Facile cascade-anchored synthesis of ultrahigh metal loading single-atom for significantly improved Fenton-like catalysis
Shuaishuai Li, Wei Wang, Huizhong Wu, Xuechun Wang, Shihu Ding, Jingyang Liu, Xiuwu Zhang, Jiangli Sun, Chunhong Fu, Minghua Zhou
Abstract
It is crucial to break the low metal-loading limitation and reveal the intersite synergy-governed catalytic behavior of single-atom catalysts (SACs). Here, a universal synthesis strategy achieves record loadings of transition metals (Fe 41.31 wt%, Mn 35.13 wt%), rare-earth metals (La 28.62 wt%), and noble metals (Ag 27.04 wt%). The strong oxalic acid-metal chelation and concurrent entangled polymer networks enable high-loading SACs. High-density single atoms induce site-intensive effects, modulating electron density and valence states to achieve peroxymonosulfate-based Fenton-like reactions with rate constants 1-2 orders of magnitude higher than conventional SACs. Elevated metal loading boosts Fenton-like potential jumps, facilitates electron transfer, and reduces the rate-limiting energy barrier in 1O2 production. This material is also proven effective in real wastewater treatment, combining high decontamination efficiency with operational stability. It is anticipated that the cascade-anchoring synthesis strategy will take SACs a step closer to practical applications. Single-atom catalysts typically suffer from low metal-loading limitations. Here, authors develop a universal method for achieving record loadings via chelation-polymer networks. These high-density catalysts exhibit enhanced electron modulation and catalytic activity.