Boosting electro-Fenton performance by constructing a large-scale 3D-architected amorphous–nanocrystalline structure

Abstract

Metallic glasses (MGs) catalysts have shown promise in Fenton-like reactions for environmental remediation. However, the challenge of balancing catalytic activity and recyclability has hindered their practical application. Here, we present a novel approach to fabricate a three-dimensional (3D) amorphous-nanocrystalline catalyst on Cu-foam using thermal spraying, which shows excellent catalytic activity-recyclability synergy. This method enables large-scale production of a 3D porous MG composite (referred to as 3DP MGC) without the need of post-treatment. The architected 3DP MGC exhibits exceptional electro-Fenton activity, surpassing the performance of most Fe-based catalysts reported to date, with a kinetic rate constant 1.4 times higher than that of the amorphous FeSiB MG ribbon. Furthermore, the 3DP MGC catalyst demonstrates excellent reusability, maintaining efficiency for over 60 cycles without decay. The excellent catalytic activity of the 3D-architected MGC is attributed to the galvanic coupling between the MG and α-Fe phases with a low grain boundary effect and accelerated electronic transfer kinetics, facilitating the generation of multiple reactive oxygen species. Additionally, the catalyst benefits from a sustainably active surface enriched with Fe(II) species, resulting in ultrahigh reusability. Finally, we demonstrate the exceptional environmental tolerance of the architected 3DP MGC catalyst, showcasing its high efficiency in degrading real oilfield wastewater and suggesting its potential for the 3D engineering of MG materials in catalytic applications.