Modified geopolymers as promising catalyst supports for abatement of dichloromethane

Abstract

Geopolymers have not been extensively employed as catalytic materials despite of their zeolite-resembling Si–Al structure. Geopolymerization offers a novel way for preparation of catalysts and possibility to use waste or industrial side-stream derived raw material as a resource for catalyst manufacturing. This work concentrates on metakaolin-based geopolymer materials that were prepared, characterized and tested as alternative environmentally benign catalyst supports for the oxidation of dichloromethane. The geopolymers with the Si/Al ratio of 1.5 were modified with HCl to increase their specific surface area, which is important in catalytic applications. Significant increase in specific surface areas was achieved via leaching of Na and Al from the geopolymer structure. Highest specific surface areas achieved for calcined geopolymers were over 500 m2g-1. Use of acid concentrations higher than 1 M led to the dehydroxylation of the geopolymer. Dehydroxylation decreased the total acidity of geopolymer through the loss of the Brønsted acid sites, which are responsible for the adsorption of dichloromethane in the beginning of the catalytic reaction. Absence of Brønsted acid sites was observed by the formation of CH2O as the only reaction intermediate. The best result in the dichloromethane oxidation was found with the geopolymer treated with 1 M HCl. Without using any additional active sites, the maximum dichloromethane conversion of 90% was reached at 525 °C with the maximum HCl yield of 83%. This result indicates the good potential of modified geopolymers to be used as catalyst supports in environmental applications.