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 O2
•– and 1O2, 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.