Journal
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
Volume 10, Issue 5, Pages -Publisher
ELSEVIER SCI LTD
DOI: 10.1016/j.jece.2022.108257
Keywords
Carbon nanotubes; N-doping; Different oxygen groups; Structure-activity correlation; PDS activation; Acetaminophen degradation
Categories
Funding
- National Research Foundation of Korea (NRF) - Korean government (MSIT) [2022R1A2B5B02001584]
- National Research Foundation of Korea [2022R1A2B5B02001584] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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The study revealed that the oxygen content on the surface of carbon nanotubes affects the catalytic degradation of acetaminophen via PDS activation, with the C-OH group being the dominant factor. Furthermore, graphitic nitrogen plays a key role in PDS activation, while pyridinic N and pyrrolic N have less impact on PDS adsorption and AAP oxidation.
Carbon nanotube (CNT) surfaces with different oxygen contents have been fabricated through an N-doping/chemical oxidation to investigate the relationship between structural features (defects and nitrogen and oxygen contents) and catalytic degradation of acetaminophen (AAP) via potassium peroxydisulfate (PDS) activation. Scavenging experiments and EPR analysis indicated that PDS activation was initiated by radical ((OH)-O-center dot, SO4 center dot-, and O2(center dot-)) and non-radical (O-1(2), surface-bound radicals and free electrons) mechanisms for AAP degradation. The surface-area-normalized AAP degradation rate constant (k(N)) at 0.6 mM PDS increased from 0.30 x 10(-2) m(-2 )s(-1) for pristine CNT to 0.82 x 10(-2) m(-2) s(-1) for Ox-NCNT. The k N was well-correlated with defects (I-D/I-G), the fraction of N 0 (hybrid sp 3 /sp 2 configuration), and oxygen groups (C-OH, C=O and COOH). Correlation analysis indicates that the electron-donating C-OH group dominantly governs the PDS activation and AAP oxidation. Similarly, among N-groups, a good correlation between k N and graphitic N also substantiates the idea that substitutional N plays on key active sites for PDS activation rather than boundary Ns (pyridinic N and pyrrolic N). The above findings were also validated through the quantitative relationship between PDS adsorption ability (Q(PDS)) and structural features of the catalyst (defects, N + O fractions, graphitic N and oxygen groups). Pyridinic N and pyrrolic N exhibited a weak linear relationship with Q PDS as well as k(N), indicating that the PDS adsorption and AAP oxidation is not directly controlled by these boundary N-groups.
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