Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations

Long，Yangke; Dai，Jian; Zhao，Shiyin; Huang，Shixin; Zhang，Zuotai

2022-02-15

10.1016/j.jhazmat.2021.126786

JOURNAL OF HAZARDOUS MATERIALS   影响因子和分区

0304-3894

1873-3336

Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as Co@NC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation, surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation.

MOF derivatives Nonradical mechanism Surface atomic engineering Water treatment

SCI ; EI

英语

第一 ; 通讯

Engineering ; Environmental Sciences & Ecology

Engineering, Environmental ; Environmental Sciences

WOS:000711845700006

ELSEVIER

20214211023981

Carbon ; Chemical activation ; Cobalt ; Cost effectiveness ; Density functional theory ; Doping (additives) ; Metal nanoparticles ; Organic pollutants ; Reusability ; Water treatment

Water Treatment Techniques:445.1 ; Nonferrous Metals and Alloys excluding Alkali and Alkaline Earth Metals:549.3 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Industrial Economics:911.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

ENGINEERING

2-s2.0-85116893420

Scopus

Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control,School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China

Long，Yangke,Dai，Jian,Zhao，Shiyin,等. Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations[J]. JOURNAL OF HAZARDOUS MATERIALS,2022,424.

Long，Yangke,Dai，Jian,Zhao，Shiyin,Huang，Shixin,&Zhang，Zuotai.(2022).Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations.JOURNAL OF HAZARDOUS MATERIALS,424.

Long，Yangke,et al."Metal–organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations".JOURNAL OF HAZARDOUS MATERIALS 424(2022).