2024年11月20日，Elsevier 旗下top期刊《Journal of Hazardous Materials》在线发表了云南师范大学化学与化工学院胡蓉教授课题组最新研究成果《Electronic structure engineering of Fe/Co dual-atom catalysts enhances ultrafast Fenton-like reactions mediated by high-valent iron-oxygen-cobalt bridged complexes for safe pollutant removal》。云南师范大学化学化工学院胡蓉教授为通讯作者。

https://www.sciencedirect.com/science/article/pii/S0304389425034752

High-valent metal-oxo (HVMO) species promote advanced oxidation processes (AOPs) for effective pollutant removal, owing to their high redox potential, extended half-life, and selectivity. However, stabilizing HVMO species and elucidating their formation mechanisms remains a considerable challenge. In this study, we developed an S-doped Fe/Co dual-atom catalyst (Fe1Co1S2-NC), which demonstrated exceptional Fenton-like catalytic activity, enabling the selective removal of various pollutants within 25 min. The corrected pseudo-first-order kinetic constant (kvalue) for pollutant removal was 183.8 min−1 M−1, substantially surpassing the most previously reported single-atom/PMS systems. Probe experiments and isotope-labeling studies indicated the HVMO species (FeⅣ=O=CoⅣ) was the main active species driving pollutant degradation (contributing 94.42 %), rather than •OH, SO4•-, or 1O2. Density functional theory (DFT) calculations indicated that S doping optimized the electronic structure of the active site, thereby increasing its affinity for PMS and the adsorption strength of intermediates. The oxygen atom was stabilized in a distinct bridging configuration between Fe and Co, which improved the stability of FeⅣ=O=CoⅣ and lowered its formation energy barrier. This heteroatom-doped electronic structure engineering facilitated electron transfer from metallic active sites to oxygen atoms, enhancing the oxidation capacity of FeⅣ=O=CoⅣ. Furthermore, mass spectrometry and toxicity analysis further revealed that the Fe1Co1S2-NC/PMS system degraded sulfamethoxazole (SMX) into less toxic oxidation products via multiple pathways. This work provides novel insights into the efficient activation of PMS and the generation mechanism of HVMO species, offering crucial guidance for the rational design of highly efficient atom-scale Fenton-like catalysts.

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