Amino-funkcionalizacija polimera na bazi metakrilata i njihova interakcija sa oksianjonima Cr(VI), Tc(VII), Re(VII) i Mo(VI) u vodenim sistemima

Abstract

Cilj ove doktorske disertacije je bio ispitivanje uticaja stepena umreženja imakroporoznosti na strukturne karakteristike i termička svojstva neporoznih imakroporoznih metakrilatnih homopolimera i kopolimera sintetizovanih suspenzionom(ko)polimerizacijom. Pored toga u disertaciji je ispitivana mogućnost primenekopolimera glicidilmetakrilata (GMA) i etilenglikoldimetakrilata (EGDMA) sarazličitim udelom umreživača funkcionalizovanih dietilentriaminom (skraćenoPGME-deta) za uklanjanje oksianjona teških metala i radionuklida Cr(VI), 99Tc(VII),Re(VII) i Mo(VI) iz vodenih sistema. Šaržnom metodom pri nekompetitivnim uslovimaje ispitan uticaj nekoliko ključnih faktora na kapacitet i kinetiku sorpcije u ovimsistemima: vremena kontakta, početne koncentracije metala u rastvoru, pH rastvora,temperature i parametara porozne strukture kopolimera.Polimeri su okarakterisani fizičkohemijskim metodama: mikroanalizom,skenirajućom elektronskom mikroskopijom sa energetski disperzivnomspektroskopijom x-zraka (SEM/EDS) i transmisionom elektronskom mikroskopijom(TEM), infracrvenom spektroskopijom (FTIR-ATR), živinom porozimetrijom,adsorpciono–desorpcionim izotermama N2 na 77 K i termijskom analizom (TG/DSC) samasenom spektrometrijom (MS).Rezultati dobijeni ispitivanjem sorpcije Cr(VI), 99Tc(VII), Re(VII) i Mo(VI) izvodenih rastvora na amino-funkcionalizovanim kopolimerima u laboratorijskimuslovima bili su osnova za proučavanje kinetičkih reakcionih i difuzionih modela,adsorpcionih izotermi i termodinamike sorpcije, da bi se dobio uvid u mehanizamprocesa i ocenila efikasnost ovih sorbenasa.

The goal of this doctoral dissertation was to investigate the influence ofcrosslinking extent and macroporosity on structural characteristics and thermalproperties of nonporous and macroporous methacrylate-based homopolymers andcopolymers synthesized by suspension (co)polymerization. Also, the possibleapplication of the copolymers of glycidyl methacrylate (GMA) and ethylene glycoldimethacrylate (EGDMA) with different crosslinker content functionalized withdiethylene triamine (abbreviated PGME-deta) was investigated for the removal of heavymetal and radionuclide oxyanions Cr(VI), 99Tc(VII), Re(VII) and Mo(VI) from aqueoussystems. The influence of several key characteristics on sorption capacity and kinetics:contact time, initial metal concentration in the solution, solution pH, temperature andparameters of porous structure, was investigated using batch method undernoncompetitive conditions.Polymers were characterized using physicochemical methods: microanalysis,scanning electron microscopy with energy-dispersive x-ray spectroscopy (SEM/EDS)and transmission electron microscopy (TEM), infrared spectroscopy (FTIR-ATR),mercury porosimetry, N2 adsorption‒desorption isotherms at 77 K and thermal analysis(TG/DSC) with mass spectrometry (MS).The obtained results of Cr(VI), 99Tc(VII), Re(VII) and Mo(VI) sorption fromaqueous solutions on the amino-functionalized copolymers in laboratory conditionswere the base of the analysis of the surface reaction-based and pore diffusion-basedkinetic models, adsorption isotherms and thermodynamics of sorption, in order to gaininsight into the mechanism of the process and evaluate the efficiency of these sorbents.