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氮掺杂碳基质中零价铁/碳化铁纳米粒子同时吸附和氧化降解双酚 A。

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

机构信息

College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China.

College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China.

出版信息

Environ Pollut. 2018 Dec;243(Pt A):218-227. doi: 10.1016/j.envpol.2018.08.061. Epub 2018 Aug 26.

Abstract

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/FeC@C) with graphitized shell and highly dispersed active kernel via the pyrolysis process under N atmosphere. Batch adsorption experimental results showed that N-doped Fe/FeC@C had high adsorption capacity for BPA (∼138 mg g at pH = 7 and 298 K). Degradation of BPA adsorbed on N-doped Fe/FeC@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/FeC@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) was almost completely degraded within 60 min in the presence of N-doped Fe/FeC@C (∼0.2 g L). When the BPA content increased to 25 mg L, 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 π-π interactions between the π 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/FeC@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.

摘要

双酚 A(BPA)在受污染废水中的释放和积累增加,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。本研究从金属有机骨架出发,提出了一种在氮气气氛下通过热解过程合成具有石墨化壳和高度分散活性核的磁性多孔微球(N 掺杂的 Fe/FeC@C)的简单方法。批量吸附实验结果表明,N 掺杂的 Fe/FeC@C 对 BPA 具有高吸附能力(在 pH=7 和 298 K 时约为 138mg/g)。进一步研究了 BPA 在 N 掺杂的 Fe/FeC@C 上的吸附降解作为 BPA 浓度、过硫酸盐量、温度和溶液 pH 的函数。结果表明,过一硫酸盐可以被 N 掺杂的 Fe/FeC@C 激活,生成大量自由基,这对 BPA 的降解至关重要。在单独的过硫酸盐体系中,BPA 的浓度几乎没有变化。当存在 N 掺杂的 Fe/FeC@C(约 0.2g/L)时,BPA(10mg/L)在 60min 内几乎完全降解。当 BPA 含量增加到 25mg/L 时,BPA 的去除效率在 150min 内达到 98.4%。从 XRD、拉曼和 XPS 分析可知,BPA 的主要吸附机制是π轨道在碳基面和 BPA 芳香环中的电子密度之间的π-π相互作用。而优越的降解归因于酚类氧化过程中自由基的产生和演变。这项工作不仅证明了 N 掺杂的 Fe/FeC@C 在 BPA 的吸附和降解中的潜在应用,而且为使用这种磁性材料在有机污染物清理中消除有机污染物开辟了新的可能性。

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