Pivotal roles of N-doped carbon shell and hollow structure in nanoreactor with spatial confined Co species in peroxymonosulfate activation: Obstructing metal leaching and enhancing catalytic stability

• DOI: 10.1016/j.jhazmat.2021.128204
• Publication Date: 2022-01-04T16:16:53Z
• Authors: Zelin Wu; Zhaokun Xiong; Rui Liu; Chuanshu He; Yang Liu; Zhicheng Pan; Gang Yao; Bo Lai
• Keywords: Tandem Mass Spectrometry; Nanotechnology; 01 natural sciences; Carbon; Catalysis; Peroxides; 0104 chemical sciences

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•, SO4•- and 1O2 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.