Fabricated layered g-C3N4 nanosheets for high efficiency photocatalytic degradation of atrazine：Insight into terminal-NHx in-situ activation of H2O2

Abstract

It is well known that graphite-like carbon nitride (g-C3N4) is a good photocatalyst for in-situ the production of H2O2. However, how to activate H2O2 generating the strong oxidizing ·OH is the key factor to affect the degradation of pollutants. In this paper, the layered g-C3N4 nanosheets were prepared by using urea and H2O with different mass ratios and calcined in Muffle furnace by one-step synthesis method. The morphology, composition and structure of photocatalysts were analyzed, indicating that the as-prepared L-g-C3N4-7 had abundant edge regions in comparison with L-g-C3N4 made by solid urea. The photocatalytic performance of g-C3N4 nanosheets was investigated with atrazine (ATZ) as the target pollutant in water. The results revealed that the prepared L-g-C3N4-7 exhibited the best photocatalytic activity in visible light (λ ≥ 420 nm). The degradation of 1.0 mg/L ATZ reached over 96% after 3 hours and the photocatalytic degradation rate constant (k) was 6.8 times than that of L-g-C3N4 photocatalyst. In addition, under the same conditions, the H2O2 production of L-g-C3N4-7 was 4.5 times than that of L-g-C3N4 photocatalyst. Based on the capture experiments of free radicals, it was found that the contribution rate of ·OH in L-g-C3N4-7 photocatalytic increased to 17 % compared to 4 % of L-g-C3N4 photocatalyst during the degradation of ATZ. The ·OH quantitative experiment indicated that the L-g-C3N4-7 photocatalyst could obviously activate H2O2 to generate ·OH and the amount of ·OH was 2.5 times than that of the L-g-C3N4 photocatalyst. More importantly, a large amount of terminal-NHx (14.6 %) in L-g-C3N4-7 was measured by the XPS, FT-IR and zeta potential. The additive H2O2 adsorption experiment in the dark was used to confirm terminal-NHx sites of L-g-C3N4-7 photocatalyst, which was beneficial to adsorb and activate H2O2. The results illustrated that the L-g-C3N4-7 photocatalyst with rich edge regions and terminal-NHx had the characteristics of in-situ the activation of H2O2 to generate ·OH. The findings suggest that designing and developing efficient g-C3N4 photocatalysts pave a new avenue for activating in situ self-synthesizing H2O2 and the removal of atrazine in water.