期刊
SEPARATION AND PURIFICATION TECHNOLOGY
卷 276, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.seppur.2021.119286
关键词
Peroxymonosulfate; Nitrogen and phosphorus co-doped porous carbon; Heteroatom doping; Phytic acid; Non-radical
资金
- National Natural Science Foundation of China [21407026]
- Natural Science Foundation of Fujian Province, China [2020J01506]
- Fuzhou University [2021T012]
The nitrogen and phosphorus co-doped metal-free porous carbon (NPC) with core/shell structure demonstrated outstanding catalytic performance on PMS activation for the degradation of phenol. The optimized N-P co-doping strategy played a synergistic effect in promoting the catalytic activity of NPC. In addition, NPC showed excellent acid-base tolerance and insensitivity to anions and humic acid, making it a promising PMS activator for phenol degradation.
A nitrogen and phosphorus co-doped metal-free porous carbon (NPC) with core/shell structure was successfully synthesized by pyrolysis of ZIF-8@phytic acid (PA) and demonstrated outstanding catalytic performance on PMS activation for the degradation of phenol (98.0% within 30 min at pH = 7.0). Results suggested that optimized NP co-doping strategy played a synergistic effect in promoting the catalytic activity of NPC. In addition, NPC displayed excellent acid-base tolerance (pH = 3.0-10.0) and insensitive to anions (Cl-, HCO3- and H2PO4-) and humic acid when employed as PMS activator for phenol degradation. Based on quenching tests, electron paramagnetic resonance (EPR) measurements and electrochemical analysis, singlet oxygen (O-1(2)) is the key active specie and the surface-bound sulfate radical (SO4 center dot-) plays an auxiliary role in the removal of phenol in NPC/PMS system while surface electron transfer is also a non-radical pathway. Large BET specific surface areas (SSA), total pore volumes (TPV) and hierarchical porous structure are beneficial to expose more active sites (essentially graphite N and C=O) for generating O-1(2) and surface-bound SO4 center dot- to enhance catalytic performance of NPC. This work opens up a new way for the synthesis of highly efficient N-P co-doped metal-free PMS activators and provides novel insights into the mechanism of PMS activation by NPC.
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