeneous catalyst in the degradation of contaminants of emerging concern in water. The stoichiometry of the complex was experimentally verified with different metals, namely, Cu(II), Fe(III), Fe(II), Co(II), Pd(II), and Mn(II), and we identified the chitosan-Fe(III) complex as the most efficient catalyst. This complex effectively degraded phenol, triclosan, and 3-chlorophenol in the presence of hydrogen peroxide. A putative ferryl-mediated reaction mechanism is proposed based on experimental data, density functional theory calculations, and kinetic modeling. Finally, a film of the chitosan-Fe(III) complex was synthesized and proven a promising supported heterogeneous catalyst for water purification.

【 授权许可】

Free