Properties and computational insights of catalysts based on amide linked polymer for photo-Fenton remediation of Rhodamine B dye

基于酰胺连接聚合物的光芬顿法修复罗丹明B染料催化剂的性质和计算研究

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Abstract

In this elucidation, the use of advanced oxidation processes (AOPs) is anticipated as a promising green technology for deducting water contamination. Here, we announce the use of an amide polymer accumulated with bimetallic oxide, CuFe(2)O(4), based on a cellulose moiety as photo-Fenton catalysts. Firstly, the condensation of terephthaloyl dichloride with aminoacetophenone utilized to afford the corresponding N(1),N(4)-bis(4-acetyl phenyl)terephthalamide (BAT), which easily reacts with carboxymethyl cellulose, resulting in the cleavage of H(2)O and chelation on the cellulose surface, forming the novel N(1),N(4)-bis(4-acetyl phenyl) terephthalamide/carboxymethyl cellulose (BAT/CMC). It adsorbs bimetallic oxide, CuFe(2)O(4) through physical interaction to form N1,N4-bis(4-acetylphenyl) terephthalamide/carboxymethyl cellulose/CuFe(2)O(4) (BAT/CMC/CuFe(2)O(4)). All synthesized compounds were confirmed through spectral analysis, including FT-IR, NMR, SEM, and XRD. In addition to nitrogen adsorption-desorption measurements of evaluated catalysts. Furthermore, the (BAT/CMC/CuFe(2)O(4)) exhibits superior reactivity for Fenton-like reactions in degrading Rhodamine B (RhB) dye under solar irradiation compared to the prepared heterogeneous catalyst, CuFe(2)O(4). Moreover, under optimal conditions, a comparative experiment between conventional and photo-Fenton catalytic degradation was conducted. After 80 min, BAT/CMC/CuFe(2)O(4) achieved a maximum removal efficiency for RhB of 39.5% at 303 K, while the photo-Fenton oxidation process completely decomposed RhB (94.2%). The first-order kinetic simulation is the most appropriate model for RhB onto all developed materials, as demonstrated by the higher values of correlation coefficients, R(2). Thermodynamic studies disclosed that the system functions through endothermic, non-spontaneous processes; also, the created samples have activation energies (Ea) greater than 20 kJ/mol, suggesting a chemical mechanism for RhB decomposition. Four successive cycles were conducted to evaluate the reusability of developed catalysts under optimal conditions, with a drop-in degradation activity. Furhermore, the Density Functional Theory (DFT) investigation of BAT/CMC/CuFe(2)O(4) with RhB dye using the B3LYP/LANL2DZ(G) basis set confirmed their hydrogen bond interaction and determined their different physical describitors.

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