Copper-based Ruddlesden-Popper perovskite oxides activated hydrogen peroxide for coal pyrolysis wastewater (CPW) degradation: Performance and mechanism

Abstract

Coal pyrolysis wastewater (CPW) contained all kinds of toxic and harmful components, which would seriously threaten the natural environment and human health. However, the traditional advanced oxidation processes frequently failed to remove phenolic substances. An A₂BO₄-type perovskite (La₂CuO₄) was successfully synthesized through sol-gel process and first applied in the treatment of CPW. More than 90% of 3, 5-dimethylphenol (DMP) was removed within 200 min at neutral conditions. Moreover, La₂CuO₄ also displayed excellent catalytic activity and stability in the actual CPW treatment process. Results demonstrated that DMP was removed through the attack of ∙OH, ∙O₂^- and ¹O₂ in La₂CuO₄/H₂O₂ system. The La₂CuO₄ were more favorable for H₂O₂ activation and have a lower adsorption energy than LaFeO₃. XPS of fresh and spent La₂CuO₄ illustrated that the decomposition of hydrogen peroxide (H₂O₂) was mainly due to the redox cycle between surface copper and oxygen species. Moreover, the possible degradation pathway of DMP was deduced by identifying degradation products and analyzing density functional theory (DFT) calculations. This research provided a novel strategy for the development of perovskite-based catalytic materials on the treatment of practical CPW.

Keywords: Coal pyrolysis wastewater; Density functional theory; Heterogeneous fenton; Perovskite.