Recently, a research team led by Prof. Li Wenwei from Suzhou Institute for Advanced Research (SIAR), the University of Science and Technology of China (USTC) made progress in advanced oxidation decontamination technologies, revealing the structure-activity correlations of crystal structure and Fenton-like catalytic selectivity of metal oxide nanomaterials and designing a new type of heterogeneous catalysts for efficient and selective water decontamination. The study was published in Proceedings of National Academy of Sciences of the United States of America with a title of Electron Delocalization Triggers Nonradical Fenton-like Catalysis over Spinel Oxides.

Heterogeneous Fenton-like advanced oxidation processes based on inexpensive transition metal oxides has great potential to control water pollution. However, due to the interference of various complex components in wastewater, the existing technology is not satisfactory in removing degradation-resistant organic micropollutants. As a result, it is urgent to develop transition metal-based catalysts with high activity and selectivity.

Dr. Guo Zhiyan utilized the synergistic catalytic effect of Fe-Mn in the spinel oxide ZnFeMnO4. By fine-tuning the coordination environment at the active Mn site, Guo investigated the structure–activity correlations between catalytic activity and selectivity of the electronic structure of material surface and activated peroxymonosulfate (PMS) in degrading pollutants and found that Fe-Mn superexchange interaction at the spinel octahedra can help create the Mn-O unit with high-degree electron delocalization and thus PMS binding and activation and selective oxidation of pollutants are enhanced. Based on this, the ZnFeMnO4 catalyst with high activity and near 100% nonradical catalytic selectivity was created, which exhibits excellent pollutant degradation, superior resistance to environmental interferences as well as unprecedented PMS utilization efficiency in complex wastewater treatment.

The work opens up a new way for modulating the catalytic selectivity of Fenton-like catalysis of metallic oxides and is of great significance to further promote the development and application of advanced oxidation water treatment technology.

Paper Link: https://www.pnas.org/doi/full/10.1073/pnas.2201607119