Highly dispersed single-atom Fe and Fe3O4 clusters anchored hierarchical-pore carbon as efficient persulfate activation catalyst

文献类型： 外文期刊

第一作者： Lin, Jiawei

作者： Lin, Jiawei;Zhou, Hao;Wei, Linting;Zhao, Cheng;Dai, Xiaoxin;Wang, Qing;Zheng, Guangming;Yin, Yi;Zhang, Hongfeng;Hu, Yongyou

作者机构：

关键词： MIL-88B pyrolysis; Acid etching; Single-Atom Fe; Atomic clusters; Hierarchical-pore Carbon

期刊名称：SEPARATION AND PURIFICATION TECHNOLOGY （ 影响因子：9.0； 五年影响因子：8.5 ）

ISSN： 1383-5866

年卷期： 2025 年 358 卷

页码：

收录情况： SCI

摘要： The selective removal of Fe particles from carbonized Fe-MOFs presents an intriguing strategy for developing efficient peroxydisulfate (PDS) activators. It is commonly accepted that their outstanding performance is largely attributed to the high specific surface area/pore volume. However, our investigation into the structure-function relationship of these materials has revealed new insights. In this study, a highly dispersed single-atom Fe and Fe3O4 clusters anchored hierarchical-pore carbon (CM88-H) was obtained via post-acid treatment of carbonized MIL-88B (CM88). Various characterizations were comparatively conducted to highlight the beneficial effects of iron dissolution. The CM88-H/PDS system achieved a notable BPA degradation efficiency, with a reaction rate of 0.323 min-1, which is 3.94 times higher than that of the CM88/PDS system. DFT calculations indicate that the Fe3O4 clusters optimize the charge distribution around single-atom Fe, promoting favorable PDS adsorption and facilitating a higher oxidation state of CM88-H. As a result, BPA can be completely degraded within 10 min with 0.1 g L-1 CM88-H and 0.05 g L-1 PDS via both radical and non-radical pathways. The CM88-H/PDS/BPA system performs effectively under various conditions, with a general reduction in toxicity. Furthermore, the CM88-H/ PDS system shows broad oxidation activity towards BPA substitutes and pollutants with high ionization potential (IP). Notably, the CM88-H sponge-based fixed-bed catalytic reactor demonstrated satisfactory BPA degradation, highlighting the promising application of CM88-H in water purification. This study provides a sustainable solution for water treatment and accelerates the practical application of powdered nanocatalysts to improve water quality.

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