Markedly boosted peroxymonosulfate- and periodate-based Fenton-like activities of iron clusters on sulfur/nitrogen codoped carbon: Key roles of a sulfur dopant and compared activation mechanisms

Long，Yangke1,2; Huang，Shixin2; Sun，Jianlin1; Peng，Dan1; Zhang，Zuotai2

2023-01-10

10.1016/j.scitotenv.2022.158752

SCIENCE OF THE TOTAL ENVIRONMENT   影响因子和分区

0048-9697

1879-1026

Highly dispersed iron nanoclusters on carbon (FeNC@C) hold great promise for wastewater purification in Fenton-like reactions. The microenvironment engineering of central Fe atom is promising to boost the activation capacity of FeNC@C, which is however remains a challenge. This study developed a self-sacrificed templating strategy to S, N-codoped carbon supported Fe nanoclusters (FeNC@SNC) activator and find the key role of sulfur heteroatoms in regulating the electron structure of Fe sites and final activation property. Investigations revealed that the FeNC@SNC composite exhibited unusual bifunctional activity in both peroxymonosulfate (PMS)- and periodate (PI)-based Fenton-like reactions. We also offered insights into the differences between the degradation of organics by the FeNC@SNC/PMS and FeNC@SNC/PI systems. Specifically, under identical conditions, the FeNC@SNC/PMS system delivered a higher oxidation capability and stronger resistance to nontarget matrix constituents, but showed more severe Fe leaching than the FeNC@SNC/PI system. Furthermore, while mediated electron-transfer process was identified as the major route for pollutant decomposition in both systems, the high-valent Fe-oxo species [Fe (IV)] was the auxiliary reactive species found only in the FeNC@SNC/PMS system. Based on these findings, our results provide profound insights into the design of active and durable Fe-based activators toward highly efficient Fenton-like reactions.

Electronic structure modulation Fenton-like reactions Iron-based activator Refractory pollutant Wastewater treatment

SCI ; EI

英语

其他

National Natural Science Foundation of China[51772141];

Environmental Sciences & Ecology

Environmental Sciences

WOS:000888904200011

ELSEVIER

20224012834687

Carbon ; Chemical activation ; Electron transport properties ; Electronic structure ; Iron compounds ; Nanoclusters ; Oxidation ; Sulfur

Industrial Wastes Treatment and Disposal:452.4 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Solid State Physics:933

ENVIRONMENT/ECOLOGY

2-s2.0-85139077829

Scopus

1.Department of Transportation and Environment,Shenzhen Institute of Information Technology,Shenzhen,518172,China
2.Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control,School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China

Long，Yangke,Huang，Shixin,Sun，Jianlin,et al. Markedly boosted peroxymonosulfate- and periodate-based Fenton-like activities of iron clusters on sulfur/nitrogen codoped carbon: Key roles of a sulfur dopant and compared activation mechanisms[J]. SCIENCE OF THE TOTAL ENVIRONMENT,2023,855.

Long，Yangke,Huang，Shixin,Sun，Jianlin,Peng，Dan,&Zhang，Zuotai.(2023).Markedly boosted peroxymonosulfate- and periodate-based Fenton-like activities of iron clusters on sulfur/nitrogen codoped carbon: Key roles of a sulfur dopant and compared activation mechanisms.SCIENCE OF THE TOTAL ENVIRONMENT,855.

Long，Yangke,et al."Markedly boosted peroxymonosulfate- and periodate-based Fenton-like activities of iron clusters on sulfur/nitrogen codoped carbon: Key roles of a sulfur dopant and compared activation mechanisms".SCIENCE OF THE TOTAL ENVIRONMENT 855(2023).