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一步合成铁碳核壳纳米颗粒以活化过硫酸盐用于有效降解四溴双酚A:性能与活化机制

One-Step Synthesized Iron-Carbon Core-Shell Nanoparticles to Activate Persulfate for Effective Degradation of Tetrabromobisphenol A: Performance and Activation Mechanism.

作者信息

Yu Yunjiang, Liu Chang, Yang Chenyu, Yu Yang, Lu Lun, Ma Ruixue, Li Liangzhong

机构信息

State Environmental Protection Key Laboratory of Environmental Pollution Health Risk Assessment, Center for Environmental Health Research, South China Institute of Environmental Sciences, Ministry of Ecology and Environment, Guangzhou 510655, China.

Inner Mongolia Autonomous Region Key Laboratory of Water Pollution Control, School of Ecology and Environment, Inner Mongolia University, Hohhot 010021, China.

出版信息

Nanomaterials (Basel). 2022 Dec 18;12(24):4483. doi: 10.3390/nano12244483.

DOI:10.3390/nano12244483
PMID:36558336
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9787185/
Abstract

Tetrabromobisphenol A (TBBPA), as an emerging endocrine disrupter, has been considered one of the persistent organic contaminants in water. It is urgently necessary to develop an efficient technique for the effective removal of TBBPA from water. Herein, a one-step hydrothermal synthesis route was employed to prepare a novel iron-carbon core-shell nanoparticle (Fe@MC) for effectively activating persulfate (PS) to degrade TBBPA. Morphological and structural characterization indicated that the prepared Fe@MC had a typical core-shell structure composed of a 5 nm thick graphene-like carbon shell and a multi-valence iron core. It can be seen that 94.9% of TBBPA (10 mg/L) could be degraded within 30 min at pH = 7. This excellent catalytic activity was attributed to the synergistic effect of the porous carbon shell and a multi-valence iron core. The porous carbon shell could effectively prevent the leaching of metal ions and facilitate PS activation due to its electron transfer capability. Furthermore, numerous micro-reaction zones could be formed on the surface of Fe@MC during the rapid TBBPA removal process. Radical quenching experiments and electron paramagnetic resonance (EPR) technology indicated that reactive oxygen species (ROS), including OH, SO, O and O, were involved in the TBBPA degradation process. Based on density functional theory (DFT) calculation, the carbon atoms linked by phenolic hydroxyl groups would be more vulnerable to attack by electron-rich groups; the central carbon was cracked and hydroxylated to generate short-chain aliphatic acids. The toxicity evaluation provides clear evidence for the promising application potential of our prepared material for the efficient removal of TBBPA from water.

摘要

四溴双酚A(TBBPA)作为一种新兴的内分泌干扰物,已被视为水中的持久性有机污染物之一。迫切需要开发一种有效的技术来从水中有效去除TBBPA。在此,采用一步水热合成路线制备了一种新型的铁 - 碳核壳纳米颗粒(Fe@MC),用于有效活化过硫酸盐(PS)以降解TBBPA。形态学和结构表征表明,所制备的Fe@MC具有典型的核壳结构,由5nm厚的类石墨烯碳壳和多价铁核组成。可以看出,在pH = 7时,94.9%的TBBPA(10mg/L)可在30分钟内降解。这种优异的催化活性归因于多孔碳壳和多价铁核的协同作用。多孔碳壳由于其电子转移能力,可以有效防止金属离子的浸出并促进PS活化。此外,在快速去除TBBPA的过程中,Fe@MC表面可形成大量微反应区。自由基猝灭实验和电子顺磁共振(EPR)技术表明,包括·OH、SO、O和O在内的活性氧物种(ROS)参与了TBBPA的降解过程。基于密度泛函理论(DFT)计算,与酚羟基相连的碳原子更容易受到富电子基团的攻击;中心碳发生裂解并羟基化生成短链脂肪酸。毒性评估为我们制备的材料在从水中高效去除TBBPA方面具有广阔的应用潜力提供了明确的证据。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/afd145526695/nanomaterials-12-04483-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/37cf1051f7a1/nanomaterials-12-04483-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/87aa295e2916/nanomaterials-12-04483-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/e06a2bf2abfc/nanomaterials-12-04483-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/5ec92675406d/nanomaterials-12-04483-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/a043be91102f/nanomaterials-12-04483-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/ac0fa9d8877e/nanomaterials-12-04483-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/7deb0ee155b9/nanomaterials-12-04483-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/2da19c2759bb/nanomaterials-12-04483-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/afd145526695/nanomaterials-12-04483-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/37cf1051f7a1/nanomaterials-12-04483-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/87aa295e2916/nanomaterials-12-04483-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/e06a2bf2abfc/nanomaterials-12-04483-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/5ec92675406d/nanomaterials-12-04483-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/a043be91102f/nanomaterials-12-04483-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/ac0fa9d8877e/nanomaterials-12-04483-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/7deb0ee155b9/nanomaterials-12-04483-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/2da19c2759bb/nanomaterials-12-04483-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/531a/9787185/afd145526695/nanomaterials-12-04483-g009.jpg

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