解开单原子Fe-N4催化位点选择性,通过激活硫酸盐产生单片氧:极化电场改变了电子转移路径
Yan Wang1, Shiyu Zuo2, Cheng Zeng2
1School of Environment and Energy, South China University of Technology, Guangzhou, 510006, China; Guangdong Plant Fiber High-Valued Cleaning Utilization Engineering Technology Research Center, Guangzhou, 510006, China; State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, 510006, China.
Chemosphere
|October 1, 2023
概括
单原子催化剂有效降解有机污染物. 在Fe (MIL) -SAC中的Fe-N4活性位点选择性地产生单点氧 (1O2),以有效处理水.
科学领域:
- 环境化学环境化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 单原子催化剂 (SAC) 在去除有机污染物方面表现有前途.
- 污染物降解中的SACs的结构-活性关系仍然不清楚.
- 为废水处理开发高效的催化剂至关重要.
研究的目的:
- 准备一个具有Fe-N4活性位点 (Fe (MIL) -SAC) 的单原子铁催化剂.
- 为了研究Fe (MIL) -SAC/Peroxydisulfate (PDS) 系统对硫甲 (SMX) 降解的性能.
- 为了阐明单点氧 (1O2) 生成的机制.
主要方法:
- 铁 (MIL) -SAC催化剂的合成.
- 使用Fe (MIL) -SAC/PDS系统进行降解实验.
- 动力分析和与芬顿和Fe (MIL) 系统的比较.
- 密度函数理论 (DFT) 计算以了解机制.
主要成果:
- Fe (MIL) -SAC/PDS实现了完全的SMX降解,并观察到高速率常数 (kobs = 0.466 min-1).
- 铁 (MIL) -SAC / PDS系统的性能优于芬顿系统 (kobs = 0.422 分钟-1) 和铁 (MIL) (kobs = 0.029 分钟-1).
- 据DFT计算,Fe-N4结构通过PDS激活促进了选择性1O2生成.
结论:
- 在Fe (MIL) -SAC中的Fe-N4活性位点在选择性1O2生成中起着关键作用.
- 铁 (MIL) -SAC/PDS系统为SMX移除提供了一种高效和强大的方法.
- 这项研究提供了有关为有针对性的污染物降解设计SAC的见解.
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