Solid catalytic materials, especially iron-based materials, have attracted tremendous attention in the oxidative removal of pollutants using H2O2 as oxidant due to their high stability, low-cost and non-toxic nature. Among all iron-based materials, FeOCl exhibits excellent H2O2 activation ability, whose hydroxyl radical generationrate is 1-3 orders of magnitude higher than traditional iron-based materials. The coordination structure of iron sites on the surface FeOCl directly affected the generation of hydroxyl radical from H2O2. Thus, the controllable synthesis of FeOCl with more reactive crystal planes is important for enhancing its heterogeneous Fenton activity. We prepared FeOCl with abundant exposed crystal planes by using small sized Hematite nanoparticles as precursor, showing the higher activity than traditional FeOCl, in which the size of Hematite was controlled by high energy ball milling method. The growth of inert (010) plane on the as-prepared FeOCl is suppressed compared to the plate-like structure of traditional FeOCl, and the ratio of exposed (100) and (110) planes with rich iron sites increased, leading to the significant improvement of its Fenton activity. In addition, based on the typical layered structure of FeOCl, we further modulated the coordination environment of iron sites by the surface modification (etching) and structural modification (intercalation). These modifications can create new reaction space on the FeOCl surface (or interlayer surface) for the conversion of pollutants. More importantly, phenolic compounds are no longer degraded into small molecular products in the treated FeOCl system, but are coupled to polycyclic polymers, which is very similar to the oxidative coupling process catalysed by peroxidases. This may indicate that the H2O2 activation pathway is changed from the homolytic cleavage of O-O bond to the heterolytic cleavage of H-OOH bond. The transformation of H2O2 activation behaviour has provided an excellent example to understand the reactivity of H2O2 on the surface of solid iron-based materials, which is of great significance for the design and development of highly efficient iron-based solid catalysts.

Promising FeOCl material for wastewater treatment: Controllable synthesis, modification and the investigation of H2O2 activation behavior

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.