Journal
ACS ES&T ENGINEERING
Volume 3, Issue 11, Pages 2038-2050Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsestengg.3c00323
Keywords
Defect-rich carbon; Metal-organicframeworks; Pyrolysis; Sulfadiazine; Peroxymonosulfateactivation
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This study introduces an innovative approach utilizing MOFs for defect engineering of carbon materials, demonstrating the significance of defects in activating peroxymonosulfate (PMS). The defect-rich carbon-based catalysts synthesized through this method showed excellent potential for practical applications.
The significance of defects in carbon materials for activating peroxymonosulfate (PMS) has garnered significant attention, and enhancing the heteroatom content of carbon materials is critical in defect engineering. In this study, defect-rich carbon-based catalysts (NOCs) were synthesized through one-step pyrolysis by utilizing metal-organic frameworks (MOFs) MIL-101-NH2(Fe) as precursors. These catalysts were employed as PMS activators for the degradation of sulfadiazine (SDZ). The design and regulation of organic ligands in MOFs facilitated the introduction of high levels of oxygen- and nitrogen-containing groups, which decomposed under a regulated pyrolysis temperature gradient, to result in the formation of defects. Furthermore, both experimental and theoretical calculations confirmed that edge defects (armchair edges and zigzag edges) and carbon vacancies played specific active roles by promoting adsorption and electron absorption from PMS. Consequently, this process led to the generation of O-2(center dot-) and O-1(2), which played a dominant role in the degradation of SDZ. The NOC-1000/PMS system demonstrated universal applicability to various antibiotics, anions, and water matrices. Notably the defects could be regenerated through secondary calcination, thereby highlighting their excellent potential for practical applications. This study introduces an innovative approach utilizing MOFs for defect engineering of carbon materials.
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