Surface-bound radicals generated from cobalt single-atom catalyst: Mechanism of boosting Fenton-like reactions
CHEMICAL ENGINEERING JOURNAL(2023)
摘要
environmental treatment. However, their identification on catalyst surface and contribution to pollutant degradation have never been well addressed. In this study, single Co atom anchored on Al-doped SiO2 (Co@Al-SiO2) catalyst was well designed for peroxymonosulfate (PMS) activation to produce a high concentration of surface-bound sulfate radicals (SO4 center dot-) and reached 100 % removal percentage of antibiotics, dyes and volatile organic compounds (VOCs) pollutants within several minutes. In-situ cyclic voltammetry-electrochemical quartz crystal microbalance (CV-EQCM) and the derived calculation method were firstly employed to quantitatively identify the surface-bound SO4 center dot-. Results show that abundant surface-bound SO4 center dot- was generated on Co-Si bond and its concentration reached 1.17 x 10(-6) mol/m(2), which was very close to the theoretical maximum (1.34 x 10(-6) mol/m(2)). Further experiments demonstrated that Co atoms can provide rich binding sites for SO4 center dot-, resulting in the enrichment of surface-bound SO4 center dot- in nanoscale surface. This behavior can remarkably boost the degra-dation kinetics towards various organic contaminants. Coupled with a membrane in water treatment, this system showed an outstanding performance for degradation of pollutants such as dyes (>99 %) with the flow rate of 20 ml/min after 0.5 s, which was considerably faster than traditional treatments. This study provides a fundamental insight into surface-bound radical, guiding the rational design of catalyst for Fenton-like reactions in environ-mental application.
更多查看译文
关键词
Fenton -like reactions,Single -atom catalyst,Peroxymonosulfate,Surface-bound radicals,CV-EQCM
AI 理解论文
溯源树
样例
生成溯源树,研究论文发展脉络
Chat Paper
正在生成论文摘要