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

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作者
Farinelli, Giulio [1 ]
Di Luca, Andrea [2 ]
Kaila, Ville R.I. [2 ]
MacLachlan, Mark J. [3 ]
Tiraferri, Alberto [1 ]
机构
[1] Department of Environment, Land and Infrastructure Engineering (DIATI), Politecnico di Torino, Corso Duca degli Abruzzi 24, Turin,10129, Italy
[2] Department of Biochemistry and Biophysics, Stockholm University, Svante Arrhenius väg 16C, Stockholm,10691, Sweden
[3] Department of Chemistry, University of British Columbia, 2036 Main Mall, Vancouver,BC,V6T 1Z1, Canada
关键词
Density functional theory - Iron compounds - Biocompatibility - Catalysts - Copper compounds - Organometallics - Palladium compounds - Cobalt compounds - Manganese compounds - Chitosan;
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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 chitosan-based 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. © 2021 The Authors
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