Efficient peroxydisulfate activation with γ-Al2O3-C-MIL-100(Fe) framework for sulfamethazine degradation: Enhanced oxidant utilization and reduced metal leaching

Applied Catalysis B: Environment and Energy Pub Date : 2024-08-22 DOI:10.1016/j.apcatb.2024.124520

Jianxin Zhu, Haiyang Liu, Haijun Chen, Xiuyi Hua, Deming Dong, Dapeng Liang, Zhiyong Guo, Na Zheng

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Abstract

Low degradation efficiency and significant transition metal leaching are two challenges in persulfate activation systems based on metal-organic frameworks (MOFs) for organic pollutant degradation. Here, the challenges were solved by designing and synthesizing a micron-sized core-shell material, γ-AlO-C-MIL-100(Fe) (γACM), by coating the γ-AlO core with carbon (γ-AlO-C) and futher modifying with MIL-100(Fe). Testing γACM with sulfamethazine (SMZ) demonstrated its outstanding peroxydisulfate (PDS) activation, achieving 92.5 % SMZ removal within 20 min at a low oxidant/pollutant ratio. Fe leaching from γACM was effectively inhibited, with only 3.59 % Fe lost after three recycles. The system showed adaptability across a wide pH range, and usability in sewage effluent, indicating promise for practical application. The hydrophobicity of γ-AlO-C, the coordinatively unsaturated sites in MIL-100(Fe), and the strong bounding of MIL-100(Fe) on γ-AlO-C ensured the effective SMZ gather, PDS activation, and Fe stability respectively, which led to the excellent performances of γACM.

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利用γ-Al2O3-C-MIL-100(Fe)框架高效活化过硫酸氢盐以降解磺胺二甲嘧啶：提高氧化剂利用率并减少金属沥滤

降解效率低和过渡金属浸出严重是基于金属有机框架（MOFs）的过硫酸盐活化系统降解有机污染物的两大难题。本文通过在γ-AlO核上涂覆碳（γ-AlO-C）并进一步用MIL-100(Fe)改性，设计合成了微米级核壳材料γ-AlO-C-MIL-100(Fe)（γACM），从而解决了这一难题。用磺胺甲基嘧啶（SMZ）对γACM 进行的测试表明，它具有出色的过氧化二硫酸盐（PDS）活化能力，在氧化剂/污染物比率较低的情况下，20 分钟内对 SMZ 的去除率达到 92.5%。γACM中的铁沥滤作用被有效抑制，三次循环后仅损失了3.59%的铁。该系统在很宽的 pH 值范围内都有很好的适应性，并可用于污水处理，这表明该系统有望得到实际应用。γ-AlO-C的疏水性、MIL-100（Fe）中的配位不饱和位点以及MIL-100（Fe）在γ-AlO-C上的强结合分别确保了SMZ的有效聚集、PDS的活化和Fe的稳定性，从而使γACM具有优异的性能。

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Applied Catalysis B: Environment and Energy

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