确定FeOCl上表面基的作用,以弥合电子转移,实现高效的酸盐激活
Ximeng Xu1, Shujing Zhang1, Yuhao Wang1
1Faculty of Civil Engineering and Mechanics, Kunming University of Science and Technology, Kunming 650093, China.
Environmental science & technology
|August 15, 2023
概括
铁氧化 (FeOCl) 上的表面基对在先进的氧化过程 (AOP) 中激活硫酸盐 (PDS) 至关重要. 调节氧化会提高FeOCl催化剂在水处理中的效率.
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:
- 铁氧化 (FeOCl) 显示出作为高级氧化过程 (AOP) 催化剂的希望.
- 在FeOCl的催化活性背后的确切机制,特别是在硫酸盐 (PDS) 激活中,仍然不清楚.
- 表面基团被怀疑在异质催化中发挥作用.
研究的目的:
- 为了阐明FeOCl催化PDS激活的机制.
- 为了研究表面基在FeOCl/H2O接口中对电子转移的作用.
- 了解表面修饰如何影响FeOCl催化性能.
主要方法:
- 减弱总反射-里埃变换红外光谱 (ATR-FTIR) 和拉曼光谱被用来分析表面物种.
- 射线吸收细结构 (XAFS) 光谱学提供了对Fe的电子和局部结构的见解.
- 密度函数理论 (DFT) 的计算被用来建模反应机制和表面相互作用.
主要成果:
- 发现酸盐离子通过替代表面基团来抑制FeOCl活性,证实了它们的重要作用.
- 极性FeOCl表面的水解导致Fe位点周围的电子丰富,增强PDS的吸引力.
- 显著促进了PDS吸附,在PDS中延长O-O键,以及从Fe转移到PDS的电子.
结论:
- 表面基因对于FeOCl和PDS之间的过桥电子转移至关重要.
- 表面氧化增强PDS吸附和FeOCl催化剂上的激活.
- 本研究提供了一种战略,通过控制表面基化来开发高效的异质AOP催化剂.
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