材料科学
激进的
对偶(语法数字)
Atom(片上系统)
纳米技术
化学物理
结晶学
有机化学
化学
计算机科学
艺术
文学类
嵌入式系统
作者
Xin Zhou,Yanting Zhou,Shicheng Zhao,Shanshan Fan,Xing He,Jiangfang Yu,Lin Tang,Jiajia Wang
标识
DOI:10.1002/adfm.202513232
摘要
Abstract Non‐radical species exhibit selective degradation of electron‐rich pollutants, yet their practical utility is hampered by low yields and uncontrolled speciation arising from competing radical formation. Herein, a novel FeMo─N─C catalyst is designed to simultaneously activate peroxymonosulfate and steer reaction pathways toward non‐radical oxidation by reducing the formation energy of non‐radical species, thus enabling selective degradation of electron‐donating organic contaminants. The catalyst achieves complete degradation of 50 mg L −1 2,4 dichlorophenol within 12 min, exhibiting a first‐order kinetic constant of 0.587 min −1 a 20.67 fold enhancement compared to the Fe─N─C/PMS system. Experimental results identified singlet oxygen ( 1 O 2 ) as the predominant reactive oxygen species. The incorporation of Mo not only promotes the generation of non‐radical species but also accelerates the Fe 3+ /Fe 2+ cycling, thereby improving both catalytic efficiency and reusability. Density functional theory calculations reveal that the introduction of Mo modulates the d‐band center of Fe sites and optimizes charge distribution, ultimately regulating non‐radical pathway formation. Thermodynamic analysis further demonstrates that the FeMo─N─C system possesses a lower energy barrier for 1 O 2 generation compared to Fe─N─C, favoring selective 1 O 2 production. These findings can guide the rational design of robust single‐atom catalysts toward the selective and controllable generation of non‐radical species with high yield.
科研通智能强力驱动
Strongly Powered by AbleSci AI