Carbon nanotubes as catalysts for catalytic wet peroxide oxidation of highly concentrated phenol solutions: Towards process intensification uri icon

abstract

  • Commercial multi-walled carbon nanotubes with different properties (two samples from Sigma-Aldrich,SA1 and SA2; one sample from Nanocyl, NC; and two samples from Shenzhen Nanotech, SZ and LSZ),and SA2 modified by hydrothermal treatment with concentrated sulfuric acid (SA2-H), were tested ascatalysts in wet peroxide oxidation. Phenol was selected as model compound since it represents a classof noxious compounds for human health and for the environment and, due to this, phenol is typically considered in wastewater treatment studies. The experiments were carried out under the following inten-sified conditions: phenol concentration = 4.5 g L−1, hydrogen peroxide concentration = 25 g L−1, catalystload = 2.5 g L−1, pH 3.5, T = 353 K and 24 h.The results demonstrated that phenol is poorly adsorbed in this type of carbon materials (11% as max-imum when using the NC sample). However, in the catalytic experiments, complete removal of phenol isachieved when using some of the carbon nanotubes (SA1, NC and SA2), together with a remarkable total organic carbon removal (77, 69 and 67%, respectively). These materials have the less pronounced acidiccharacter, which is often considered favorable for oxidation reactions in advanced oxidation processesand may explain the higher performance of SA1, NC and SA2 regarding the other materials. Leaching of Fespecies into the solution was also observed in all cases (that can also have some influence on the degra-dation of phenol), SA1 leading to the highest concentration of Fe species leached (26 mg L−1), followedby SA2 (2 mg L−1) and NC (1 mg L−1).Considering the lower Fe leaching levels observed for SA2 and NC, these catalysts were then testedin consecutive reusability cycles. SA2 showed a superior performance than NC, but temperature-programmed desorption as well as thermogravimetric analysis suggested that the carbon material isoxidized by hydrogen peroxide at the employed conditions and/or that carboxylic acids are adsorbed onthe catalyst surface after consecutive runs (mainly after the first use). However, only a slight decrease inthe catalyst activity was observed.

publication date

  • January 1, 2015