Journal
JOURNAL OF HAZARDOUS MATERIALS
Volume 427, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.jhazmat.2021.128204
Keywords
Metal leaching; Peroxymonosulfate; Confined effect; Zeolitic imidazolate frameworks; Catalytic stability
Categories
Funding
- National Key Research and Development Program of China [2021YFA1202500]
- National Natural Science Foundation of China [52070133]
- Chengdu Science and Tech-nology Project [2021-YF05-00892-SN]
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Metal leaching and catalytic stability are important issues in Fenton-like reactions. In this study, a hollow yolk-shell nanoreactor (HYSCN) was fabricated to activate peroxymonosulfate (PMS) for the degradation of carbamazepine (CBZ). The HYSCN showed reduced metal leaching and improved catalytic stability compared to a solid structure (SCSCN). The mechanism of the HYSCN/PMS system was investigated and the degradation pathway of CBZ was proposed using UPLC-Q-TOF-MS/MS.
Metal leaching and catalytic stability are the key issues in Fenton-like reaction. Herein, a hollow yolk-shell nanoreactor (HYSCN) with shell confined Co species was fabricated for peroxymonosulfate (PMS) activation to degrade carbamazepine (CBZ). The uniform Co nanoparticles were completely anchored in a hollow void, further confined by a porous N-doped carbon shell. The unique construction significantly reduces Co species leaching in PMS activation and enhances catalytic stability. Co leaching came from HYSCN dropped by almost fourfold compared to CN-8 without shell confined (0.403 mg/L to 0.120 mg/L). The catalytic stability is also greatly improved, confirming the dominant role of heterogeneous catalysis in the HYSCN/PMS system. HYSCN exhibits excellent catalytic performance compared to a solid structure (SCSCN), demonstrating the significance of hollow structures. Mechanism study found that HO center dot, SO4 center dot- and O-1(2) induced in HYSCN/PMS system and the relative contributions were distinguished and quantified by stoichiometric methods. The UPLC-Q-TOF-MS/MS was used to identify the CBZ degraded intermediate products and the possible degradation pathway was proposed. This study will provide theoretical guidance for reducing metal leaching and improving catalytic stability in the PMS activation.
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