基于铁单原子的双反应中心催化触发了内部驱动和外部驱动的绿色芬顿式化学路径
Qingbai Tian1, Jiale Chang1, Xiaoming Peng2
1School of Environmental Science and Engineering, Shandong University, Qingdao, 266237, P.R. China.
Angewandte Chemie (International ed. in English)
|February 28, 2025
概括
这项研究探讨了双反应中心 (DRC) 的铁单原子催化剂的芬顿式化学. 它揭示了零和低氧化剂系统中独特的电子迁移机制,使得污染物的可持续降解成为可能.
科学领域:
- 环境化学环境化学
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
背景情况:
- 双反应中心 (DRCs) 芬顿式化学提供可持续的污染物降解与低或零氧化剂添加.
- 了解这些系统中的电子迁移机制至关重要,但具有挑战性.
- 铁单原子催化剂 (Fe/N-SAC) 对此类应用具有前景.
研究的目的:
- 研究Fe/N-SAC在内部驱动 (零氧化剂) 和外部驱动 (低过氧化硫酸盐 (PMS) 添加) 系统中的电子迁移机制.
- 为这些DRC系统的长期应用设计操作设备.
- 阐明促进污染物降解的催化途径.
主要方法:
- 铁单原子DRCs催化剂 (Fe/N-SAC) 的制备.
- 在零和低PMS条件下对电子转移过程的实验研究.
- 设计和测试长期运行的实验设备.
主要成果:
- 在零氧化剂系统中,Fe/N-SAC充当了主要的电子受体,在没有溶解氧激活的情况下,将铁的价值从+2.37降低到+2.07.
- 在低PMS系统中,电子转移到PMS和铁原子,涉及电子转移过程 (ETP) 和内部铁驱动机制.
- 在PMS-零Fe/N-SAC系统中没有溶解氧激活.
- 在O2大气下证明了铁单个原子的可回收性.
结论:
- 这项研究澄清了不同氧化条件下的Fe/N-SAC中独特的电子迁移途径.
- 开发的实验设备促进了内部和外部驱动的DRC系统的长期运行.
- 这些发现有助于理解用于可持续环境修复的催化机制和模块应用.
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