Simultaneous adsorption and oxidative degradation of Bisphenol A by zero-valent iron/iron carbide nanoparticles encapsulated in N-doped carbon matrix

Simultaneous adsorption and oxidative degradation of Bisphenol A by zero-valent iron/iron carbide nanoparticles encapsulated in N-doped carbon matrix
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N掺杂碳基体中零价铁/碳化铁纳米粒子同时吸附和氧化降解双酚A

DOI:
10.1016/j.envpol.2018.08.061
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发表时间:
2018-12-01
影响因子:
8.9
通讯作者:
Wang, Xiangke
Wang, Xiangke
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Jin, Qingqing;Zhang, Sai;Wang, Xiangke

文献摘要

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受污染废水中双酚A (BPA)的释放和积累增加,因其对人类健康和水生生态系统的潜在负面影响而引起了全世界的关注。从金属有机骨架出发,提出了一种简单的方法,在N-2气氛下通过热解过程合成具有石墨化外壳和高度分散活性核的磁性多孔微立方体(n掺杂Fe-0/Fe3C@C)。批量吸附实验结果表明,n掺杂Fe-0/Fe3C@C对SPA具有较高的吸附量(pH = 7, 298 K时吸附量为138 mg g(-1))。进一步研究了n掺杂Fe-0/Fe3C@C对BPA吸附的降解作用与BPA浓度、过硫酸盐用量、温度和溶液ph的关系,发现n掺杂Fe-0/Fe3C@C可以活化过氧二硫酸钾,并产生大量自由基,这对BPA的降解至关重要。BPA的浓度在单个过硫酸盐体系中几乎没有变化。双酚a (10 mg L-1)在n掺杂双酚a (10 mg L-1)存在下60 min内几乎完全降解,在n掺杂Fe-0/Fe3C@C(类似于0.2 g L-1)存在下60 min内几乎完全降解。当BPA含量增加到25 mg L-1时,经过150 min, BPA的去除率达到98.4%。从XRD、Raman和XPS分析可知,BPA的主要吸附机理是碳基面上π轨道与BPA芳环上电子密度之间的π - π相互作用。而苯酚氧化过程中自由基的生成和演化则是降解效果较好的原因。本研究不仅证明了n掺杂Fe-0/Fe3C@C在双酚a吸附降解中的潜在应用,也为利用这种磁性材料去除有机污染物在有机污染物的清除中开辟了新的可能性。(C) 2018年Elsevier Ltd.出版
The increased release and accumulation of Bisphenol A (BPA) in contaminated wastewater has resulted in the world wide concerns because of its potential negative effects on human health and aquatic ecosystems. Starting with metal-organic frameworks, we present a simple method to synthesize magnetic porous microcubes (N-doped Fe-0/Fe3C@C) with graphitized shell and highly dispersed active kernel via the pyrolysis process under N-2 atmosphere. Batch adsorption experimental results showed that N-doped Fe-0/Fe3C@C had high adsorption capacity for SPA (similar to 138 mg g(-1) at pH = 7 and 298 K). Degradation of BPA adsorbed on N-doped Fe-0/Fe3C@C was further investigated as a function of BPA concentration, persulfate amount, temperature and solution pH. It was found that potassium peroxodisulfate could be activated by N-doped Fe-0/Fe3C@C, and a large number of free radicals were generated which was crucial for the degradation of BPA. The concentration of BPA was barely changed in the individual persulfate system. BPA (10 mg L-1) was almost completely degraded within 60 min in the presence of N-doped BPA (10 mg L-1) was almost completely degraded within 60 min in the presence of N-doped Fe-0/Fe3C@C (similar to 0.2 g L-1). When the BPA content increased to 25 mg L-1, the removal efficiency of BPA achieved to 98.4% after 150 min. From the XRD, Raman, and XPS analysis, the main adsorption mechanism of BPA was pi-pi interactions between the pi orbital on the carbon basal planes and the electronic density in the BPA aromatic rings. While the superior degradation was attributed to the radical generation and evolution in phenol oxidation. This work not only proved the potential application of N-doped Fe-0/Fe3C@C in the adsorption and degradation of BPA, but also opened the new possibilities to eliminate organic pollutants using this kind of magnetic materials in organic pollutants' cleanup. (C) 2018 Published by Elsevier Ltd.