数字农科院2.0

Novel insights into ferrate (VI) activation by Mn-modified sludge biochar for sulfamethoxazole degradation: Dominance of hydroxyl group and Mn-O bond in the non-radical pathway

文献类型： 外文期刊

作者： Zhikang Deng;Yongfei Ma;Jinyao Zhu;Chenyu Zeng;Rui Mu;Yifan Liu;Ping Li;Zulin Zhang

作者机构：

关键词： Biochar;DFT;Ferrate (VI);High-valent iron;SMX

期刊名称： Separation and Purification Technology

ISSN： 1383-5866

年卷期： 2024 年 349 卷

页码：

收录情况： SCIE（2024版） ; ; EI（2024版）

摘要： Ferrate (Fe (VI)), as a versatile oxidizer, has been widely employed for water treatment. However, the rapid self-decomposition of Fe (VI) diminishes its practical application efficiency. In this study, a novel Mn-modified sludge biochar (MSBC) was synthesized for the first time to activate Fe (VI) and generate highly reactive Fe (IV)/Fe (V) for the rapid removal of sulfamethoxazole (SMX). The results showed that MSBC (0.10 g/L) effectively activated Fe (VI) (100 μM), and 87.39 % of SMX (10 μM) and 40.26 % of total organic carbon (TOC) were removed within 10 min. Notably, raising the solution pH (e.g., from 6.0 to 11.0) would result in decreasing the reactivity of Fe (VI) and a lower removal efficiency of SMX. The quenching, electron paramagnetic resonance and probe experiments suggested that •O2– and high-valent iron species (Fe (V)/Fe (IV)) were identified as the major contributions to the removal of SMX. The detailed activation sites of MSBC were –OH and Mn-O, as corroborated by density functional theory (DFT) calculation and characterization. These activation sites facilitated activation of Fe (VI) through efficient electron transfer. The Fukui index indicated that the N, S, and O atom of SMX were the primary attacked sites. Subsequently, five potential degradation pathways were proposed, with the cleavage of the S-N bond being the predominant one. The toxicity of these products was examined using ECOSAR program, revealing that main products showed low toxicity or non-toxicity. The Cl-, SO42-, and NO3– had negligible effect on SMX degradation, although excessive concentrations of HCO3– and humic acid (HA) showed slightly inhibition. Additionally, the Fe (VI)/MSBC system also effectively removed 87.34 % of sulfadiazine (SDZ) and 93.91 % of sulfamethoxypyridazine (SMP). Overall, this study offered a practical and cost-effective approach for the activation of Fe (VI) and provided new insights to the degradation mechanism.

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