Development of MCM-41 based catalysts for the photo-fenton's degradation of dye pollutants

The continuous advancement in most industries has resulted in serious water pollution problems. The industrial effluents contain a variety of highly toxic organics such as dye pollutants. Numerous processes have been demonstrated for treating such pollutants. Among them, photo-Fenton's reaction is effective for organic mineralization by hydroxyl radicals generated from the Fenton's reagents (Fe2+ and H2O2). However, there is a drawback that it requires a separation system to recover the homogeneous ferrous ion in the treated wastewater. In this research, new heterogeneous Fenton's catalysts are developed to solve such a problem and to achieve an efficient mineralization of dye pollutants. Two methods for catalyst preparation, including sol-gel hydrothermal (SG) and metal-organic chemical vapor deposition (MOCVD) techniques, were studied in this work. For SG-prepared catalysts, the iron element was successfully doped into the MCM-41 structure. These catalysts demonstrated a good catalytic efficiency but leaching of metal ions from the developed catalyst was found. In the MOCVD technique, a rotated tubular reactor system was developed to synthesize Fe/MCM-41 catalyst with uniform metal dispersion. It was found that using oxygen as a carrier gas during metal deposition was able to increase the stability of the deposited metal. In degradation of a model dye pollutant, Orange II, a total of 85% TOC mineralization was achieved at pH 3. A disadvantage of using Fe/MCM-41 was the reduced efficiency at higher pH. Cu/MCM-41 was thus developed and showed better catalytic activities than Fe/MCM-41 at neutral pH. Having the specific catalytic properties of Fe/MCM-41 and Cu/MCM-41, bimetallic (Fe+Cu) catalysts supported on MCM-41 were developed which show better activities in the Orange II mineralization than those monometallic (Fe or Cu) catalysts. The preparation conditions of the catalysts were experimentally optimized. The effects of catalyst dosage, metal loading, hydrogen peroxide concentration, initial solution pH, Orange II concentration, and UV source on the photo-Fenton degradation of Orange II were extensively studied. The reaction kinetics study indicated a lower activation energy for the bimetallic catalyst. The methodology described here provides a sound foundation to develop a simple yet economical wastewater treatment process