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Sulfur-doped porous carbon sheets embedded with rich iron sites for 1O2 dominated peroxymonosulfate activation
Environmental Science: Nano ( IF 7.3 ) Pub Date : 2024-04-02 , DOI: 10.1039/d3en00971h
Yadan Song 1 , Yalong Liu 1 , Yangju Li 1 , Haipeng Hu 1 , Kexin Huang 1 , Zhe Zhang 1 , Zhongxian Li 2 , Wanning Cao 3 , Kai Jiang 1 , Dapeng Wu 1
Affiliation  

The poor anti-interference ability of radical-dominated processes continues to be a hindrance to the effectiveness of purification and the practical use of peroxymonosulfate-based advanced oxidation processes (PMS-AOPs). Herein, iron, nitrogen, and sulfur co-doped porous carbon sheets (Fe–SNC) were successfully synthesized via a one-step pyrolysis process by adopting Mohr's salt and ZIF-8 sheets as precursors to efficiently activate PMS. Quenching experiments and electron paramagnetic resonance (EPR) characterization indicated that singlet oxygen (1O2) played the most important role in phenol degradation. Based on the variation in the material structure and density functional theory (DFT) calculations, the study revealed the specific mechanism of sulfur embedded in rich Fe3C, Fe4N, and Fe–Nx catalytic sites as an activator of PMS in the degradation of the pollutant of interest. In addition, S-doping sites were shown to shorten the distance between PMS and the catalyst due to electron polarization of the catalyst surface, which facilitated PMS adsorption. According to ultra-high-resolution electrospray time-of-flight mass spectrometry and the predictions of ECOSAR software, the aquatic ecological environment would not be harmed by degradation intermediates. As a consequence, this heterogeneous system possesses admirable anti-interference in pollutant elimination. These conclusions provide instructions for the creation of S-doped porous carbon sheets for effective water treatment.

中文翻译:

嵌入丰富铁位点的硫掺杂多孔碳片用于 1O2 主导的过一硫酸盐活化

以自由基为主的过程的抗干扰能力差仍然是纯化有效性和基于过一硫酸盐的高级氧化过程(PMS-AOP)的实际应用的障碍。在此,采用莫尔盐和 ZIF-8 片作为前驱体,通过一步热解过程成功合成了铁、氮和硫共掺杂多孔碳片(Fe-SNC),以有效激活 PMS。淬火实验和电子顺磁共振(EPR)表征表明单线态氧(1 O 2)在苯酚降解中发挥着最重要的作用。基于材料结构的变化和密度泛函理论(DFT)计算,研究揭示了嵌入丰富的Fe 3 C、Fe 4 N和Fe-Nx催化位点中的硫作为PMS降解激活剂的具体机制感兴趣的污染物。此外,由于催化剂表面的电子极化,S掺杂位点缩短了PMS与催化剂之间的距离,从而有利于PMS的吸附。根据超高分辨率电喷雾飞行时间质谱和ECOSAR软件预测,降解中间体不会对水生生态环境造成危害。因此,这种异质系统在污染物消除方面具有令人钦佩的抗干扰性。这些结论为创建用于有效水处理的硫掺杂多孔碳片提供了指导。
更新日期:2024-04-02
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