期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 276, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119146
关键词
Carbon edge; defect; carbocatalysis; persulfate activation; nonradical pathway
资金
- National Natural Science Foundation of China [51425302, 51702062]
- Chinese Academy of Sciences
- Australian Research Council [DP190103548]
Graphitic multi-walled carbon nanotubes (MWCNTs) are controllably unzipped into edge-rich graphene nanoribbons to reveal the roles of edges and defects in persulfate activation for bisphenol A (BPA) oxidation. Enriched carbon edges remarkably enhance the catalytic performance and can serve as hosting sites for heteroatom (N, S) doping to promote carbocatalysis. A sample (NS-2) presented a complete BPA removal in 20 min at a rate constant of 0.182 min(-1). The rate constants were relating to the defect speciation in a negative correlation to an indicator (I-D/I-D') from Raman spectra. Excessive edges induce defects and structure transformation of sp(2) to sp(3), resulting in deterioration of the organic oxidation. Furthermore, unzipped MWCNTs were clarified to follow a nonradical electron transfer pathway by radical screening tests, in situ Raman and electrochemical characterizations. The unveiled mechanism emphasizes the importance of an essential graphitic degree and conductivity in the edge-enriched carbocatalysts for better catalytic performance.
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