4.7 Article

Highly efficient photocatalytic degradation of organic pollutants by mesoporous graphitic carbon nitride bonded with cyano groups

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 419, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.129503

Keywords

Tetracycline; Rhodamine B; g-C3N4; Intermediates; Toxicity evaluation

Funding

  1. National Research Foundation of Korea (NRF) - Korea Government (MIST: Ministry of Science and ICT) [2019R1A2C2085250]

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Constructing a high-performance visible-light responsive photocatalyst for remediation of organic pollutants from wastewater has been a significant challenge in recent years. In this study, mesoporous graphitic carbon nitride nano-clusters (NC MCN) were fabricated as a high-activity photocatalyst using SiO2 clusters as a template. The NC MCN photocatalyst showed enhanced light-harvesting efficiency and suppressed electron-hole recombination due to the introduction of structural defects, leading to high catalytic activity and stability in degrading organic pollutants under visible light irradiation.
Constructing high-performance visible-light responsive photocatalyst to remediate organic pollutants from wastewater is of great challenge in recent years. In this study, by using SiO2 clusters as a template, mesoporous graphitic carbon nitride nano-clusters (NC MCN) were fabricated as a high-activity photocatalyst. The confined growth of carbon nitride in the presence of SiO2 clusters introduced extra structural defects to the carbon nitride framework including nitrogen vacancies and cyano groups, which was confirmed by employing different characterization analyses. These structural defects created midgap states below the conduction band, which improved light-harvesting efficiency and suppressed electron-hole recombination. Thus, NC MCN showed high photocatalytic activity toward degradation of both tetracycline and rhodamine B under visible light irradiation. Complete degradation of 15 mL solution of 15 ppm tetracycline was achieved in 30 min compared to the bulk catalyst (taking more than 3 h). Furthermore, NC MCN demonstrated high stability after reusing for 8 consecutive photodegradation cycles. The total organic carbon concentration at different reaction time showed a rising and falling trend, which illustrate photodegradation process, i.e. adsorption, photodegradation, and mineralization. By liquid chromatography-mass spectroscopy analysis, the produced intermediates during the tetracycline degradation were proposed, which showed the formation of smaller molecules in just 15 min. The toxicity of the intermediates was analyzed using quantitative structure-activity relationship estimation and the outcomes exhibited that the toxicity of the solution reduced as the reaction time increased. This comprehensive study from photodegradation process to mineralization of TC demonstrated NC MCN as a promising photocatalyst for sustainable treatment of wastewater.

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