School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China; Sichuan Province Engineering Technology Research Center of Novel CN Polymeric Materials, Chengdu 611731, China.
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu 611731, China; Sichuan Province Engineering Technology Research Center of Novel CN Polymeric Materials, Chengdu 611731, China.
J Environ Sci (China). 2023 Jul;129:213-228. doi: 10.1016/j.jes.2022.09.037. Epub 2022 Oct 12.
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-CN 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) 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-CN 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-CN contents, verifying pyridine N and Fe-N 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 SO) 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.
双酚 A(BPA)由于其长期的工业应用和在环境污染中的持久性而受到越来越多的关注。基于铁的碳催化剂活化过一硫酸盐(PMS)对于有效消除水中难降解污染物具有良好的前景。在此,考虑到铁离子浸出的问题和杂原子掺杂的优化,使用少量铁、S-CN 和低成本壳聚糖(CS)通过浸渍-煅烧法合理设计了铁、氮和硫共掺杂银耳状碳催化剂(Fe-NS@C)。所制备的 Fe-NS@C 通过活化 PMS 表现出优异的性能,可在 15 分钟内以 1.492 min 的高动力学常数完全去除 20mg/L 的 BPA。此外,Fe-NS@C/PMS 体系不仅具有较宽的 pH 适应范围和较强的环境干扰抗性,而且对不同污染物也保持了优异的降解效率。令人印象深刻的是,增加 S-CN 掺杂量调节了 Fe-NS@C 中不同 N 物种的含量,并且随着 S-CN 含量的增加,Fe-NS@C-1-x 的催化活性明显增强,验证了吡啶 N 和 Fe-N 作为体系中的主要活性位。同时,噻吩硫(C-S-C)作为活性位发挥辅助作用。此外,猝灭实验、EPR 分析和电化学测试证明了表面结合自由基(OH 和 SO)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。这项工作为合成新型铁、氮和硫共掺杂碳催化剂提供了一种有前景的方法,用于降解有机污染物,具有低金属浸出率和高催化能力。