Zero-Valent Iron Inside Carbon Nanocube as an Efficient Peroxymonosulfate Activator toward Catalytic Oxidation of Organic Pollutants

IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry C Pub Date : 2025-03-24 DOI:10.1021/acs.jpcc.4c08677
Xinyue Li, Shuang Jin, Yi Wang, Zhimin Cui, Zhe Chen
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Abstract

The agglomeration tendency of nano zero-valent iron (Fe0) limits its practical applications toward catalytic oxidation of organic pollutants. Herein, an in situ encapsulation of polydopamine on the surface of Prussian blue (PB) nanocubes followed by a confined reduction treatment strategy was presented to confine the zero-valent iron nanoparticles (Fe0) inside hollow carbon nanocube (Fe0@C) as an efficient peroxymonosulfate (PMS) activator toward catalytic oxidation of toxic organic contaminants. The catalytic results showed that 100% degradation of bisphenol A (BPA) could be completed within 5 min with Fe0@C nanocube as a catalyst to activate PMS. This delicately designed Fe0@C nanocube displayed a superior kinetic rate constant compared with the pure Fe0 nanoparticles (4.2-fold). Experimental evidence revealed that the generation of multiple reactive oxygen species in the nanocubes played a vital role for the significantly enhanced catalytic efficiency for organic contaminants. Both SO4•–, •O2, and •OH dominated radical processes, and nonradical pathways involving 1O2 were accounted for PMS activation and organic contaminant degradation. The superior catalytic performance was attributed to a carbon layer with large specific surface area and highly dispersed Fe0 nanoparticles to provide abundant active sites, distinct nanocube structure to concentrate the reactant molecules within a confined space, and an excellent electron/mass transport property.

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碳纳米管内零价铁作为高效过氧单硫酸盐活化剂催化氧化有机污染物的研究
纳米零价铁(Fe0)的结块倾向限制了其在催化氧化有机污染物方面的实际应用。本文提出了一种将聚多巴胺原位包封在普鲁士蓝(PB)纳米立方体表面,然后采用限制性还原处理策略,将零价铁纳米颗粒(Fe0)限制在空心碳纳米立方体(Fe0@C)内,作为一种高效的过氧单硫酸盐(PMS)活化剂,催化氧化有毒有机污染物。结果表明,Fe0@C纳米微球作为催化剂激活PMS,可在5 min内完成对双酚A (BPA)的100%降解。与纯Fe0纳米颗粒相比,这种精心设计的Fe0@C纳米立方体显示出优越的动力学速率常数(4.2倍)。实验证据表明,纳米立方中多种活性氧的生成对显著提高有机污染物的催化效率起着至关重要的作用。SO4•-、•O2 -和•OH主导了自由基过程,而涉及1O2的非自由基途径则被认为是PMS活化和有机污染物降解的主要途径。具有较大比表面积的碳层和高度分散的Fe0纳米颗粒提供了丰富的活性位点,独特的纳米立方体结构使反应物分子集中在有限的空间内,并且具有优异的电子/质量输运性能。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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