Gingerbread ingredient-derived carbons-assembled CNT foam for the efficient peroxymonosulfate-mediated degradation of emerging pharmaceutical contaminants
Gingerbread ingredient-derived carbons-assembled CNT foam for the efficient peroxymonosulfate-mediated degradation of emerging pharmaceutical contaminants
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DOI：
10.1016/j.apcatb.2018.11.064
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发表时间：
2019-05
期刊：
影响因子：
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通讯作者：
T. D. Minh;M. C. Ncibi;V. Srivastava;S. Thangaraj;J. Jänis;M. Sillanpää
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文献类型：
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作者：
T. D. Minh;M. C. Ncibi;V. Srivastava;S. Thangaraj;J. Jänis;M. Sillanpää
这篇文章报道了自支撑的3D CNT泡沫的宏观化，该泡沫由通过温和热解从可再生烘焙成分获得的富含杂原子的多孔壳互连。合成的杂化物能够将过一硫酸盐（PMS）分解为活性氧化剂（硫酸根、羟基自由基和单线态氧），用于降解阿替洛尔、碘帕醇、二甲双胍、甲氧苄啶和苯酚。分级结构的氮和氧掺杂显着增强吸附和催化性能，而磁性的3D框架，促进质量传输，多组分使用和诱导协同效应，通过Me-Nx-C接口。在低催化剂和PMS投加量下，样品对模型污染物的降解去除效率很高。催化剂负载量，PMS剂量，接触时间和温度的积极影响的去除效力，而pH值和水基质支配的速率不同。自旋捕获，氧化剂淬灭和溶剂同位素效应的研究，再加上液相色谱和傅立叶变换离子回旋共振质谱分析表明，通过双模式（自由基和非自由基）激活PMS的转化产物的足迹。这种耐用的磁性碳泡沫可能是氧化减少受污染沃茨水中药物微污染物的有前途的催化剂。
This article reports on the macronization of self-supported 3D CNT foam inter-connected by heteroatom-enriched porous shells derived from renewable baking ingredients via mild pyrolysis. The synthesized hybrids enabled disintegrating peroxymonosulfate (PMS) into reactive oxidants (sulfate radicals, hydroxyl radicals, and singlet oxygen) for the degradation of atenolol, iopamidol, metformin, trimethoprim, and phenol in water. Hierarchically structured nitrogen- and oxygen-doping significantly enhanced adsorptive and catalytic performance whereas the magnetic 3D framework promoted mass transport, multicycle use and induced synergetic effects via the Me-Nx-C interfaces. The samples were highly efficient for degradative removal of model pollutants at low catalyst and PMS dose. The catalyst loading, PMS dose, contact time, and temperature positively influenced the removal potency while pH and water matrix governed the rates differently. Spin trapping, oxidant quenching and solvent isotope effect study coupled with liquid chromatography and Fourier transform ion cyclotron resonance mass spectrometry analysis suggested the footprints of transformation products via a dual-mode (radical and non-radical) activation of PMS. This durable, magnetic carbofoam might be a promising catalyst for the oxidative abatement of pharmaceutical micropollutants from contaminated waters.