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硼改性Fe/C催化剂介导过二硫酸盐活化去除全氟辛烷磺酸的见解:硼的增强机制及全氟辛烷磺酸降解途径

Insights to PFOS elimination with peroxydisulfate activation mediated by boron modified Fe/C catalysts: Enhancing mechanism of boron and PFOS degradation pathway.

作者信息

Jiang Yanting, Yu Zhendong, Lv Yuancai, Li Xiaojuan, Lin Chunxiang, Ye Xiaoxia, Yang Guifang, Liu Yifan, Dai Leilei, Liu Minghua, Ruan Roger

机构信息

Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Safety Engineering, Fuzhou University, Fuzhou 350116, China.

Fujian Provincial Key Laboratory of Ecology-Toxicological Effects & Control for Emerging Contaminants, Putian University, Putian 351100, China.

出版信息

J Colloid Interface Sci. 2023 Dec 15;652(Pt B):1743-1755. doi: 10.1016/j.jcis.2023.08.198. Epub 2023 Sep 1.

DOI:10.1016/j.jcis.2023.08.198
PMID:37672977
Abstract

In this study, the boron-doped iron-carbon composite (Fe@B/C-2) was prepared via a simple solvothermal and secondary calcination process by using iron metal-organic frameworks (Fe-MOFs) as precursor. The obtained Fe@B/C-2 possessed abundant active sites and low iron ion leaching, and exhibited excellent performance on peroxydisulfate (PDS) activation for efficient PFOS (10 mg/L) degradation (94 %) in 60 min, with 0.2 g/L of catalyst dosage, 1.0 g/L of PDS dosage and at 5.0 of initial pH. The radical scavenging and electron paramagnetic resonance (EPR) tests demonstrated that SO· and ·OH were the primary active species during PFOS elimination. Under the attack of these species, PFOS was first transformed into PFOA, followed by a sequential defluorination process, and lastly mineralized into CO and F. Notably, DFT results revealed that Fe species, -BC/-BCO structures on the carbon matrix performed crucial roles in PDS activation. The extraordinary catalytic activity of Fe@B/C-2 was attributable to the synergistic effects of Fe nanoparticles and the B-doped on carbon matrix. The doped B not only could activate the inert carbon skeleton and provided more catalytic centers, but also could accelerate the electron transfer efficiency, leading to a boost in PDS decomposition.

摘要

在本研究中,以铁基金属有机框架(Fe-MOFs)为前驱体,通过简单的溶剂热和二次煅烧工艺制备了硼掺杂的铁碳复合材料(Fe@B/C-2)。所制备的Fe@B/C-2具有丰富的活性位点和低铁离子浸出率,在0.2 g/L的催化剂用量、1.0 g/L的过二硫酸盐(PDS)用量以及初始pH值为5.0的条件下,对10 mg/L的全氟辛烷磺酸(PFOS)进行高效降解(60分钟内降解率达94%)时,表现出优异的PDS活化性能。自由基清除和电子顺磁共振(EPR)测试表明,SO·和·OH是PFOS去除过程中的主要活性物种。在这些物种的攻击下,PFOS首先转化为全氟辛酸(PFOA),随后依次进行脱氟过程,最后矿化为CO和F。值得注意的是,密度泛函理论(DFT)结果表明,碳基体上的铁物种、-BC/-BCO结构在PDS活化中起关键作用。Fe@B/C-2的卓越催化活性归因于铁纳米颗粒和碳基体上硼掺杂的协同效应。掺杂的硼不仅可以活化惰性碳骨架并提供更多的催化中心,还可以加速电子转移效率,从而促进PDS的分解。

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