Role of Boron in Enhancing Electron Delocalization to Improve Catalytic Activity of Fe-Based Metallic Glasses for Persulfate-Based Advanced Oxidation

Metallic glasses (MGs) with superior catalytic performance have recently been recognized as attractive candidates for wastewater treatment. However, further improving their performance will require knowledge of how to precisely regulate their electronic structures via compositional control. Here, two Fe-based MGs (Fe78Si9B13 and Fe80Si9B11) were prepared to compare how slightly altering boron content affected their electronic structure and catalytic performance. Density functional theory revealed that the Fe78Si9B13 MG with 2 atom % higher boron exhibits an attractive electron delocalization, a high persulfate adsorption energy, and a superb work function due to precise regulation of the electronic structure, leading to exceptional degradation performance for seven organic pollutants. Furthermore, it can be reused 23 times without significant deterioration of catalytic performance, amorphous structure, and surface morphology. This work provides a new paradigm for the fundamental theory explaining how electronic structure is controlled by composition, creating a solid foundation to explore novel catalysts for water treatment.