Molecular self-assembled synthesis of highly dispersed Co single-atom coordinated 2-methylimidazole modified carbon nitride for peroxymonosulfate activation

催化作用 化学 吸附 活性炭 氮化碳 无机化学 光化学 物理化学 有机化学 光催化
作者
Ruilan Wei,Hui Wang,Longbo Jiang,Jinjuan Yang,Wenqin Li,Xingzhong Yuan,Hou Wang,Jie Liang,Yaoning Chen,Yuanqing Bu
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:471: 144494-144494 被引量:31
标识
DOI:10.1016/j.cej.2023.144494
摘要

Although single-atom catalysts are pioneers in peroxymonosulfate (PMS) activation, selection of substrates and enhanced binding remains ambiguous. Here, a novel highly dispersed cobalt single-atom loaded 2-methylimidazole (MeIm) ligand-modified carbon nitride catalyst (Co-MCAMeIm) was prepared by a molecular self-assembly strategy. The densely distributed SA-Co with Co-N sites were corroborated by HAADF-STEM and XAFS analysis. The strong chelation of pre-dispersed ligands and triazine ring of g-C3N4 confers higher stability to the catalyst, reducing Co leaching. Meanwhile, the g-C3N4 substrate offers additional adsorption sites to shorten the reaction distance. The embedded Co-N functions as an electron donor capable of bridging N-rich carbon networks, hence accelerating the electron transport. Experimental findings demonstrated that sulfamethoxazole (SMX) could be effectively cleared through Co-MCAMeIm/PMS process (99.1%, 0.13 min−1). Several key influencing factors like Co to MeIm molar ratio, PMS concentration, Co-MCAMeIm dosage, pH value, anions, and humic acid were examined. The catalytic pathway is dominated by the activation of PMS with SA-Co-N as active sites to form 1O2. Meanwhile, a multi-ROS process with occurrence of SO4•-, O2•- and •OH was confirmed. Additionally, the SMX degradation routes and toxicity variations were derived and analyzed. Herein, the research may provide new insights for stable single-atom catalyst towards water treatment.
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