Metal-organic framework-derived magnetic carbon for efficient decontamination of organic pollutants via periodate activation: Surface atomic structure and mechanistic considerations.
J Hazard Mater
; 424(Pt B): 126786, 2022 02 15.
Article
em En
| MEDLINE
| ID: mdl-34655874
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.
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Texto completo:
1
Coleções:
01-internacional
Contexto em Saúde:
12_ODS3_hazardous_contamination
Base de dados:
MEDLINE
Assunto principal:
Poluentes Ambientais
/
Estruturas Metalorgânicas
Idioma:
En
Revista:
J Hazard Mater
Ano de publicação:
2022
Tipo de documento:
Article