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Fe-N₄网站的旋转状态调节PMS激活途径对于超快的硫甲醇降解

Jing Lu¹, Anting Ding², Luning Wang^2,3

¹College of Environmental & Resource Sciences, Zhejiang University, Hangzhou, China.

Small (Weinheim an der Bergstrasse, Germany)

|January 17, 2026

概括

单原子FeN4催化剂的旋转状态工程精确地控制过氧硫酸盐激活通路. 这一突破使得高度选择性的氧化能够有效地去除水处理中的污染物.

科学领域:

材料科学材料科学材料科学
环境化学环境化学
催化剂是一种催化剂.

背景情况:

对氧硫酸盐 (PMS) 激活的芬顿类催化剂的合理设计受到Fe旋转状态和反应途径之间的相关性缺乏理解的阻碍.
原子分散的FeN4催化剂提供可调节的电子结构,但需要精确控制旋转配置以优化性能.

研究的目的:

调查单原子Fe位点的旋转配置与PMS激活路径的选择性之间的精确相关性.
开发一种方法来设计FeN4催化剂的低旋转和高旋转状态,用于增强水处理应用.

主要方法:

合成原子分散的FeN4催化剂 (Fe1NC) 与工程低旋转和高旋转状态,使用sol-gel衍生,气相辅助碳化策略.
通过PMS激活进行硫甲醇降解的性能评估,评估各种条件下的催化剂稳定性 (离子,pH,水矩阵).
密度函数理论 (DFT) 计算以阐明旋转状态指定的活性氧物种 (ROS) 路径和反应机制.

主要成果:

设计的Fe1NC催化剂证明了超快速的PMS激活,在3分钟内实现了超过95%的硫甲醇降解,并观察到高速率常数 (kobs = 0.96 min-1).
DFT的计算显示,低旋转的FeN4促进单片氧 (1O2) 的形成,而高旋转的FeN4则促进Fe(IV) =O的形成,从而创造出明显的ROS通路.
催化剂对干扰离子,pH值波动和各种水矩阵具有强大的抵抗力,并在连续膜反应堆中保持超过85%的清除能力超过7小时.

结论:

单原子FeN4催化剂的旋转状态工程提供了一种机械杆,可以精确控制PMS激活中的ROS选择性.
开发的Fe1NC催化剂通过非激素主导的氧化模式运行,对富含电子的污染物具有很高的选择性和最小的矩阵干扰.
这项工作为设计用于水处理中先进氧化过程的高性能单原子催化剂建立了新的范式.

关键词:

过氧单硫酸盐的使用有活性氧物种的反应性氧物种.一个原子的催化剂.旋转状态是指旋转状态.硫甲佐 (sulfamethoxazole) 是一种硫甲的化合物.

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