Photochemical reactivity of nitrogen-doped biochars under simulated sunlight irradiation: Generation of singlet oxygen

J Hazard Mater. 2021 May 15:410:124547. doi: 10.1016/j.jhazmat.2020.124547. Epub 2020 Nov 11.

Abstract

This study explored the photochemical activity of nitrogen-doped biochars (NCMs) by investigating their role in the degradation of sulfamethazine under simulated sunlight irradiation. NCMs with different doping amounts were prepared from corn straw and urea. Results showed that nitrogen doping can notably enhance the photodegradation of SMT rather than raw char. NCMs are of photochemical activity under visible light, which was confirmed by monochromatic light experiments. Quenching experiments, ESR, pH effect, and the influence of O2 were carried out to explore the involved oxidation mechanism in this system. Results showed that 1O2 was the main reactive oxygen species. 1O2 was produced from O2 by both energy transfer and electron transfer. DFT calculations showed that pyridinic N doping can decrease the energy of intersystem crossing and thus benefit the generation of 1O2 by triplet-triplet energy transfer. Results underscore the explicit importance of nitrogen element in photochemical reactivity of chars under simulated light irradiation even when the nitrogen content is low. It is a meaningful reminder for us to pay more attention to the assessment of the fate and transport of contaminants in the soil where it is rich in NCMs as well as the potential use of NCMs for pollutants remediation, since visible light is very abundant near the earth's surface.

Keywords: Nitrogen-doped char; Photodegradation; Singlet oxygen; Sulfamethazine; Sunlight.

Publication types

  • Research Support, Non-U.S. Gov't