Pyrolyzed iron-nitrogen-carbon hybrids for efficient contaminant decomposition via periodate activation: Active site and degradation mechanism

Long, Yangke1; Huang, Shixin2; Zhao, Shiyin3; Xiao, Guicong1; Sun, Jianlin1; Peng, Dan1

2023-07-15

10.1016/j.seppur.2023.123945

SEPARATION AND PURIFICATION TECHNOLOGY   影响因子和分区

1383-5866

1873-3794

The practical application of periodate-based advanced oxidation technologies (PI-AOTs) for wastewater treatment requires efficient and cost-effective activators. Pyrolyzed Fe-N/C materials are potential candidates, however, their actual active sites and activation mechanisms are yet to be fully understood. Herein, a series of Fe-N/C samples (denoted as Fe@NC-X) with differing structures and iron components were delicately synthesized. Experimental studies on the structure-activity relationship and density functional theory (DFT) computations revealed that Fe-Nx species serve as the dominant active site for periodate activation, while the inactive iron-based particles (i.e., Fe-0 and Fe3C) optimized the binding affinity of surrounding carbon layers with periodate, resulting in enhanced activity. In-depth exploration of the oxidative mechanism revealed that Fe@NC-X activated periodate through an electron transfer regime. Our results also showed that the optimal Fe@NC-0.2/ periodate system was highly effective in catalyzing the oxidation of 4-CP, outperforming many reported activators. These findings provide an indispensable foundation for the rational development of advanced Fe-N/C activators and offer vital insights into the mechanism underlying pollutant destruction through PI-AOTs.

Wastewater treatment Advanced oxidation technology Zero-valent iron Fe-N-x Nonradical oxidation

SCI ; EI

英语

其他

Stable Support Plan Program of Shenzhen Natural Science Fund[20220817174758001] ; University Key Research Project in Guang-dong Province[2022ZDZX4103] ; Youth Research Pro-gram of Shenzhen Institute of Information Technology[XJ2021001501] ; Innovation Team Project in Guangdong Prov-ince[2022KCXTD058] ; China Postdoctoral Science Founda-tion[2019 M661695]

Engineering

Engineering, Chemical

WOS:000992418000001

ELSEVIER

20231814035565

Binding energy ; Chemical activation ; Cost effectiveness ; Degradation ; Density functional theory ; Iron compounds ; Nitrogen ; Oxidation

Industrial Wastes Treatment and Disposal:452.4 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Industrial Economics:911.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

CHEMISTRY

Web of Science

1.Shenzhen Inst Informat Technol, Dept Transportat & Environm, Shenzhen 518172, Peoples R China
2.Southern Univ Sci & Technol, Sch Environm Sci & Engn, Guangdong Prov Key Lab Soil & Groundwater Pollut C, Shenzhen 518055, Peoples R China
3.Natl Univ Def Technol, Coll Sci, Changsha 410073, Peoples R China

Long, Yangke,Huang, Shixin,Zhao, Shiyin,et al. Pyrolyzed iron-nitrogen-carbon hybrids for efficient contaminant decomposition via periodate activation: Active site and degradation mechanism[J]. SEPARATION AND PURIFICATION TECHNOLOGY,2023,317.

Long, Yangke,Huang, Shixin,Zhao, Shiyin,Xiao, Guicong,Sun, Jianlin,&Peng, Dan.(2023).Pyrolyzed iron-nitrogen-carbon hybrids for efficient contaminant decomposition via periodate activation: Active site and degradation mechanism.SEPARATION AND PURIFICATION TECHNOLOGY,317.

Long, Yangke,et al."Pyrolyzed iron-nitrogen-carbon hybrids for efficient contaminant decomposition via periodate activation: Active site and degradation mechanism".SEPARATION AND PURIFICATION TECHNOLOGY 317(2023).