Activation of persulfate by MOF-derived MnFeOx to efficiently degrade sulfadiazine: Synergistic effects from free radicals and singlet oxygen

IF 2.7 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Inorganica Chimica Acta Pub Date : 2024-10-19 DOI:10.1016/j.ica.2024.122407

Ruifu Han, Wenhao Zhao, Jiawei Wei, Chenglong Ge, Denghui Zhang, Wenqiang Jiang

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Abstract

In this study, a facile hydrothermal approach was used to synthesize the MOFs materials [Mn-doped MIL-101(Fe)]. These materials were subsequently subjected to high temperature annealing process via calcination to generate the MOFs derivatives (MnFeO_x). The synthesized materials were utilized for the removal of sulfadiazine (SDZ) removal through activated peroxymonosulfate (PMS). At the optimum Mn doping, the removal ratio of SDZ could reach 98.9 % (at natural pH) within 20 min. In addition, the study investigated the influence of PMS dosage, catalyst dosage, initial pH, various inorganic anions, and humic acid (HA) on the degradation of SDZ. The activation processes of both free and non-free radicals in the MnFeO_x/PMS system were examined by free radical quenching experiments and electron paramagnetic resonance (EPR) techniques. The analysis of the degradation products of SDZ was conducted by using high performance liquid chromatography-mass spectrometry (HPLC-MS), and the breakdown pathways of SDZ in the MnFeO_x/PMS system were proposed.

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由 MOF 衍生的氧化锰铁氧体活化过硫酸盐，从而高效降解磺胺嘧啶：自由基和单线态氧的协同效应

本研究采用简便的水热法合成了 MOFs 材料 [掺锰 MIL-101(Fe)]。这些材料随后通过煅烧进行高温退火处理，生成 MOFs 衍生物（MnFeOx）。合成的材料被用于通过活化过一硫酸盐（PMS）去除磺胺嘧啶（SDZ）。在最佳锰掺杂条件下，20 分钟内对 SDZ 的去除率可达 98.9%（自然 pH 值）。此外，该研究还考察了 PMS 用量、催化剂用量、初始 pH 值、各种无机阴离子和腐植酸（HA）对 SDZ 降解的影响。通过自由基淬灭实验和电子顺磁共振（EPR）技术考察了 MnFeOx/PMS 体系中自由基和非自由基的活化过程。利用高效液相色谱-质谱联用技术分析了 SDZ 的降解产物，并提出了 SDZ 在 MnFeOx/PMS 体系中的分解途径。

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来源期刊

Inorganica Chimica Acta 化学-无机化学与核化学

CiteScore

6.00

自引率

3.60%

发文量

440

审稿时长

35 days

期刊介绍： Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews. Topics covered include: • chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies; • synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs); • reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models; • applications of inorganic compounds, metallodrugs and molecule-based materials. Papers composed primarily of structural reports will typically not be considered for publication.