铁-N-S共掺杂银耳样碳催化剂对过氧单硫酸盐降解双酚A的活化作用:吡啶N、铁- nx、噻吩S的协同作用

IF 6.9 Q1 Environmental Science Journal of environmental sciences Pub Date : 2023-07-01 DOI:10.1016/j.jes.2022.09.037
Wenjin Chen , Lele Lei , Ke Zhu , Dongdong He , Hongmei He , Xiulan Li , Yumeng Wang , Jin Huang , Yushi Ai
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引用次数: 3

摘要

双酚A(BPA)由于其长期的工业应用和对环境污染的持久性而受到越来越多的关注。铁基碳催化剂活化过一硫酸盐(PMS)在有效消除水中难降解污染物方面显示出良好的前景。在此,考虑到铁离子的浸出和杂原子掺杂的优化问题,铁、氮、硫共掺杂银耳类碳催化剂(Fe-NS@C)采用极少量的铁、S-C3N4和低成本的壳聚糖(CS)通过浸渍煅烧法合理设计。按准备Fe-NS@C通过在15分钟内以高动力学常数(1.492 min-1)活化PMS,表现出优异的完全去除BPA(20 mg/L)的性能。此外Fe-NS@C/PMS系统不仅具有广泛的pH适应性和对环境干扰的高抵抗力,而且对不同污染物都保持着良好的降解效率。令人印象深刻的是,增加的S-C3N4掺杂量调节了Fe-NS@C,以及Fe-NS@C-1-x随着S-C3N4含量的增加明显增强,证实吡啶N和Fe-Nx是系统中的主要活性位点。同时,噻吩硫(C-S-C)作为活性位点起到了辅助作用。此外,猝灭实验、EPR分析和电化学测试证明,表面结合自由基(·OH和SO4·−)和非自由基途径在BPA降解中起作用(前者起主导作用)。最后,提出了可能的BPA降解途径。该工作为合成新型Fe、N和S共掺杂碳催化剂提供了一条有前途的途径,该催化剂用于降解低金属浸出率和高催化能力的有机污染物。
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Peroxymonosulfate activation by Fe-N-S co-doped tremella-like carbocatalyst for degradation of bisphenol A: Synergistic effect of pyridine N, Fe-Nx, thiophene S

Bisphenol A (BPA) has received increasing attention due to its long-term industrial application and persistence in environmental pollution. Iron-based carbon catalyst activation of peroxymonosulfate (PMS) shows a good prospect for effective elimination of recalcitrant contaminants in water. Herein, considering the problem about the leaching of iron ions and the optimization of heteroatoms doping, the iron, nitrogen and sulfur co-doped tremella-like carbon catalyst (Fe-NS@C) was rationally designed using very little iron, S-C3N4 and low-cost chitosan (CS) via the impregnation-calcination method. The as-prepared Fe-NS@C exhibited excellent performance for complete removal of BPA (20 mg/L) by activating PMS with the high kinetic constant (1.492 min−1) in 15 min. Besides, the Fe-NS@C/PMS system not only possessed wide pH adaptation and high resistance to environmental interference, but also maintained an excellent degradation efficiency on different pollutants. Impressively, increased S-C3N4 doping amount modulated the contents of different N species in Fe-NS@C, and the catalytic activity of Fe-NS@C-1-x was visibly enhanced with increasing S-C3N4 contents, verifying pyridine N and Fe-Nx as main active sites in the system. Meanwhile, thiophene sulfur (C-S-C) as active sites played an auxiliary role. Furthermore, quenching experiment, EPR analysis and electrochemical test proved that surface-bound radicals (·OH and SO4⋅−) and non-radical pathways worked in the BPA degradation (the former played a dominant role). Finally, possible BPA degradation route were proposed. This work provided a promising way to synthesize the novel Fe, N and S co-doping carbon catalyst for degrading organic pollutants with low metal leaching and high catalytic ability.

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来源期刊
Journal of environmental sciences
Journal of environmental sciences Environmental Science (General)
CiteScore
12.80
自引率
0.00%
发文量
0
审稿时长
17 days
期刊介绍: Journal of Environmental Sciences is an international peer-reviewed journal established in 1989. It is sponsored by the Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, and it is jointly published by Elsevier and Science Press. It aims to foster interdisciplinary communication and promote understanding of significant environmental issues. The journal seeks to publish significant and novel research on the fate and behaviour of emerging contaminants, human impact on the environment, human exposure to environmental contaminants and their health effects, and environmental remediation and management. Original research articles, critical reviews, highlights, and perspectives of high quality are published both in print and online.
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